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Materials & Design 226 (2023) 111661

Contents lists available at ScienceDirect

Materials & Design


journal homepage: www.elsevier.com/locate/matdes

Multi-material additive manufacturing: A systematic review of design,


properties, applications, challenges, and 3D printing of materials and
cellular metamaterials
Aamer Nazir a,b,⇑, Ozkan Gokcekaya c,d,⇑, Kazi Md Masum Billah e, Onur Ertugrul f, Jingchao Jiang g,
Jiayu Sun h, Sajjad Hussain a
a
Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon 999077, Hong Kong, China
b
State Key Laboratory of Ultra-precision Machining Technology, Department of Industrial and Systems Engineering, The Hong Kong Polytechnic University, Hung Hom, Kowloon, Hong
Kong, China
c
Division of Materials and Manufacturing Science, Graduate School of Engineering, Osaka University, 2-1, Yamadaoka, Suita, Osaka 565-0871, Japan
d
Anisotropic Design & Additive Manufacturing Research Center, Osaka University, 2-1, Yamadaoka, Suita, Osaka 565-0871, Japan
e
Mechanical Engineering Program, University of Houston-Clear Lake, 2700 Bay Area Blvd, Houston, TX, USA
f
Department of Materials Science and Engineering, Izmir Katip Celebi University, Cigli Campus, Central Offices 1, 35620 Cigli, Izmir, Turkey
g
Department of Mechanical and Automation Engineering, The Chinese University of Hong Kong, Shatin, Hong Kong, China
h
Institute for Materials Research, Tohoku University, Japan

h i g h l i g h t s g r a p h i c a l a b s t r a c t

 Recent developments in multi-


material additive manufacturing
(MMAM) were comprehensively
reviewed.
 The applications of MMAM were
discussed regarding various materials
and AM methods.
 The aspect of MMAM design,
modeling, post-processing, and
analysis was summarized.
 Limitations, challenges, future trends
of MMAM were highlighted.

a r t i c l e i n f o a b s t r a c t

Article history: Extensive research on nature-inspired cellular metamaterials has globally inspired innovations using sin-
Received 2 December 2022 gle material and limited multifunctionality. Additive manufacturing (AM) of intricate geometries using
Revised 23 January 2023 multi-materials provides additional functionality, environmental adaptation, and improved mechanical
Accepted 24 January 2023
properties. Recently, several studies have been conducted on multi-material additive manufacturing
Available online 27 January 2023

Abbreviations: ABS, Acrylonitrile Butadiene Styrene; ASA, Acrylonitrile Styrene Acrylate; AJ, Aerosol jetting; AF, Aramid fibre; AM, additive manufacturing; BJ, Binder
jetting; B4C, Boron carbide; CAD, Computer-aided design; CaP, Calcium phosphate; CFD, Computational fluid dynamics; CPE, Chlorinated polyethylene; DED, Direct energy
deposition; DLD, Direct laser deposition; DMD, Direct metal deposition; DEM, Discrete element method; DMLS, Direct metal laser sintering; DfAM, Design for AM; DIW, Direct
ink writing; DLP, Digital light processing; EAP, Electroactive polymer; EPBF, Electron beam powder bed fusion; FEM, Finite element method; FFA, Flexible fluidic actuation;
FDM, Fused deposition modelling; FFF, Fused filament fabrication; FGM, functionally graded materials; GelMA, Gelatin methacryloyl; HA, Hydroxyapatite; HIPS, High Impact
Polystyrene; IJ, Inkjet; ISS, International Space Station; IN718, Inconel 718; LENS, Laser Engineered Net Shaping; LOM, Laminated object manufacturing; LPBF, Laser powder
bed fusion; LMD, Laser metal deposition; LBF, Laser based fusion; MD, Molecular dynamics; ME, Material Extrusion; MJ, Material jetting; MJF, Multi Jet Fusion; MM, multi-
material; MMAM, multi-material additive manufacturing; MMFGAM, Multi-material functionally graded additive manufacturing; OLED, Organic light emitting diode; PBF,
Powder bed fusion; PneuNet, Pneumatic network; PLA, Polylactic acid; PETG, Polyethylene terephthalate glycol; PJ, PolyJet; PEEK, Polyether ether ketone; PET, Polyethylene
terephthalate; PC, Polycarbonate; PCL, Polycaprolactone; PVA, Polyvinyl alcohol; PEGDA, Poly(ethylene glycol) diacrylate; SLA, Stereolithography; SiC, Silicon carbide; SCF,
Short carbon fiber; SMMs, Shape-memory materials; TPU, Thermoplastic polyurethane; TCP, Tricalcium phosphate; TPE, Thermoplastic Elastomer; SLS, Selective laser
sintering; VW, Vero White Plus; WoS, Web of Science.
⇑ Corresponding authors.
E-mail addresses: [email protected], [email protected] (A. Nazir), [email protected] (O. Gokcekaya).

https://doi.org/10.1016/j.matdes.2023.111661
0264-1275/Ó 2023 The Author(s). Published by Elsevier Ltd.
This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

(MMAM) technologies, including multi-materials, methodologies, design, and optimization. However, in


the past six years, very few or no systematic and complete reviews have been conducted in this research
domain. This review intends to comprehensively summarize MMAM systems and the working principles
Keywords:
of its fundamental processes. Herein, the Multi-material combinations and their design, modeling, and
Multi-material
Additive manufacturing
analysis strategies have been reviewed systematically. In particular, the focus is on applications and
3D printing opportunities for using MMAM for several industries and postprocessing MMAM fabricated parts.
Cellular metamaterials Furthermore, this review identified the limitations and challenges of existing software packages,
Cellular structures MMAM processes, materials, and joining mechanisms, especially at the multi-material interfaces.
DfAM Finally, we discuss the possible strategies to overcome the aforementioned technological challenges
and state the future directions, which will provide insights to researchers and engineers designing and
manufacturing complex nature-inspired objects.
Ó 2023 The Author(s). Published by Elsevier Ltd. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).

1. Introduction and background overview addressing the aforementioned challenges [2-4]. Moreover, the
recent advancements in AM techniques have enabled the fabrica-
Nature demonstrates incredibly optimized design and fabrica- tion of MMs and compositions with functionally graded structures
tion by selecting application-specific combinations of composi- in a single component, thereby providing a design and manufactur-
tional and functional gradation of both materials and structures. ing platform for imitating nature-inspired MMs and structures.
Several examples of nature-inspired structures and multi- In a recent study published in Nature Physics, Yasuga et al. [5]
materials (MMs) for inspiration of designing cellular metamateri- developed a two-step platform—FLUID3EAMS—that can create
als and multi-material additive manufacturing (MMAM) are collec- MM structures for scaffolds and several other applications. They
tively illustrated in Fig. 1. As captioned in the subsets of Fig. 1, validated the process by fabricating various structures, e.g., extre-
these exemplary cases demonstrate excellent performance by mely soft tissue-like architecture. Inspired by nature, Mirzaali et al.
combining the advantages of multiple materials with functionally [6] designed bioinspired functionally graded materials (FGM) to
graded structures. However, the objects designed by humans exhi- investigate the deformation and fracture behaviors of continuous
bit simple structures and are manufactured using single materials. and hard–soft composites, which offer numerous applications in
Thus, they are not completely optimized for specific applications high-tech industries such as aerospace and soft robotics. In several
because of the unique challenges and limitations in design and other studies, the nature-inspired multi-material fabrication con-
conventional manufacturing methods [1]. As additive manufactur- cept has been adopted to design and additively manufacture
ing (AM) and Design for AM (DfAM) provides unlimited freedom of objects for numerous applications, such as energy harvesting [7],
design and layer-by-layer or particle-by-particle deposition of soft sensors [8], lightweight automotive parts [9], and denture
material, they are deemed as the most potential candidate for 3D printing [10]. In the last six years, over 200 Scopus and SCI-
indexed research articles have been published in the research
domain of MMAM.
Based on the significance and progress of MMAM research, sev-
eral reviews have been reported on specific aspects. However, a
complete and systematic review encompassing the advancements
in this research domain in the past six years is yet to be prepared.
Wang et al. reviewed the interface characteristics, manufacturing
challenges, and applications of MM structures fabricated using
the laser powder-bed fusion (LPBF) process [11]. Goh et al.
reviewed MMAM and the 3D printing process of electronics by
exploring the fabrication techniques, design considerations, and
challenges of multilayered electronics [12]. In the context of recent
advancements in technologies and applications, Collado et al. [13]
and Zheng et al. [14] reported a systematic review of MMAM of
polymer materials. Wei and Li (2021) reviewed the MM powder-
deposition mechanism, molten pool behavior, and process param-
eters of LPBF [15]. Zhang et al. [16] and Loh et al. [17] reported pro-
gress in design, modeling, and AM technologies capable of
fabricating FGM. Blanco et al. reviewed the applications of MMAM
in the automotive and aeronautical industry [18]. Ravanbakhsh
et al. comprehensively assessed the emerging technologies for
MM bioprinting [19], following which Viola et al. [20] reported
the progress on multimaterial biofabricated tissue structures in
the same year. More recently, Mitchell et al. published a review
on 4D printing [21]. Ha and Lu reviewed various bioinspired mate-
rials and structures for energy absorption applications [22]. Earlier,
the AM of MM structures was reviewed by Bandyopadhyay and
Heer [23].
To the best of our knowledge, the progress of MMAM in the
Fig. 1. Nature-inspired structures and multi-materials (with composition and
structural variations) inspire the design of cellular metamaterials and multi-
recent years has not yet been comprehensively reviewed.
material additive manufacturing. Consequently, several aspects of MMAM have not been adequately

2
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

discussed, such as MM design and analysis, recent technological


advancements, design, and MM-related developments in finite ele-
ment analysis software, post-processing, and strengthening meth-
ods for MMAM. Thus, the potential applications, technical issues,
limitations of MMAM should be comprehensively discussed to
ensure the sustainability of this technology.
This article aims to provide a comprehensive and systematic
review of all the aspects of the research area of MMAM. Following
the introduction and background overview provided in this sec-
tion, the methodology and procedure of data acquirement and
analysis are described in Section 2. The types of multi-materials,
including metal–metal, metal–ceramics, polymer–polymer, and
other combinations, are reviewed in Section 3. The multi-
material modeling, numerical simulations of objects, and struc-
tures using MMs are elaborated on in Section 4. The AM processes
Fig. 2. Number of articles published annually on multi-material additive manu-
capable of manufacturing multi-materials, research gaps, and lim-
facturing from 2017 to April 2022.
itations of these processes are discussed in Section 5. In Section 6,
the post-processing of MM-manufactured objects are discussed.
Thereafter, the MM applications and potential opportunities in
several industries are illustrated in Section 7. The limitations and 3. Multi-materials for additive manufacturing
critical challenges of adopting MMAM are discussed in Section 8.
Finally, the conclusion of this review and overall future trends in Nature offers excellent functionalities and performance by
the MMAM research domain are summarized in Section 9. exploiting the combinations of excellent structures and composi-
tions of materials [1]. Inspired by nature, such excellent personal-
ized performance in engineered designs can be realized through
emerging AM technologies, especially MMAM techniques that
can enhance the performance of 3D printed components by
2. Methodology increasing its functionality and complexity with the addition of
multiple materials or varying compositions of the same material
The literature search methodology adopted in this review arti- within a single component. Thus, MMAM offers several opportuni-
cle follows several literature search criteria, including literature ties for designing complex, functional, highly personalized, and
inclusion and exclusion criteria, as listed in Table 1. An initial high-value products with improved properties, as depicted in
search of the keywords listed in Table 1 displayed 27,230 research Fig. 3. Simple and general combinations of the materials fabricated
publications, but not all studies were related to MMAM research. using a suitable AM process based on material types and the pos-
Thus, an inclusion–exclusion criterion was defined in which all sible improvements in properties are presented in Fig. 3. This inte-
publications were filtered to increase the relevancy and reduce gration of materials at various scales can tailor the properties of the
the number of searched articles. Furthermore, in-depth reading components, including electrical, thermal, mechanical, optical, and
and filtering were conducted on article titles, abstracts, keywords, multifunctional properties [24,25].
conclusions, materials, and methods sections. Consequently, 205 As summarized in Fig. 4, almost all types of materials have been
articles relevant to MMAM were screened, which primarily focused utilized in MMAM. The materials combinations being studied
on multi-material technology development, mechanical property either pertain to the same category (e.g., polymer–polymer) or
investigation, types of material, design, and structure, and printing two distinct categories (e.g., polymer–metal). According to the ana-
parameters. lyzed literature, the two most widely investigated categories of
The number of articles on MMAM published each year from materials include polymers and metals, studied in 76 and 66 pub-
2017 to April 2022 is charted in Fig. 2, which indicates an increas- lications, respectively. Among polymers, the most commonly
ing trend throughout the search period and implies the growing investigated MM include PLA [26-39], ABS [32,39-46], PEEK
significance of MMAM research and development. [30,47,48], and PET [36] to improve strength, stability, functional-
ity, etc. For metals, the majority of research on MMs has been con-
Table 1
ducted on alloys of titanium, copper, aluminum, and steels for
Summary of literature search and inclusion–exclusion criteria included in present improving the functionality of designed components as well as
study. enhancing the characteristics such as hardness, conductivity, and
Literature searching criteria
magnetic properties, wear resistance, strength, and thermal perfor-
mance. As elastomers, e.g., TPU [32,37,38,45] and hydrogels, are
Language English
the least studied multi-materials. TPU is a difficult-to-print elas-
Publication period 2017 to 2022 tomer due to incomplete melting, material feeding issues chal-
Date of search May 2022
lenges due to buckling, higher viscosity and melt strength, and
Bibliography sources Web of Science (WoS): Elsevier, Emerald, Wiley,
Springer, Sage, Nature, JAMA, Taylor and Francis, incomplete integration between layers and rasters [49]. Moreover,
Science, MDPI, ASME databases. precise AM of hydrogels is also difficult to achieve due to their
Search keywords Dual materials, multimaterial, multi-material, large gelling temperature ranges, and low viscosity [50]. Therefore,
multiple material additive manufacturing, multi-
most of the aspects of the combinations of these materials require
material 3D printing, multi-material additive
manufacturing further investigation.
Inclusion and exclusion criteria The selection of a suitable MMAM method for manufacturing
Publication type Original research articles multifunctional components requires a comprehensive under-
Scope Properties studied, printing parameters, material standing of the advantages and limitations of each AM process,
types, design and structure types, technology
as described in Section 5. The fundamental concerns for MMAM
development.
include the successful delivery of multiple materials and the strong
3
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Fig. 3. General classification of Multi-materials and their respective improvements in properties.

Fig. 4. Materials combinations utilized in additive manufacturing of multi-materials literature.

bonding between materials with various types and compositions. and allows lattice design, which is impossible with conventional
The possible variations in material types and compositions studied manufacturing methods (Fig. 5b). To overcome the multiple pow-
with the opted MMAM process are outlined in Table 2 and detailed der feeding and weak bonding limitations during the LPBF process,
in the following subsections. Demir et al. proposed an in-house developed in-situ powder mixing
unit to fabricate pure Fe, Fe/Al–12Si (volume ratio 55:45), and Al–
3.1. Metal–metal 12Si multi-material products using LPBF, which exhibited ade-
quately strong bonding because of mixed Fe and Al–12Si composi-
Although numerous AM methods exist for printing metals, most tion acting as the interface and improved hardness [78]. Although
of them are limited to the fabrication of single-metal composition Demir et al. obtained promising results, the processability of Fe/Al–
at a given time owing to machine-specific restrictions such as a 12Si multi-material displayed a lack of dimensional accuracy
single powder-feeding unit. Thus, a new powder-feeding design (Fig. 5c). Wei et al. studied two metallurgically compatible Ti5Al2.5-
with multiple materials feeding sources can resolve this limitation. Sn and Ti6Al4V processing using LPBF [75]. A defect-free interface
Otherwise, premixed powders can be used for printing multifunc- with an elemental diffusion zone exhibited good-quality bonding.
tional components (Fig. 5a) [119]. Other material- and process- Nonetheless, Scaramuccia et al. reported severe cracking between
related limitations include dimensional accuracies and post- Ti6Al4V and IN718, indicating metallurgical incompatibility that
process requirements. Overall, the major challenge is the bonding results in brittle intermetallic phase formation [87].
of dissimilar materials. Therefore, the compatibility of the MMs Among other MMAM methods, the directed-energy deposition
is an essential consideration for MMAM. (DED) process has garnered considerable research attention owing
The PBF process was applied to fabricate 316 L/CuSn10 MM and to its capability for manufacturing large-scale components with a
enhance its structural and functional properties for applications in high building rate and no requirement for powder recycling
automobile, rail, and aviation industries [120]. The traditional fab- (Fig. 6a). Moreover, multiple or mixed powder-feeding systems
rication of steel–copper MM components involve the following are possible (Fig. 6a&b). Therefore, SS316L/IN718 (Inconel 718)
steps: welding, hot-rolling, and compound casting. However, multi-material components have been fabricated by DED to com-
MMAM can produce 316 L/CuSn10 components with improved bine the high strength of IN718 and adequately high ductility of
mechanical properties in a single step under the optimized process SS316L in a single product [79]. The results revealed the brittleness
condition that prevents the occurrence of cracks at the interface of the obtained IN718, which conveniently facilitated crack
4
Table 2

A. Nazir, O. Gokcekaya, K. Md Masum Billah et al.


MMAM materials and their compositions with applied AM processes and properties studied in analyzed literature.

Material composition AM process Properties studied Refs. Material composition AM process Properties studied Refs.

Polymer–polymer
-ABS FDM -Interfacial bonding [41] -PLA FDM -Tensile [51]
-TPU -ABS
-Nylon FFF -Thermal [30] -PLA FFF -Fracture toughness [52,53]
-Carbon fiber -Mechanical -Nylon
-PC/ABS FFF -Fracture toughness [54] -PLA FFF -Impact resistance [36]
-PE -TPU
-PET
-ABS – HIPS FDM -Tensile [32] -PCL FDM -Printability [55]
-ABS – PLA -PLA -Porous scaffolds
-PLA – HIPS
-ABS – HIPS – PLA
-Difunctional urethane acrylate oligomer DLP -Modulus [56] -Nylon ME -Thermal expansion [57]
-Ultimate strength -PVA -Strength/ stiffness
-Elongation -Thermal stress
-Silicones SLA -Shore hardness [58] -Aramid fibre (AF) MJF -Ultimate tensile strength [59]
–PA12 -Young’s modulus
-TPE SLS -Poisson’s ratio [60] -PEEK FFF -compression [47]
-PA12 MJF -Thermal expansion -CFR-PEEK
-PLA FDM -Printability [61] -ABS FDM -Orthosis design [62]
-ABS -TPU -Printability
-HIPS
-PET FDM -Poisson’s ratio [63] -TPU - PLA FDM -Tensile [26]
-polycarbonate (PC) -Thermal deformation
-PLA - CPE
-CPE - TPU
5

-Monomers SLA [64] -Albumen /alginate/gelatin ME -Compressive and tensile strength [65]
- poly(ethylene glycol) diacrylate (PEGDA) -Young modulus -Hydrogel
-initiators -Hardness
-ABS FDM -Compressive and energy absorption [42] -Polymers FDM -Digital anisotropy [66]
-TPU -Drying adhesives
-Thixotropic fluids
-alginate PJ -Printability [67] -ABS FFF Strength and stiffness [45]
-methylcellulose -Rheological properties -Short carbon fiber (SCF)
-Sodium alginate/ Methylcellulose -Viscosity
-UV curable ME -Printability [68] -CF nylon FFF -Elastic stiffness [30]
-silicone inks -flow parameters to optimize the mixing -Carbon PEEK-PLA -Poisson’s ratio
process -Coefficient of thermal expansion
-PET film SLA -Heterogeneous properties [69] -ABS FDM -Tensile Strength [70]
-embedded piezoelectric elements -carbon fiber -Modulus
-Porosity
-Resins of different mechanical property SLA -Mechanical properties [10] -PCL FDM -Osteoconduction [71]
-Material waste -TCP -Bioactivity
-Fabrication time

Materials & Design 226 (2023) 111661


-biopolymers ME -Shear thinning ratio [72] -ABS FDM -Tensile [44]
-hydrogels -Viscosity -polycarbonate (PC)
-chitosan -Ultimate tensile stress
-cellulose -Elongation at break
-pectin

(continued on next page)


A. Nazir, O. Gokcekaya, K. Md Masum Billah et al.
Table 2 (continued)

Material composition AM process Properties studied Refs. Material composition AM process Properties studied Refs.
-Agilus30 (FLX935) MJ -Compressive and tensile [73] -silicone rubber Hybrid -Density [74]
-Vero Magnet (RGD852)) -Geometric -silicone/ethanol composite -Tensile and tear strength
-Dimensional accuracy analysis -Elongation
-Hardness
-Tensile stress and strain
-Stiffness
-Acrylonitrile Styrene Acrylate (ASA) FFF -Ultimate stress [29]
-PETG -Elastic
-Modulus
-Bonding strength
-Hardness
-Stiffness
Metal–metal
-Ti5Al2.5Sn LPBF -Strength [75] -Al-12Si LBF -Interface bonding [76]
-Ti6Al4V -Interface bonding -Al-3.5Cu-1.5 Mg- -Flexural
1Si -Tensile
-Nanohardness
-Zinc Fusion -Printability [77] -Fe LPBF -Crack propagation [78]
-Aluminum bonding -Al-12Si -Microhardness
-Copper
-SS316L DED -Ductility [79] -AlSi10Mg LBF -Tensile strength [80]
-Ti6Al4V -C18400 -Flexural strength
-SS316 DED -Magnetic property [81] 316L LBF -Metallurgical bonding [82]
-SS430 -C18400 -Tensile strength
-Micro harness
-aluminum PBF -Chemical etching [83] 316L LPBF -Printability [84,85]
-silicon -CuSn10 -Hardness
6

-Al – -Young’s modulus [86] -Ti6Al4 V LPBF -Defect formation [87]


-Steel -Physical density -IN718 -Micro harness
-Poisson’s ratio
-Al – -Stress [88] -steel SLM -Roughness [89]
-Steel -nickel -Hardness
-copper
layered 50Cr6Ni2 DLD -Wear resistance [90]
-Stellite X-40 composite -Corrosion resistance
Metal–polymer
-SS316L -LPBF -bone implant interface [91] -ABS FDM -Thermal conductivity [92]
-Cu10Sn -ME -Fe -Tensile strength
-PLA -Cu

-Cu-reinforced FDM -Mechanical property [93] -Soft elastomer resin Hybrid [43]
-PLA -Conductive ink
-ABS
-Photocurable acrylate-based

Materials & Design 226 (2023) 111661


polymer
-carbon-fibre thermoplastic composite Hybrid -Shear deformation [94] -Bismuth telluride Extrusion Thermoelectric property [95]
-aluminum adherent -TE inks
-Chalcogenide metallic binders

-Maraging steel ME -Magnetic property [96] -Resin FFF -Surface shape [97]
-PLA -Metal

316L LBF -Printability [91] -Metal DIW -Young’s modulus [98]


-CuSn10 -Rubber -Density
-PLA) -Plastic -Poisson’s ratio
-Porosity
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al.
Table 2 (continued)

Material composition AM process Properties studied Refs. Material composition AM process Properties studied Refs.
316L LBF -Tensile [99]
-CuSn10 -Shear strength
-PA11
Ceramic–ceramic
-silica sand SLS -Surface roughness [100] -Boron carbide (B4C) DIW -Yield stress [101]
-zircon sand -Compactness -Silicon carbide (SiC) -Viscosity
-Hardness
-Shear
Metal–ceramic
-Al2O3 LOM -Mechanical property [102] 1.2367 tool steel SLM -tensile strength [103]
-Cu–O -Electrical property -ZrO2 + Al2O3 -adhesive strength

-Ti6Al4V LPBF -Hardness [104] -SiC LBF -surface roughness [105]


-TiB2 -Wear 316L
-Cp-Ti LENS -Wear [106] 16NCD13 LC -Hardness [107]
-CaP -TiC -Defects analysis
-Fe ME -Osteosynthesis [108] -CpTi LENS -Wear [109]
30CaSiO3 -Zr -Cell Attachment
-Hardness
-zirconia–alumina SLM -Tensile strength [110] -IN718 LENS -Thermal conductivity [111]
-steel -Adhesive strength -Cu -Diffusivity
-TiB2 SLM -Nano hardness structural stabilities [112] -ceramics selective laser -Compression -Density [113]
-Ti6Al4V (Bi2Mo2O9) burnout -Porosity
-Ag -Viscoelastic properties
Polymer–ceramic
-PEEK SLS -Compressive thermal properties [48]
-b-tricalcium phosphate (b-TCP) bioactivity,
7

-PEEK/b-TCP/PLLA -biodegradability
-cytocompatibility.
Photopolymer–photopolymer
-TangoPlus (FLX980) MJ -Young’s modulus [114] -Vero Plus PJ -Flexibility and shock absorption [115]
-rigid VeroClear (RGD810) -Tensile strength and elongation at break. -Agilus
-acrylic-based photopolymers -Vero White MJ -Young’s modulus [116]
Plus (VW) -Fracture strength
-Ultimate tensile strength -Bond strength -
Stiffness
Polymer–wood Polymer–glass
-Wood Hybrid -Rigidity [117] -Polyethylene MJ -Impact-Transmitted force and [118]
-polymer -Opacity -Glass fibre penetration
-Tensile strength -Carbon fibre or Kevlar
-Flexural strength -Low-density polymer
-Elongation
-Elastic modulus

Materials & Design 226 (2023) 111661


A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Fig. 5. (a) Illustration of LPBF processing premixed dissimilar powders [119], (b) process-parameter optimization of 316L/CuSn10 multi-material processed by LPBF prevents
interface cracking under optimum process condition and successfully materializes multi-material lattice fabrication [120], (c) Fe/Al–12Si multi-material processing by LPBF
exhibiting dimensional inaccuracy but sufficiently strong bonding [78].

Fig. 6. (a, b) Schematics of multi-material DED processing [119], (c, c’) tensile performance of DED processed SS316L/IN817 multi-material with corresponding stress
distribution [79], (d) SS316/SS430 multi-material with selective magnetic functionality fabricated by LENS with adequate interface bonding [81].

growth. However, the other half of the product fabricated by realize a single structure composed of stainless steel 316 (SS316)
SS316L manifested ductile properties and supported plastic strain and SS430 with selective magnetic functionality [81].
during tensile deformation (Fig. 6c), representing the multifunc-
tionality of the SS316L/IN718 MM component. LENS method with 3.2. Metal–ceramic
multiple powder-feeding system was applied to fabricate mag-
netic–nonmagnetic bimetallic structure with compositional grad- Currently, the MMAM with metals and ceramics are still in the
ing to enhance the bonding between dissimilar metals (Fig. 6d), developmental stage. Forming a strong bond between metals and
8
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

ceramics is extremely challenging because of the high melting been extensively researched and applied by AM technologies as a
point mismatch and thermal expansion, which results in thermal filament material. The low working temperature of the FDM tech-
stresses. At sufficiently high temperatures, the ceramic melt can nique enables the use of materials with low melting temperatures,
attain flowability that causes metals to evaporate, creating difficul- e.g., PLA [124]. Considering the advantages of PLA with the
ties in controlling the desired multi-material composition. More- mechanical strength of metals, metal-polymer MMAM has been
over, the thermal stress and significant difference in thermal implemented for bio-inspired soft robot fabrication [125]. How-
expansion coefficients promote delamination or cracks between ever, the insufficiently low process temperature fails to form a
metals and ceramics, jeopardizing the mechanical strength and strong bonding between metals and polymers. Therefore, metal–
limits the structural application of the metal–ceramic MMAM polymer MMAM has primarily focused on using metal–polymer
components. hybrid filament to enhance the properties of polymer materials.
Laminated object manufacturing (LOM) is a sheet lamination Herein, metals are considered fillers to improve the functionality
method that can successfully fabricate metal–ceramic structures of polymers. Nonetheless, the dearth of research on mechanical
via its low-temperature processing (Fig. 7a) [119] and prevention properties related to these polymer filaments incorporating vari-
of thermal stress-related limitations. The composite structure of ous filler metals is concerning. Upon increasing the metal ratio in
Al2O3/Cu–O was fabricated using LOM with applied heat treat- metal–polymer MMAM, shrinkage and pore formation emerge as
ment. The results displayed dense material with appropriate the main limitations.
mechanical and electrical properties, while ensuring reasonable Kottasamy et al. studied Cu-reinforced PLA using the FDM
bonding quality (Fig. 7b) and the fabrication of geometrically com- method [93]. With 25 wt% Cu addition, Cu–PLA composites exhib-
plex components such as gears (Fig. 7c) [102]. ited the most suitable mechanical properties and implied a possi-
Recent studies have investigated a mixture of commercially ble alteration of the properties with the adjustment of the metal
pure Ti with 1.6 wt% Bromide (B) powder processed using LENS filler content. Diaz-Garcia used maraging steel as a filler for PLA
[121] and a mixture of Ti6Al4V powders with 3 wt% TiB2 powders to induce magnetic functionality within the multi-material fabri-
processed using PBF [104]. Both MMAM processes improved the cated via the extrusion AM method [96]. Upon increasing the metal
hardness and wear properties of titanium. Furthermore, LENS fab- ratio to 85 wt% with 15 wt% of the polymer [126], the products
rications of Ti6Al4V with 5 wt% hydroxyapatite (HA) [122] and Cp– printed with the bronze–PLA filament exhibited approximately
Ti with 10% calcium phosphate (CaP) [106] were studied for 20% shrinkage and significant porosity after sintering (Fig. 9a).
biomedical applications. The results exhibited enhanced wear Although the literature on metal–polymer MMAM is limited, a
properties with the formation of the corresponding CaTiO3 and combination of the fused filament fabrication, extrusion-based
Ca(PO4)3 phases as a tribological protection layer on the biomate- AM method, and electroforming process has successfully demon-
rial surface. However, controlling the reaction phases, e.g., Ti5P3, strated a metal–plastic multi-material structure [128].
CaTiO3, and Ca(PO4)3, is crucial for the mechanical performance As discussed earlier, the realization of metal–polymer bonding
of biomedical components because these fragile phases induce vul- with a single AM process is challenging. Therefore, utilizing two
nerability to crack due to the thermal differences in metal and distinct AM processes to manufacture metal–polymer structures
ceramic. Furthermore, the material extrusion MMAM method is proposed (Fig. 9c&d) [91]. Several MMAM components com-
was applied to fabricate lattice bone implants composed to Fe- posed of SS316L, Cu10Sn, and polymer (PLA, PET) were successfully
30CaSiO3 (in wt%) [108]. Fe-30CaSiO3 biomaterial significantly fabricated through integrated extrusion and PBF methods, whereas
improved the in-vivo osteosynthesis compared to pure-Fe lattice poor metal–polymer bonding and surface quality posed a signifi-
structure and exhibited promising results for bone cancer therapy cant problem. However, the metal–polymer interface exhibited
(Fig. 8b). reliable strength with an interlocking design, indicating adequate
infiltration of the polymer into both macroscopic design and
3.3. Metal–polymer microscopic mechanical structures.
The IN625 alloy fabricated using the binder jetting process with
AM processing of polymers has been extensively studied an intentional reaction during the debonding of polymer resulted
because of their low temperature and more manageable processing in the formation of a strengthening Cr3C2 phase (Fig. 9b) at the
condition than metals, which are applied in medical, automotive, polymer binder–metal powder interface [127]. This confirmed
and aerospace industries [123]. Among various polymers, PLA has the significance of the reaction between the polymer and metal

Fig. 7. (a) Illustration of multi-material sheet lamination process [119], (b) successful fabrication of Al2O3/Cu–O sandwich structure by sheet lamination process with
interface observations, and (c) demonstrative gear shape fabrication [102].

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Fig. 8. (a) Illustration of multi-material processing of premixed powders by material extrusion [119], (b) 3D-printed scaffolds with gradient composition (left to right: CaSiO3
100%, 40%, 30%, 20%, 10%, and 100% Fe) and promising bone regeneration results of MMAM processed 30% CaSiO3/70% Fe scaffold [108], (c) MMAM processing metal–metal–
polymer with mechanical interlock to enhance metal–polymer bonding and (d) its successful application to bone implant [91].

Fig. 9. (a, b) Illustration of metal-reinforced polymer extrusion and premixed multi-material binder jetting, respectively, with interface and porosity observations [126,127].

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that can alter the properties of the final components. To achieve The major process limitations related to the equipment are sta-
the goal of producing higher-quality metal components, future ted as follows: (a) reduction of the available printing area and cal-
research should focus on optimizing the metal–polymer ratio, ibration of the extrusion heads; (b) precise alignment of the two
diminishing the differences in the melting points of metal–poly- (or more) extrusion heads during the deposition process. For com-
mer MMs, and optimizing the sintering conditions to minimize ponent design, multi-material printing enables the development of
the porosity of the printed components [129]. various geometrical interfaces in the component. However, dis-
crete material properties at the interface produce inferior bonding
3.4. Polymer–polymer strength compared to the bulk material strength. Moreover, the fil-
ament’s residence interval inside the extruder forms an additional
In the context of the material extrusion AM, several materials aspect of the design-related challenge. In general, the residence
have been used to fabricate multi-material yet monolithic compo- interval impacts the thermophysical and rheological properties of
nents. The MMAM process can yield functionally gradient struc- the extruded material and does not provide sufficient opportuni-
tures with multicolor regions/shades and spatial variations of ties for optimization through the flow rate in a dual extrusion sys-
mechanical, thermal, electrical, and optical properties. Depending tem. Thus, the plastic tends to drool more often in the traditional
on the application and requirement of the manufacturing process, extrusion system [131].
various combinations of the polymers (refer to the related section The materials-related challenges are associated with the chem-
of Table 2) can be observed in the analyzed literature. Thermoplas- ical structures and formulation of the thermoplastics used in the
tic polymer chains offer considerable challenges in mobilization via extrusion process. The discrete polymer materials exhibit distinct
chemical reaction, which can facilely yield the counterpart of ther- chemical structures, i.e., thermoplastic materials often comprise a
moset plastics. The combination of the thermoset and thermoplas- mature polymer chain, unlike the thermosets that execute the
tic polymer is seldom used in the MMAM system. The dominant crosslinking of the open monomer and dictate the curing process.
use of thermoplastic polymers in hot-melt extrusion-based system Dissimilar plastic materials (refer to Fig. 10) can create problems
promoted the growth of the MMAM system across diverse research associated with the mismatch between the thermal expansion
areas, including the study of the affinity of dissimilar materials and coefficients. Therefore, dissimilar shrinkage upon cooling eventu-
their mechanical properties in fabricated yield of a monolithic ally results in distortion and low dimensional stability of the com-
structure. ponents. Furthermore, the mechanical integrity expected at the
The interface formed between the discrete materials at their interfaces between various printed materials reduces in case of
geometrical boundary is regarded as the critical element in multi- chemical incompatibility or low chemical affinity [36].
material 3D printed components, which varies with the properties
and printing conditions of the materials [130]. To date, no signifi- 3.5. Functionally-graded multi-materials
cant research work has been reported regarding multi-material
fused-filament fabrication-based AM, focused on the relationship FGMs offer remarkable applications in which the service condi-
between printing conditions and dissimilar materials interface tions and material requirements vary spatially throughout the
quality in comparison to those of standard (single material) extru- component and a material gradient is required [133]. As thermal
sion 3D printing [36]. The scarcity of information concerning gradients are desired in components in aerospace and aviation
multi-material extrusion-based 3D printing persists to be an unex- applications, engineers and designers leverage the interaction
plored area, specifically regarding the limitations of equipment, between the material properties. For instance, the temperature in
component design, and printing materials. the center portion of a turbine blade is relatively low, and thus,

Fig. 10. Representative polymer–polymer MMAM example, (a) ABS and TPU specimen fabricated using FFF [41] (b) ABS and PC parts fabricated using modified FFF system
[130], (c) functionally graded multi-material components fabricated in FFF system using ABS and PC [132], and (d) FFF of wrist orthosis using ABS and TPU [62].

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the center portion is required to exhibit adequate tensile strength functions and properties of the final component, which aims to
and fatigue resistance, which is designed to obtain specific physical improve the interfacial bonding between dissimilar or incompati-
or chemical performances [134]. Thus, the functional grading of ble materials, as depicted in Fig. 11b. A compositional transition
two or more materials is required [133]. FGMs can be classified from a dispersed to an interconnected second-phase structure—
as follows: (a) FGMs via construction, such as addition of layers layered and graded with discrete compositional parameters or
to manufacture a component, and (b) FGMs via mass transport or smooth concentration gradients—can be obtained to eliminate
diffusion to create a material gradient [133]. the severe properties of two dissimilar materials. Thus, this
Current AM methods can adapt to the constructive method of method can avoid the common failures of conventional multimate-
preparing FGMs with infinite combinations of ceramics, polymers, rial AM, e.g., delamination and cracks induced by surface tension
metals, and even composites designed with complex geometries. owing to the discrete variations in material properties (Fig. 11a)
The fundamental goal of using AM in FGM production is to produce [17].
performance-based freeform components driven by their gradient After a three-dimensional fusion between two materials using a
in material properties [135]. In the DED process, also known as dynamic gradient, the printed component exhibits the optimal
laser metal deposition (LMD), the powder is fed into the melt pool properties of both materials. It can be transitional in weight yet
under a moving laser, and it can be used for fabricating FGMs by retain its toughness, wear resistance, impact resistance, or physi-
varying the powder composition between layers. This method cal, chemical, biochemical, or mechanical properties. Heteroge-
can be conveniently managed using conventional or robotic DED neous mixtures of materials no longer require a compromise of
machines equipped with two or more powder feeders [133], and their intrinsic properties to achieve the desirable properties of
thus, it has been utilized for preparing graded structures of several the component [17]. MMAM of FGMs can be varied across material
alloys such as titanium alloys, nickel alloys, steels, and metal combinations of metal–metal [133,134,136,138,139], metal–ce-
matrix composites. In particular, DED offers several benefits com- ramic, ceramic–ceramic [140], and polymer-based materials
pared with traditional manufacturing techniques, such as casting [141]. The FGMs developed using MMAM technology along with
or powder metallurgy. The components are constructed layer-by- their potential application areas are listed in Table 3.
layer, reproducing interior features and channels design. Simulta- As observed in Table 3, the potential application areas of addi-
neously, it does not require special tooling such as that involved tively manufactured functionally graded multi-materials vary in
in casting and powder metallurgy. Therefore, it can efficiently fab- aerospace, military, biomedical, and automotive industries. Certain
ricate complex geometries and coatings [136]. As FGMs are classi- examples of the developed functionally graded MMAM compo-
cal MM structures involving compositional gradient, DED can nents are illustrated in Fig. 12.
rapidly produce MM components when coupled with multinozzles. In addition to these applications, certain parts of die-mold
During DED, multinozzles can satisfy this requirement by adjusting applications can be produced by MMAM [139]. Although FG mate-
the powder types fed and their relative percentages. Compared rials were initially designed for heat-resistant applications, they
with other AM processes, such as PBF, this is a beneficial advantage can be employed to control the deformation, pressure, wear, and
of this method [136]. Recently, scholars have attempted to produce corrosion, as well as to replace sharp material transitions in which
FGMs using PBF–AM techniques [137]. high stresses are generated. Traditionally, their application was
Functionally graded MMAM addresses the MM aspect through confined to the development of ceramic coatings and composite
the dynamically generated gradients approach or complex mor- materials [139], and the grading of metallic materials has not
phology. The geometry and material arrangements control the received considerable attention. However, with the development

Fig. 11. (a) Conventional multi-material additive manufacturing vs. (b) functionally graded MMAM [17].

Table 3
Literature review of functionally graded MMAM studies.

Reference Materials/Products AM Process Potential Application Areas


Pelz et al. [140] SiC-B4C ceramics Direct ink writing (DIW) Ballistic applications
Lee et al. [141] Biopolymer composites Extrusion based Biomedical applications, Tissue engineering
Carroll et al. [133] AISI 304L-Inconel 625 DED Aerospace, Nuclear power generation
Ren et al. [134] Ti6Al4V-Ti6.5Al3.5Mo1.5Zr0.3Si alloys DED Compressor blisks
Xu et al. [138] AISI 316L-Ti6Al4V DED Aerospace industry
Hengsbach et al. [137] AISI 316L-H13 SLM Aerospace and Biomedical industries
Hasanov et al. [45] Carbon fiber reinforced ABS FFF Aerospace and Automotive
Markandan et al. [142] Cu-PE foam Selective heat melting Electromagnetic field devices, Graded index lenses
Li et al. [136] AISI 316L-Ti6Al4V DED Aerospace, Nuclear, and Chemical industries
Ostolaza et al. [139] AISI 316L-H13 DED Die and Mould industries

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Fig. 12. (a) a continuous FG carbide-based sample produced via DIW [140], (b) deposited stainless steel-superalloy sample [133], (c) titanium-based FG deposit [134], (d) two
variations of 316L-H13 deposition [137], (e) CuO foam fabrication with graded porosity [142], (f) hardness distribution in a 316L-H13 FGM [139]

of AM processes such as the aforementioned L-DED [139], the databases have resolved several of these aforementioned issues,
FGMs of complex metallic gradients of dissimilar alloys have several challenges must be addressed.
emerged. Obtaining good metallurgical bonds between various
alloys is not trivial. Complete solubility over all compositions and 3.6. Properties studied
temperatures is uncommon in binary alloys, and it is much more
complex in ternary or multicomponent alloys [139]. This issue From the literature reviewed thus far, we have identified that
might be addressed by introducing compositional gradients. only a limited number of materials in each category (Fig. 4) can
Aremu et al. [143] used AM to develop functionally graded lattice be utilized for MMAM. Therefore, a customized and optimized
structures with variations of cell properties in the structure. object cannot achieve the required characteristics if it is manufac-
Nonetheless, several challenges existed, such as controlling numer- tured using either a single material or a combination of unsuitable
ous variables, fluctuations in thermal fields, and AM process opti- materials. Thus, the MM additive manufacturability of a wide
mization for the fabrication of FGMs. Although the development range of materials (under each category of materials in Fig. 4) is
of artificial intelligence techniques, design and development of crucial for achieving the complete benefit of the products fabri-
AM process diagnostic methods, and creation of thermodynamic cated using MMs.
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A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Fig. 13. Properties of multi-material components/samples investigated from analyzed literature.

4. Multi-material components design and analysis

4.1. Design and modelling

Multi-material AM can be referred to as multi-material func-


tionally graded additive manufacturing (MMFGAM) that considers
the aspect of multi-material gradients and/or complex morpholo-
gies. The arrangements of material and/or morphology gradience
govern the properties and functionalities of multi-material compo-
nents. In MMAM components, distinct boundaries can be elimi-
nated using a heterogeneous compositional transition or smooth
concentration gradients. The implementation of diverse materials
in integrated structures has improved functionality, reduced
weight, and adjusted the manufacturing processes by combining
assembly and production into a single processing step [144]. In
summary, the required properties can be designed by combining
multiple materials into a single integrated component.
The design of MM components can be classified based on sev-
eral materials combined into a single piece, as depicted in Fig. 14
[17]. According to the desired properties and functionality, the
material in a MM component can be distributed in several manners
Fig. 14. Design combinations of multi-material compositions. (a) Transition (Fig. 14(a–e)). Qiu and Langrana [145] have developed a computer-
between two materials. (b) Heterogeneous compositional transitional between aided design (CAD) system to provide high-quality tool parts dur-
two materials. (c) Transition between three materials. (d) Switched composition ing the multi-material AM process. In another study, Bhashyam
between various locations. (e) Combination of two materials in terms of density and
et al. [146] developed a CAD system with libraries of planning algo-
compositional gradation. [17]
rithms and material compositions, which can be utilized for
designing the compositions and geometries of multi-material
Various properties of multi-material additive manufactured objects.
components are presented in Fig. 13. Most studies have focused Multi-material workflow is similar to the AM workflow for sin-
only on the compressive and tensile properties (compressive/ten- gle material. However, the primary difference is that the MM pro-
sile stress, strain, etc.) of multi-material additive manufactured cess prioritizes the definition and allocation of the materials (of
components/samples. Although these components might possess every layer and/or every voxel) within the designed MM compo-
customized properties such as high functionality, a standardized nent [17]. In a recent study, Yao et al. [147] proposed a complete
design of the experiment has not been employed to investigate framework (Fig. 15a) for designing the multi-material components
the aforementioned (Fig. 13) properties. Owing to this issue, the that can be realized using AM process. Their design framework
results and methodologies of existing literature cannot be feasibly comprises four integrated modules, including the identification of
compared. As the majority of the existing literature has focused design requirements, primary material selection, AM method
only on basic properties, the essential properties of fatigue, 3D selection, multi-material composition, and determination of com-
printing, optical, impact/shock, flexural, and shear of MMAM com- ponent geometry. Furthermore, they compiled a database covering
ponents still require further investigation. the rules and guidelines, constraints, and capabilities of AM
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A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Fig. 15. Flowcharts of several designs for MMAM frameworks. (a) Design for MMAM procedure proposed by Yao et al. [147]. (b) Variant design workflow by Shin et al. [148].
(c) Material searching procedure and tools for multi-material solutions by Wargnier et al. [150].

Fig. 16. Numerical simulations for MMAM designs. (a) integrated DEM-CFD approach for 316 L/Cu10Sn deposition in PBF process [156], (b) DEM–CFD approach for IN718/
Cu10Sn in PBF process [157].

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processes, which assisted in decision-making in several MM pro- thermophysical properties. Furthermore, powder fraction can be
duct design phases. Their method can be a critical guide for design- conveniently adjusted via simulation instead of repeated experi-
ers working in the MMAM research area. Shin et al. [148] proposed ments for MMAM design.
two methods for designing the MM objects. The first method However, most simulation methods encounter several chal-
involves the generative design approach in which the material dis- lenges, such as large computational power requirements and diffi-
tribution and geometry of the object were optimized using homog- culty in acquiring multimaterial data. Among the available
enization design algorithms [149]. In the second approach, they software packages, only a few have features for designing and opti-
employed a knowledge-based variant approach (Fig. 15b) in which mizing MMs. Moreover, the existing FEM packages (Fig. 17) offer
the designers could use their personal experience and creative limited functionality for MMs. Currently, no software package
thinking to design a MM object. In another study, Wargnier et al. has been specifically developed for the design, optimization, and
[150] developed a conceptual procedure for designing MM objects simulations of MM-related studies. In the analyzed literature, most
by following material-searching approach (Fig. 15c) according to researchers employed a general software for design, optimization,
the functional requirements of the designed components. and finite element analysis (Fig. 17), e.g., ABAQUS [31,40,158-160],
However, multi-material design rules for each AM process and ANSYS [30,161,162], level set model [163], COMSOL Multiphysics
various materials still require to be studied. In addition, in-depth [7,164,165], Rhino [117,118,166], and MATLAB[98,167-171]. Nota-
studies should be conducted on the MM component design for bly, these software are not specifically designed for MM-related
each AM process. Furthermore, CAD software packages capable of research and development. Thus, significant development is
design, multidisciplinary optimization, and simulation methods required to apply these packages for MM-related investigations.
for MM components require further investigation.

4.3. Multi-material lattice structures


4.2. Advances in numerical simulations
The realization of an optimized and application-specific struc-
In the MMAM design procedure, numerical analyses are essen-
ture using AM [172-174] is possible only if their 3D models can
tial for improving the reliability of components, prediction of stres-
be created digitally using a software. Nevertheless, most commer-
ses, and parameter processing optimization. Owing to the
cially available software can design models with limited material
complexity of fusing MMs (shape of the melt pool, interface mor-
information, which is critical if the part is designed for fabrication
phology, and microstructures), study, observation, and simulation
of MMAM processes is difficult, computationally expensive, and
time-consuming, especially the fusion of multimaterials involving
metals [151]. Owing to the development of high-performance
computers and simulation workstations, the simulations can be
applied to predict and solve the MM-related problems, either
based on the material fusion mechanics or fabrication processes
[152]. In the DED and PBF processes, numerical simulations,
including the finite element method (FEM) [153], discrete element
method (DEM), computational fluid dynamics (CFD) [154], and
molecular dynamics (MD) were implemented for MMAM designs
to explain and predict the melt-pool phenomena such as convec-
tion, surface tension gradients, recoil pressure, vaporization, and
momentum losses in mushy zones [155]. The rack morphology
obtained after the solidification and elemental distribution of the
multi-material combination of 316 L/Cu10Sn and IN718/Cu10Sn
by DEM-CFD approach is depicted in Fig. 16a & b. Prior to experi-
ments, the MMAM design simulation simulates the inhomoge-
neous temperature distribution owing to the mismatch in

Fig. 17. Software packages used for design and finite element analysis of multi- Fig. 18. (a) Compression model of lattice structures designed using four distinct
materials components investigated in analyzed literature are as follows: ABAQUS, materials [176]. (b) Multi-materials 4D printable two-dimensional lattice structure
12; SolidWorks, 6; ANSYS, 5; MATLAB, 10; COMSOL, 6; Nastran, 2; Rhino, 3; that can morph into the shape of a spherical cap [177]. (c) Veroblack and Veroclear
LabVIEW, 3; OptiStruct, 4; Level set model, 2; Materialise, 2; SIMP Method, 3; materials are 3D printed using a DLP system [178]. (d) Multi-material designed
Python, 1; C++, 1; ImageJ, 1; Cura, 3. Kelvin lattice structure comprising three distinct materials [179].

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with MMs. This is a formidable task if the 3D models require to be


designed with the incorporation of lattice structures [175]. Wei
et al. [82] presented a manual data preparation procedure for
designing multi-material structures, although their method
requires a significant amount of manual work. Thus, their approach
cannot be employed for extensive production and industrial appli-
cations. Therefore, developing an advanced data interface and 3D
file is crucial for integrating the geometric and multi-materials
information, while simultaneously connecting to the AM system
for the fabrication of the MM structures [17].
Several researchers have studied the 3D-printed lattice struc-
tures of MMs using various materials. Zhang et al. [176] studied
the MM porous structures fabricated using SLM of four distinct
materials (CuSn, 316L, CoCrMo, 18Ni300) in a single specimen, as
depicted in Fig. 18a. They concluded that the compression behavior
of lattice structures can be improved by combining high-strength
brittle material and low-strength plastic material. Boley et al. Fig. 19. Additive manufacturing technologies used for fabricating multi-material
[177] studied 4D printing of heterogeneous morphable lattices components.
(Fig. 18b) to investigate design and fabrication issues. These struc-
tures with multi-material 3D printing can transform a diverse
range of applications. Recently, strut-based lattice structures were functional MMAM components, the selection of AM method for
fabricated using photosensitive materials [178,179] to realize elas- the fabrication is critical to ensure strong bonding between various
tomeric and rigid material properties in a single component. types and compositions of materials. Thus, the success of produc-
However, the design procedures of MM structures are very lim- ing such components primarily depends on the applied AM tech-
ited. Thus, they require new methods of computational modeling nology and the optimization of AM process parameters. Each AM
that contain detailed geometric (availability of a wide range of method offers its unique advantages and limitations for multi-
strut, surface, and stochastic-based lattice structures) and materi- material processing. The advantages and limitations of each AM
als information while managing material distribution at the voxel method for multi-material fabrication are examined in the follow-
level. Generally, voxel-level material distribution and modeling ing subsections and summarized in Table 5.
of structures are computationally expensive. Therefore, to reduce Each AM method is capable of MM fabrication with a recently
the amount of computation, Richards [180] proposed a modeling designed powder feeding system or powder mixing process. How-
system for representing material–geometry–topology using volu- ever, MMAM processes are still in progress to overcome the chal-
metric texture maps. This system can enable the designer to per- lenges caused by the selection of dissimilar materials. In
form modifications at the voxel level. Thus, the functional principle, the MMAM process bonds dissimilar materials to
representation-based modeling methods effectively describe enhance the performance of the structure, considering location-
multi-materials and incorporate complex lattice structures. specific properties. However, the bonding quality remains a major
issue for the success of MMAM processes. Lumpe et al. investigated
MM interfaces and determined that bonding quality relies on the
5. Multi-material additive manufacturing processes material combination [184], thereby rendering the selection of
MM for MMAM a critical consideration. Otherwise, the failure at
The high level of complexity of design and material distribution the interface zones can be detected [116]. Lately, studies have
in MM components creates insurmountable challenges for fabrica- focused on the gradient transformation in the material composi-
tion using traditional manufacturing processes. This limitation tion for MMAM processes to increase the interface bonding
motivated certain researchers to explore MMAM technologies in [45,132,185,186]. However, the effect of the material transition
the late 1990s [13]. Consequently, the continuous advancements zone and gradient composition remains unclarified. Accordingly,
in AM processes enabled almost all AM processes to fabricate com- the properties of the transition zone with respect to the combining
ponents with multiple materials in a single component. As multi-materials require further research [187].
depicted in Fig. 19, nearly all AM processes can fabricate multi-
materials. In particular, materials extrusion, PBF, and material- 5.1. Extrusion-based systems
jetting methods are most commonly utilized. Furthermore, the
vat-photopolymerization process, commonly referred to as SLA, Extrusion-based AM method is one of the most well-known AM
was the first AM technology and has been widely used for manu- processes (Fig. 19) that displaces the material feedstock through a
facturing MMs. A single AM technology encounters several chal- nozzle or multiple nozzles, enabling the construction of a 3D struc-
lenges during the combined printing of multiple materials. Thus, ture with multiple materials [188]. This process is capable of print-
hybrid AM technologies [94,117] have gained considerable ing various materials, including thermoplastics [189], metal-filled
research attention. In a recent study [43], researchers have inte- thermoplastics, composites [190], flexible elastomers [41], and
grated four AM technologies, namely, fused filament fabrication blended multi-material powder-based feedstock [132,185]. Similar
(FFF), direct ink writing (DIW), aerosol jetting (AJ), and inkjet (IJ), to the BJ method, the compatibility of the binder with the feed-
for developing a hybrid 3D printer that can rapidly fabricate com- stock material is crucial for the success of the process considering
plex multiple materials with a range of functionalities. unintended interactions/reactions during extrusion or sintering. To
Several commercial and laboratory-developed multi-materials ensure structural integrity, the components produced by the ME
3D printers commonly used for fabricating multi-materials compo- process require post-AM de-binding and sintering. Moreover, as
nents and complex lattice structures in the reported literature are the binder is mixed with the material instead of being extruded
listed in Table 4, which is a valuable reference for readers. on a powder bed, the powder recycling/reuse process is not
In general, a MMAM system includes the delivery of multiple required, thereby saving both time and cost. Nonetheless, the pre-
materials and layer bonding systems [183]. To construct multi- dominant disadvantage of this technology is the printing resolu-
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Table 4
Prevalent 3D printers for multi-material additive manufacturing.

Technology with 3D printer Company/institute (country) Multi-materials


refs.
DLP [56] D7 Plus Wanhao, China Urethane acrylates
Extrusion [95] Lab developed Ulsan National Institute of Science and Technology BiSbTe materials, TE inks
(UNIST), South Korea
SLS HORI H1 Beijing Huitianwei Technology, China TPE
[60]
PJ [115,117] Objet 500 Connex 3 Stratasys, USA VeroPlus, agilus, wood, polymer
DLP [181] Lab developed Tsinghua University Beijing, China Different compositions of Kaolin ceramic materials and
ceramic–metal MM
Extrusion [67] BioX 3D printer Cellink, USA Alginate and methylcellulose – Sodium alginate/
Methylcellulose
Extrusion [68] A custom-built 3D printer McMaster University Hamilton, Canada UV curable silicone inks
system
MJ [73,114] Stratasys J750 Stratasys, USA TangoPlus (FLX980, FLX935) and the rigid VeroClear
(RGD810, RGD852).
Two-photon Lab developed University of Nottingham, Nottingham, United Photopolymers
lithography [64] Kingdom
Hybrid [43] m4 3D printer 3D systems, USA Soft elastomer resin, Conductive ink, ABS, photocurable
acrylate-based polymer
DMLS [83] ProX200 3D Systems, USA AlSi12 powder: aluminum and silicon
Hybrid [98] Custom-built Imperial College London, United Kingdom Metal, rubber, and plastic
multimaterial 3D printer
Extrusion Objet1000 Stratasys, USA Biodegradable hydrogel composites
[166] (natural hydrogels, such as chitosan and sodium alginate)
VP [182] Lab developed Johns Hopkins University Baltimore, USA Hydrogel and gelatin methacryloyl (GelMA)
FDM [28] Commercial FDM printer 3D systems Multi-blended and hybrid-blended PLA matrix
FDM [44] CL1720 3D printer KAIROS ABS and polycarbonate (PC)
Hybrid [118] Objet Connex 3 260 Stratasys, USA Polypropylene, glass fibre, carbon fibre or Kevlar, and low-
density polymer
FFF [29] Ultimaker 3 dual-extruder Ultimaker, USA Acrylonitrile Styrene Acrylate (ASA), PLA, polyethylene
terephthalate glycol (PETG)

Table 5
MMAM processes and their general advantages and limitations.

Process Advantages Limitations


Powder bed fusion Dimensional accuracy Powder feeding system
Variety in material choice Powder recycling and reuse
Direct energy deposition Multi-material powder feeding Dimensional accuracy
Printable part size Surface roughness
Sheet lamination Low-cost Delamination
Time-efficient Inhomogeneity
Binder jetting Low-temperature process Post-processing
Binder compatibility
Powder recycling and reuse
Material extrusion Variety in material choice Post-processing
Binder compatibility
Material jetting High-speed process Clogging problem
Variety of material choice Low viscosity
Vat-photopolymerization High accuracy Material waste
Only photopolymers

tion that depends on the powder size and nozzle diameter. More- based feedstock filaments that transition through several thermal
over, products with a large aspect ratio and overhanging designs events, including heating and melting in a hot extruder, and are
are challenging to manufacture and require a consistent flow of extruded through a nozzle on the build platform in a layer-by-
feedstock and fast solidification. To this end, a multi-material feed- layer fashion. The FFF system often uses multiple extrusion heads
stock design is crucial. to deposit discrete thermoplastic materials and fabricate mono-
In extrusion-based MMAM systems, the novel hybrid metal lithic parts, as depicted in Fig. 20. Conventionally, the primary
extrusion and bonding method has been considered to fabricate material being extruded through an extrusion head is used as a
various multi-material systems in which Al-based components model material, and the secondary material being extruded
were highly studied, enable to produce continuous extrusion and through another head is used as a support material. However, a
good quality bonding by utilizing friction stir welding [191,192]. MM structure can be fabricated by utilizing dual extrusion heads,
However, fused filament fabrication (FFF) is one of the most com- and a secondary extrusion head can be employed for another ther-
monly used extrusion-based AM systems (several extrusion-based moplastic or various materials (e.g., carbon fiber) to produce com-
systems are listed in Table 4). Among other AM systems, the FFF is posite components. A representative example of a typical multi-
the most adopted system. In particular, it uses thermoplastic- material FFF system is presented in Fig. 20A. The ability of the

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Fig. 20. (A–F) Examples of FFF-based MMAM system. Lower case letters represent the steps of individual research work. (A) Representative FFF system with dual material, in-
situ fusion of fibers with molten thermoplastic in nozzle, and extrusion of pre-impregnated fibers [132]; (B) example of embedded copper wires in ULTEM 9085 and PC
substrates using an ultrasonic embedding tool for embedded electronics [197]; (C) continuous carbon fiber embedding in PC using ultrasonic energy [198]; (D) multi-material
electroforming parts in FFF system [97]; (E) short and continuous fiber-reinforcement in FFF system [201]; (F) Multi-material bridge span was printed with LDPE–Cu–Sn
35 vol% metal-filled composites. Simultaneously, the pillars were composed of printed polyester thermoplastic elastomer to demonstrate support-free printing and sensor
applications [202].

FFF system to fabricate continuous fiber, filament, and wires offers ical properties and increasing the anisotropy [203]. Another exam-
a tremendous opportunity for the fabrication of multifunctional ple of the part design limitation is the accessibility of the fabricated
parts, including embedded sensors [193-196], electrical circuits component. The embedded electronics fabrication with an FFF sys-
[197], reinforced composite parts [198], heating elements tem is a unique area of application that enables monolithic yet
[199,200], and functionally gradient structures [132]. multifunctional device manufacturing. However, research describ-
Regardless of the types of thermoplastics, several challenges are ing the method of assembly and disassembly for servicing has not
associated with the FFF multimaterial system. Similar to the poly- been established. Therefore, the reliability of the fabricated compo-
mer–polymer MMAM system, the FFF system poses limitations in nents should be adequately high to increase the end-user’s confi-
component design, process development, and materials. For dence in rapidly replacing the traditional components and
instance, the deposition of fiber material within the thermoplastic deploying them for multifunctional utilization. In the FFF MMAM
material is restricted to a certain volume. A higher volume percent- system, several processes are developed and maintained under
age of the fiber content reduces the matrix material within the the patent, e.g., wire coextrusion systems [201], wire embedding
component and increases the voids, thereby affecting the mechan- [204], fiber embedding [205], and fiber impregnation [206].
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A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Although each process improved the capability of MMAM, each 5.2. Powder bed fusion
process poses a limitation on the fiber placement, control, mainte-
nance of volume fraction, or the initial placement of the continuous The principle of the PBF process is to create a layer of metal
fiber/wire. Moreover, a mismatch of the CTE of the discrete mate- powder on a substrate with a powder feeding system, such as roll-
rial limits the process development of MMAM systems. Typically, ing, blade, or brush, and selectively melting or sintering the area
the thermal conductivity and CTE of the thermoplastic-based determined according to the computer-aided design (CAD) of the
matrix materials considerably reduce the continuous fiber, includ- desired component using a laser (L-PBF) or electron beam (E-
ing carbon fiber, glass fiber, and any conductive and resistance PBF) as a heat source [207]. This process is repeated for the subse-
wires. quent layer by descending the build stage, feeding the powder on

Fig. 21. Illustrations of metal AM processes [207,216] (a) Power bed fusion process, (b) binder jetting process, (c) direct energy deposition process.

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the previous layer, and melting or sintering the current layer along 5.4. Directed energy deposition
with the previous layer(s) (Fig. 21a) [188]. However, this technol-
ogy is commonly utilized for single-metal powder production with In the DED process, the material in the form of powder or wire is
one powder-bed dispensing unit [208]. Specifically, the single- fed through a nozzle that can perform multiaxial displacement
powder delivery system limits the fabrication of MM components, based on the component design, and the material is melted using
and accordingly, a mixture of metal–metal or metal–ceramic pow- the heat source (Fig. 21c) [221]. The ability of complex design
ders can be printed even with the single-powder delivery system and dimensional accuracy is compromised to increase the deposi-
to resolve this limitation. Thus, using blended materials, multi- tion rate using wire and arc additive manufacturing (WAAM)
material PBF (Fig. 19) has been achieved for various material com- [222]. Moreover, WAAM process is highly implemented for
binations [119,209]. multi-material component fabrications owing to its powder feed-
To realize the complete potential of the intended multi-material ing design making it easy for MMAM approach [223]. However,
system, several factors should be considered to achieve a strong there are challenges regarding final product performance fabri-
and long-lasting bond between dissimilar materials [210]. Primary cated by WAAM, which are excessive grain growth due to heat
concerns for the success of the fabrication involve the optimization accumulation, resulting a decrease in mechanical properties [224].
of the PBF process parameters that allow sufficient re-melting into Although high dimensional accuracy and low surface roughness
the previous layers and strengthening of the bond between the lay- is required for near-net shape AM products, powder-based DED
ers [211], which might be affected by the powder characteristics techniques, laser-engineering net shaping (LENS), and direct
[212]. During optimization of the process parameters to avoid laser/energy/metal deposition (DLD/DED/DMD), such as WAAM,
undesirable defects, the component is susceptible to exhibiting a are established as the best method for realizing these requirements
lack of fusion owing to the low-energy density of the heat source, by allowing multi-material delivery to the heat source to yield
wherein high-melting-point alloying elements are located or the multifunctional components [225]. The most critical challenge for
applied energy density of the porosity remains constant because DED and the other similar AM techniques is to form a strong bond
of the existing low-melting-point elements. Otherwise, the cracks between dissimilar materials. Although powder feeding is compa-
in between dissimilar materials are caused by differences in ther- rably more efficient than PBF processes, the mismatches in mate-
mal properties [213,214]. An approach to using smaller powder rial characteristics such as thermal expansion coefficients,
sizes for materials with high melting point has been proposed to thermal conductivity, laser absorption, and melting points are cer-
increase their surface area and the amount of energy absorption tain material-specific challenges that cause residual stress and
during the PBF process [212,215]. metallurgical defects during DED fabrications.
Thus, the fabrication of multi-material components by PBF sys-
tems requires comprehensive consideration for process parameter 5.5. Hybrid MMAM systems
optimization and powder characteristics. Furthermore, post-
process heat treatment might be required even after a successful A hybrid process merging both additive and subtractive manu-
fabrication to ensure the desired compositional homogeneity. Fur- facturing can maintain dimensional accuracy and surface finish as
thermore, PBF methods are required to provide an improved sys- well as improve the productivity through thick layers. Hybrid man-
tem for recycling and reusing the powder in the build stage, ufacturing can avoid the weaknesses of each process while exploit-
which is a limiting factor for PBF systems as an emergent technol- ing the strengths to achieve a system with capabilities beyond each
ogy for MMAM compared to DED systems. individual process [226]. The advantages of the hybrid process
have been extensively exploited in producing metal components,
with complex geometry being produced with AM and areas requir-
5.3. Jetting-based systems ing precise dimensions or surface finish being machined [226]. In
addition, hybrid systems have been used to produce polymer com-
Similar to PBF, binder jetting (BJ) requires a powder bed, but it ponents and components comprising multiple materials [227].
differs in terms of bonding methodology. Although the PBF solidi- More recently, the combination of metal AM with metal form-
fies the powder by thermal energy, the BJ bonds the powders with ing has been developed to improve the shape of the deposited
an adhesive to form the structure at low temperatures (Fig. 21b) material layers via local plastic deformation, while providing
[188]. This technique requires a compatible binder with the metal improved stiffness and wear resistance to the built components.
powder, such as polymer binders, metal inks, and metallic slat Currently, this process is evolving and has expanded rapidly by
compounds [217]. The application of bonding on a powder bed fol- encompassing new concepts from sheet and bulk metal forming
lows the same procedure as that in the PBF. Concurrently, the BJ processes. The initial developments of hybrid metal AM systems
process exhibits similar challenges as the PBF to manufacture aimed to utilize multiple thermal energy sources and apply a com-
MM components, such as multiple powder feeding and efficient bination of metal AM with metal cutting to improve the productiv-
powder recycling systems. BJ-processed components that require ity and quality of the built components. These developments
post-AM heat treatment for structural integrity do not experience resulted in the commercialization of the first hybrid metal AM sys-
residual stress and differ from the PBF process. However, post-AM tems in the mid-2010s [228,229]. The notable examples of com-
heat treatment causes structural shrinkage that can be detrimental mercialized hybrid-metal additive manufacturing
to the structural application, considering the variations in the ther- systems/companies include Optomec, Hybrid Manufacturing Tech-
mal properties of multiple materials [218]. nologies, Concurrent Technologies Corporation, etc.
Material jetting (MJ) or inkjet 3D printing system is appropriate Hybrid multi-material AM (HMMAM) technology has been used
for MMAM owing to its applicability for multiple jetting heads. to fabricate several MM components, including metal–metal as
Polyjet (PJ) [115,117] is an excellent example of MJ technology that well as metal–polymer material couples [226]. Weflen and Frank
has been widely used for multicolor AM, as noted in Table 4 and proposed a method for producing metal–polymer components
depicted in Fig. 19. However, the limited availability of materials using hybrid manufacturing systems. First, the performance of
[219] and measurement of material rheology [220] during printing the polymer extrusion AM tool is assessed, and the process param-
are the challenges of the MJ technology. eters are integrated into a machining center. To evaluate polymer

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extrusion thermal characteristics in the machining center, the rela- Fig. 22, functional materials (e.g., printed circuits) for electronic
tionship between component cooling and geometry is studied. devices have been developed. In another study, Ma [215] devel-
Thereafter, the strength of the component is baselined on various oped a novel technique named ‘‘hybrid deposition manufacturing”
cooling periods and material flow rates, which allow the compara- by combining the FDM and MJ AM processes to fabricate MM com-
tive analysis of the structural performances of the extruded poly- ponents for robotics and mechatronics-related applications. Their
mer and the metal–polymer interface [226]. method considerably reduced the manufacturing time, required
Recently, hybrid MMAM machines and setups in metal AM (ad- manual labor, amount of waste material, and complexity of assem-
ditive/subtractive) have been further developed [230]. Muguruza bly compared to alternative processes [232]. Combining the DED
et al. [231] developed a hybrid system to produce ceramic process with a multi-axis machining center enables the fabrication
particle-reinforced photosensitive resins; their system is com- of new products with MM geometries and surface finishes that
posed of digital light processing (DLP) technology and a 2D drop- cannot be achieved via additive processes alone. Consequently,
on-demand inkjet printing system. The DLP technology enables hybrid DED systems have successfully demonstrated the implanta-
the construction of 3D objects using the photopolymerization of tion of a Bluetooth active sensor within a high-strength steel com-
photosensitive resins, whereas the inkjet printing system deposits ponent [233] fabricated using pH 13–8 stainless steel and Invar 36
tiny drops of conductive inks. In a similar system, as observed in alloy multi-material deposition.

Fig. 22. (a) Developed DLP system (used for 3D printing) and inkjet system (for circuits) [231]. (b) m4 3D printer, a hybrid multi-material multi-method AM system for
fabricating intricate structures [43].

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Despite the benefits in terms of increased productivity, surface general, the post-processing processes of AM components include
quality, and dimensional precision [16], hybrid MMAM systems but are not limited to laser micromachining, chemical processing,
pose several challenges and limitations. For instance, as DED is a micromachining, manual finishing operations, electroplating,
fusion-based process, there are potential structural problems of machining, tumbling, electro-polishing [235]. Several post-
dissimilar metal welding, namely, the formation of undesirable processing techniques for complex geometries are presented in
intermetallic phases [23,133]. With the implementation of the Fig. 23, and several processes were used for application-specific
hybrid approach, certain technological challenges still remain components, e.g., Goh et al. [12] have discussed various post-
(e.g., process planning, decision planning, use of cutting fluids, processing treatments for 3D printed multi-material and multilay-
and need for post-processing). As novel hardware technologies ered electronics in a recently published review.
emerge, supporting software tools remain incompetent to fulfill Among the AM methods, certain technologies are highly cap-
the potential of hybrid systems. Considering the gap in the existing able of manufacturing various materials in combination in a con-
literature, more research effort is required to develop comprehen- tinuous and gradual process. For instance, DED and LENS AM
sive hybrid-AM software solutions [234]. Dilberoglu et al. [234] processes can realize MMs with continuous and/or discrete mate-
proposed a hybrid manufacturing simulator that enables users to rial gradient with and across the layers in comparison to PBF-based
interpret G-codes, which aids in visualizing the tool paths and technologies [241], which can fabricate only discrete material gra-
shapes of the manufactured objects. Therefore, addressing the dient. However, the high capability of the abovementioned pro-
aforementioned limitations would ultimately enhance the capabil- cesses for MMAM comes with enormous post-processing
ities of hybrid systems, especially for multimaterial fabrication. requirements to ensure dimensional accuracy and precise shape.
Commercially available post-processing technologies can man-
6. Post-processing for MMAM age components printed using homogeneous material, designed
with limited complexity, and realized using only a single material
Post-processing of MMAM components differs from those fabri- for the entire component. Therefore, to progress toward achieving
cated using a single material. In case of thermal post-processing, fully functional components for several applications, a novel sys-
temperature and other parameters should be adjusted considering tem must be developed for the post-processing of MMAM or func-
the thermal properties of both materials. Therefore, a new post- tionally graded AM components. In addition, the post-processing
processing method should be developed based on the compatibil- aspect of MM components must be considered at the design stage
ity with all materials in combination instead of accounting for only to minimize the requirement for this null-value-addition process
a single material. Post-processing confirms that the quality in [147]. Furthermore, effective post-processing, including considera-
terms of mechanical properties, surface properties, geometric tion during part design, post-heat treatment, and support material
accuracy, tolerance, and aesthetics, among other factors of AM removal, will enhance production efficiency as well as minimize
components, satisfies the standards and design specifications. In the overall cost of the component.

Fig. 23. Several processes used in post-processing of additive manufactured parts. (a) Milling machining process used for post-processing of complex AM components.
Support structures used as a clamping device [236]. (b) Single-pulsed laser polishing and hybrid laser polishing processes enhance surface characteristics [237]. (c) Hybrid
processes such as electrochemical polishing and cavitation peening [238]. (d) Design of magnetic polishing tool [239]. (e) Working principle of laser surface structuring and
laser micromachining using ultrashort laser pulses [240].

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7. Applications and opportunities nents can be fabricated using MMAM, such as pressure sensors,
smart sensor integration, and microelectromechanical systems.
New studies and technical breakthroughs concentrated on ris- Hainsworth et al. [249] introduced a malleable soft-robot actuator
ing multifunctionality in diverse applications caused by MM prod- with embedded sensors and integrated it into a robotic arm’s end-
ucts providing significant benefits to the worldwide industrial and effector grasping system to aid human-occupied processes, which
research communities. Compared to conventional structures, the was impossible if not performed by 3D printing technology
ability to fabricate specialized MM structures utilizing 3D printing because of the labor of assembly. Several MMAM techniques can
technology permitted particular material choices and improved utilize multiple materials to fabricate electronic devices or compo-
various attributes of target components [242,243]. nents, such as FDM that can fabricate embedded sensors, and
The development of MMAM has considerably aided several multi-material extrusion technology to create pressure sensors
high-tech engineering fields, especially the aerospace industry [250].
(Fig. 24). In addition, the significance of creating and using multi- The capability of electronic components fabricated via single-
material components has been recognized, because they aid in cre- layer deposition (traditional technique) poses several limitations
ating lightweight designs and enable tooling testing in space. The and renders it unsuitable for high-performance electronic applica-
material selection, e.g., metal powder, ceramics, polymer, and rein- tions. However, the multilayered capacitors and inductors can be
forced composites, and its performance is crucial for manufactur- fabricated (Fig. 25a), which eliminates the previous design restric-
ing MM components used in any aircraft or space mission [32]. tion and creates new possibilities for high-performance electron-
Moreover, technological breakthroughs related to MMAM have ics. Although the manufacturing of components with
resulted in great advances in medicine. Significant progress has multilayered MM eliminates several commonly required processes
been achieved in bio-inspired fabrications of tissue engineering in conventional manufacturing [251], multilayered circuit fabrica-
structures for delicate human-body parts, including the use of tion encounters several restrictions owing to the availability of
biodegradable polymers for cell encapsulation and drug delivery limited options in printing techniques. A particular study has suc-
systems [247]. Furthermore, 4D printing of various components cessfully demonstrated the use of AM methods for fabricating var-
and shape-memory polymers are imperative achievements of ious types of completely printed multilayered circuits [252]. A
MMAM in the medical field [248]. Thus, the significant applications stretchable multilayer strain and pressure sensor are displayed in
of MMAM in several industries have been elaborated in the follow- Fig. 25b. The active components include certain core elements for
ing subsections. logic circuits that are widely employed in sophisticated electronics,
e.g., transistors and diodes considered active components
7.1. MMAM of electronic components (Fig. 25c). These components often exhibit multilayered designs
and require various materials, including semiconductors, conduc-
MMAM has enabled the integration of electrically distinct tors, and dielectric materials [253]. The functional components of
materials, including conductors, semiconductors, and dielectrics, the OLED display comprised six layers that were 3D-printed with
which are essential components in the direct production of MMs, as portrayed in Fig. 25d. The capability of MMAM 3D printing
three-dimensional electronic devices. Several electronic compo- to incorporate various materials in the intricate design of LEDs is

Fig. 24. (a) Aerospace heat exchanger AM using stainless steel SS 316 and Inconel 718 (Image copyright: Netherlands Aerospace Centre). (b) MMAM wing section inspired by
fishbone to adjust wing curvature [244]. (c) MMAM aircraft engine disk fabricated using 316L stainless steel and Cu10Sn materials [245]. (d–f) Dual-metal components
fabricated using copper on Aerosint recoater metal 3D printer, photo by Aerosint [246].

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Fig. 25. 3D printed electronic components (a) 3D-printed passive electronic components [254] (b) Stretchable multilayer strain and pressure sensor [255] (c) 3D-printed
microfluidic capacitor, diode, and two transistors and a multiflow controller [256] (d) Exploded view of OLED display demonstrating its layer-by-layer structure. Layers 1–6
are 3D-printed components [257] (e) Design and operation principle of the 3D-printed energy harvester [258].

promising for producing innovative electronics, thus, being highly [261]. MMAM has reduced waste materials, which is essential for
researched to replace the conventional approach for electronic in-space manufacturing applications, because self-sustenance in
component fabrications. space is crucial. Earlier, only plastic components were capable of
Compared to other electronic parts and gadgets, 3D-printed being recycled and reused. However, researchers plan to construct
energy devices are comparatively new and form a developing a fully integrated fabrication system, which will be a completely
research field. Energy devices can be categorized into energy har- multi-material recycler that can process metals as well. As
vesting and energy storage devices. A schematic of the energy har- reported, MMAM can potentially provide diverse advantages
vester device using metal–plastic MMs is illustrated in Fig. 25e related to sustainability. Owing to the advancements in 4D print-
[258,259]. ing and smart MMAM, a wide range of industries will be impacted
by technology, specifically for continuous deep-space exploration
and self-sufficiency.
7.2. MMAM sustainability

In the realms of rapid manufacturing, personalized design, and 7.3. 4D printing and MMAM for soft robotics
structural applications, the realization of MMAM will be a water-
shed moment. To leverage the combined or hybridized qualities Soft robotics involves using soft, flexible materials for robotics
of several materials, multi-material 3D printing can be potentially applications instead of the stiff, hard joints used in conventional
used in structural engineering applications. In addition, it enables robots. Owing to greater degrees of freedom, they offer a variety
the rapid production of durable, high-quality structures with the of applications in the bio-robotics, medicine, industry, and aero-
qualities of all combined materials [231]. Compared to single- space industries. The primary objective of soft robotics is to
material AM, MM printing is more eco-sustainable and capable of develop robots that are flexible and resemble natural movement
creating new innovative 4D structures that can provide particular [262]. MMAM technology offers enormous potential in developing
shapes and characteristics. In addition, the components fabricated soft robotics and actuators in various fields. The widespread use of
using MMAM exhibit superior tensile strength, mechanical charac- AM technologies for the creation of soft robots is possible because
teristics, and durability [260]. of the recent advancements in the 3D printing of soft materials
Prospective space missions will be heavily dependent on man- such as thermoplastic silicone or polyurethane-based materials
ufacturing, as it will reduce the launch costs and offer on- [263], biologically inspired materials [264], shape-memory materi-
demand tools for extended operations without requiring replenish- als (SMMs) [265], stimulus–response materials, and stimuli-
ment from Earth. Recently, the International Space Station (ISS) responsive materials [266]. The major AM techniques for soft
used the FDM process with ABS material to print in microgravity, robotics fabrication include FFF, direct ink writing, DLP, and SLA
but the performance of ABS in microgravity is still unclarified. This processes.
is the initial stage in manufacturing advanced materials and more The actuation is the transformation of energy into mechanical
intricate metal structures in space. To ensure self-sustainability, work, which may be considered the backbone of a soft robot.
the primary objective of in-space manufacturing is to achieve Therefore, it influences several factors, including the motions exe-
meaningful space exploration that is less dependent on Earth cuted by soft robots and the required manufacturing process
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(Fig. 26a & b). Several actuation systems have been developed, materials, and printing techniques to resolve several printing
such as flexible fluidic actuation (FFA), cable-driven actuation, issues that negatively impact 3D-printed soft robots.
shape-memory materials (SMMs), electroactive polymer (EAP),
less-used actuation systems, and hybrid actuation. A Harvard 7.4. Multi-material bioprinting
research team created an AM-based pneumatic network (PneuNet)
actuator to increase the wall thickness and number of chambers of The term ‘‘bio-printing” refers to the use of the ‘‘material trans-
PneuNets based on an FFA actuation system, which revolutionized fer process” in producing biological materials such as cells, tissues,
the field of soft robotics [267]. A schematic of soft pneumatic actu- and organs employing cells, biological molecules, and chemicals, as
ators is presented in Fig. 26c & d. In addition to FFA soft robots, depicted in Fig. 28a. Owing to an upsurge in organ transplants but
Shintake et al. [268] developed an innovative soft actuator based limited availability of organs for transplant including the present
on a hybrid actuation system by utilizing a 3D printed PLA mold. limits of tissue engineering, the creation of a 3D or 4D bio-
Soft robots are growing in popularity owing to their versatility printing engineering branch is highly useful [275]. Single-
in diverse applications, especially for jobs requiring safety, dexter- material-based 3D bio-printing typically results in restricted diver-
ity, and conformal deformation. Soft robotics are vital for numer- sity in the physical and chemical characteristics of products. There-
ous applications, including the investigation of newly uncharted fore, a rapidly growing interest in the modification and
regions such as biomedical (robotic muscles, climbing robots, edi- diversification of generic printing materials by combining them
ble robots, wearable robots, and prosthetic robots; Fig. 27), aero- with other materials exhibiting special properties to create a 3D
space, electronics, biomimetic, food and agriculture, e-textiles, printable composite with excellent performance, such as ideal
manipulation of objects, and automation. Given the present rate mechanical properties, desired biocompatibility, improved
of advancement in the field of soft robotics, such robots may soon biomimicking of tissues structures, and appropriate fidelity pro-
be realized as MMAM for significantly enhancing this motes the application of MMAM in the bioprinting field [276].
development. The objective of MM bio-printing is to resolve the issues related
Despite all the advancements in materials science and system to single-material and imitate the intricate architecture of biolog-
design, significant gaps are still present in this area in terms of con- ical tissue and organs in scaffolds [277]. Multi-material 3D bio-
ventional production methods, which concerns the manufacturing printing integrates diverse qualities into a single project and deliv-
of several materials and the adhesion between the components for ers useful items with vital strength and performance [278]. Tech-
producing soft robots. In soft robotics, however, MMAM technolo- nological breakthroughs in MMAM technology have resulted in
gies are gradually assuming an increasingly essential role Owing to great advances in medicine. Significant progress has been achieved
their inherent qualities which are ideally suited to the needs of soft in bio-inspired fabrications of tissue engineering [279] structures
robot production, such as the scarcity of soft materials on the mar- for delicate human body parts and the use of biodegradable poly-
ket and commercial 3D printers suitable for soft materials. Thus, mers for cell encapsulation and drug delivery systems. This has
researchers should focus on enhancing the use of MMAM in soft enabled the construction of multiscale, fully functioning, heteroge-
robotics, enhancing the process parameters of unconventional neous, and multicellular hepatic structures that can deliver effi-

Fig. 26. Design of 3D-printed soft MM bending actuators; (a) bending actuator with a uniform cross-section over entire effective length of actuator; (b) bending actuator with
multiple segments of equal lengths [269]; innovative soft pneumatic actuators with (c) three and (d) four chambers can bend in any direction [270].

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Fig. 27. 3D-printed different applications of soft robotics: (a) wearable robotics for assistance and rehabilitation [271]; (b) synthetic muscle mimics natural muscle that is
three times stronger [272]; (c) natural-pose joint angles for human hand and 3D-printed prosthetic hand [273]. (d) Soft robotics hands respond to human grip [249]; (e) 3D-
printed biomimetic artificial muscles using soft actuators that contract and elongate [274]. (f) Octobot: a self-powered soft 3D-printed robot [260].

Fig. 28. (a) Diagrammatic representation of 3D bioprinting process [282]. (b) Vascularized tissues fabricated by simultaneously printing cell-laden bio-ink and sacrificial bio-
ink [283]. (c) Organ-on-a-chip development for disease modeling and therapy development for precision modeling [280].

cient and expedient performance. The schematic of vascularized ically appropriate vasculature, which made possible with multi-
tissues fabricated by simultaneously printing cell-laden bio-ink material approach. Furthermore, organ-on-a-chip is another tech-
and sacrificial bio-ink is illustrated in Fig. 28b. nique for creating biological tissues. For biological investigations,
In addition, the co-printing of hydrogel and sacrificial materials tissue/disease modeling and drug screening models have been
allows the utilization of MM bio-printing for fabricating physiolog- used to simulate human organs, as depicted in Fig. 28c [280].

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Moreover, MM bio-printing offers the potential to produce more 8. Limitations and challenges
accurate biomimetic tumor models, because it can replicate the
intricate 3D microenvironments of tumors. Based on its dynamics, MMAM does not indicate that the advantages of each material
bio-printed heterogeneous tumor models facilitate the process of can be necessarily employed for desirable applications. In certain
tumor growth [281]. cases, researchers have exploited the disadvantages of the joining
In the past few years, 3D bioprinting has achieved remarkable MMs, such as insufficient bi-material bonding and residual stress
development, spanning from straightforward proof-of-concept at the interface. Controlling the AM process is challenging owing
prints to intricate, tissue-like structures created from various to the miscibility and wetting constraints of various materials
materials. The techniques for 3D bioprinting promise immense and the dissimilarities in their properties (e.g., thermal conductiv-
potential for development. However, certain issues are still ities and expansions, melting points) [155]. Mismatches in coeffi-
required to be resolved in further investigations into bioprinting cients rely on the similar or dissimilar material selection, bi-
methods, cellular sources, biomaterial choices, etc. Compared to material systems such as metals–plastics, metals–ceramics plas-
real tissues/organs, the lack of accuracy is among the most signif- tics–ceramics can create huge mismatches, resulting in defects
icant disadvantages of existing bioprinting methods. Mostly, tis- such as cracks, pores, residual stresses that affect the integrity of
sue/organ architectures are extremely delicate for existing the components, dimensional stability, crack growth resistance,
bioprinting technologies. Additionally, slow printing speed for and mechanical properties in real-life applications [23]. Therefore,
complicated structures is problematic regarding the biofabrication future research should focus on the material selection, design, and
of several multi-materials in sequence [277]. manufacturing aspects of MMAM parts in particular the residual
and surface stresses generated during AM of metallic parts [289].
7.5. MMAM for architecture and construction Specifically, understanding the composition and optimal distribu-
tion of appropriate materials, mechanisms of reaction kinetics,
The obstacles encountered by construction industry results in bonding, residual stresses, and cracking mechanics are essential
excessive material and energy consumption and nearly stagnant for designing MMs. As such, nonuniform properties in the designed
productivity growth [284]. The current construction techniques MM components are complex; efforts in materials designs, charac-
pose several drawbacks, including high construction limitations teristics, chemical compositions, properties, and manufacturing
and the work required to align the components in accordance with constraints are necessary prior to MMAM processing [290].
them, as well as a high vulnerability to construction errors caused Furthermore, for the specific process, alloy formation at the
by inadequate communication between the design and execution. interface of bi-material in-situ is far from an equilibrium state
A significant portion of construction work is conducted in an inef- and difficult to characterize [155]. The defects at the grain bound-
fective and labor-intensive manner [285]. To address these issues, aries, e.g., microcracks, usually occur in the metal material PBF pro-
AM integrated with multiple materials can significantly alter the cess. In addition, other outstanding challenges such as low
current manufacturing and construction operations. MMAM can production throughput, poor scalability and surface finish, low
fabricate objects with varying material qualities without additional interfacial bonding, and high cross-contamination should be over-
assembly and multi-material architecture design. This modifica- come [291]. Apart from the basic understanding, technical break-
tion can manage inefficiencies in manufacturing and construction throughs such as the design-related concern of the development
by reducing the number of required production processes as well of CAD programs, design protocols, and procedures should be
as providing solutions to challenges connected with the connection developed [290].
of specific materials or elements [286]. AM of a complex MM component may require adjusting the
Although most AM procedures can use various materials, lim- materials thousands of times. Thus, MMAM processes are more
ited research has been conducted to apply these techniques to gradual in comparison to single-material AM processes. Further-
the architecture and construction field. Concrete material delivers more, varying materials does not mean that swapping the ink car-
acceptable qualities for construction at a moderate cost. Depending tridge/spool, which requires various printing process parameters
on the diverse characteristics of the mixture and the specific addi- that vary with the jetting nozzles in extrusion-based processes.
tives or fillers in concrete, as such, MMAM enables to produce this Thus, most of the AM processes designed for fabricating single-
mixture, therefore, mixed concrete offers a wide range of qualities material components face enormous challenges while employing
and uses compared to conventional applications. In context, them for manufacturing MM components. Furthermore, defining
numerous approaches can be employed to alter these qualities and distributing multi-materials in a single component requires
by adjusting the concrete mixture composition, thereby rendering extensive knowledge of 3D printable materials, their chemical
concrete as an ideal material for use in MMAM. The most prevalent compositions, optimal printing parameters, and manufacturing
strategy in MMAM of concrete is to alter the material density. The constraints [180,292]. Owing to several limitations such as a lim-
MIT Mediated Matter group studied aluminum powder as a foam- ited selection of 3D printable materials [293], scanty design guide-
ing agent for concrete, also known as variable density concrete. In lines exist on material compatibility and multi-material 3D
presence of aluminum powder and uncured concrete, the evolution printability, which is a major limitation in realizing MMAM com-
of hydrogen gas results in the foaming of the concrete mix that ponent fabrication for the end-user.
reduces the overall weight and consumption [287]. Additionally, As depicted in Fig. 29, most analyzed existing research applied
an extensive investigation of additive-based lightweight concrete empirical methodologies to investigate the properties of multi-
demonstrated that additives significantly influence the overall per- material AM components (Fig. 13). However, the majority of them
formance of concrete mixture [288]. Alternatively, MMAM can be did not conduct validation studies of experimental results using
utilized with concrete with the addition of fibers, which can FEM. As indicated in Fig. 29, approximately 140 studies fabricated
improve both the tensile strength and ductility of the material. MM samples, whereas only 23 studies included finite element
MMAM aims to alleviate more widespread problems that pla- analysis validation of their empirical results. In addition, a few
gue the construction industry; for instance, high consumption of researchers have used optimization algorithms to improve their
materials, limited adaptability of components to varying environ- multi-material designs or fabrication methodology. Overall, a neg-
mental conditions and structural requirements, and an overload ligible amount of literature has focused on software development
of complexity in the assembly and construction procedures cur- for MMAM. Therefore, MMAM software requires a significant
rently in use.
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A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

Fig. 29. Analyzed research literature of MMAM classified into six categories.

amount of research and development to utilize the full potential of challenges such as dimensional accuracies and post-processing
MM research. Another important aspect of the software for consid- requirements form the major challenges for consideration.
eration is the slicing of MM components and appropriate AM pro-  To date, no significant research has been conducted regarding
cess selection [294]. Although Hascoet [295] attempted to FFF-based MMAM, focusing on the relationship between printing
formulate the slicing of multi-material gradients, novel techniques conditions and dissimilar materials interface quality. The lack of
for preparation, analysis, and slicing of multi-material and/or func- information concerning multi-material extrusion-based 3D print-
tionally graded parts are still required. ing persists to be the area that remains unexplored, specifically
Certain research groups have focused on AM processes with the problems such as equipment, component design, and printing
MM manufacturing capabilities and new internal structures based materials.
on high performance computers and optimization tools. Metama-  According to this review, the majority of the analyzed litera-
terials and advanced lattice structures can be applied in flexible ture studied only the compressive and tensile properties of MM
materials and have potential in various disciplines, such as aero- components. Thus, other properties—chemical, fatigue, impact,
space, civil, textile, and tissue engineering applications. Using etc.—require further investigation. In addition, multi-objective
micro/nano multi-material AM with metamaterials and lattice investigations should be performed to explore the complex charac-
structures can result in innovative functional components. teristics of MMs.
 The standardized design of the experiment has not been
employed to investigate MM properties. Therefore, the results
and methodologies of existing literature cannot be feasibly com-
9. Summary and future recommendations pared for analysis. Most existing literature has focused only on
basic properties, and most characteristics such as fatigue, 3D print-
This article summarizes the progress of several aspects of MM ing properties, optical, impact/shock, flexural, and shear properties
research, including various types of MM compositions, component of MMAM components require considerable investigation.
design, modelling, and their analysis strategies. Furthermore,  The research on designing MM components is very limited,
applications, post-processing, technologies challenges, and poten- and the design rules for each AM process and material requires fur-
tial research gaps are significantly discussed and reviewed. A sum- ther study. In particular, in-depth studies should be conducted on
mary of findings, challenges, issues, and research gaps for future MM component design for each AM process.
research is stated as follows:  Only a few software packages are available with features for
 MMAM opens a range of new opportunities for the design, designing and optimizing MMs. Furthermore, the existing pack-
complexity, and functionality of highly personalized and high- ages do not offer full-range finite element analysis of MM. In par-
value products with improved properties. The integration of mate- ticular, no software package is specifically developed for the
rials at various scales can customize the thermal, electrical, design, optimization, and simulations of MM-related studies. Thus,
mechanical, optical, and multifunctional properties of the significant development is required in this research field. With the
components. development of new technologies (e.g., big data, machine learning,
 Majority of the researchers have focused on certain selected digital twin), new methods using these new techniques of MM
multi-materials of polymer and metal based. However, several design for AM can be explored in the future.
alternative materials, e.g., elastomers and hydrogels, have not been  Lastly, it is revealed that commercially available post-
studied significantly. For metal MMs, process- and material-related processing technologies still handle components printed using
29
A. Nazir, O. Gokcekaya, K. Md Masum Billah et al. Materials & Design 226 (2023) 111661

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