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A Holistic Review of Cement Composites Reinforced with Graphene Oxide

Article in Construction and Building Materials · March 2018

DOI: 10.1016/j.conbuildmat.2018.03.147

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A Holistic Review of Cement Composites Reinforced with Graphene Oxide

Yidong Xua, Juqing Zenga,b, Wei Chena, Ruoyu Jinc,*, Bo Lid,e,*, Zhihong Panb
a Ningbo Institute of Technology, Zhejiang University, Ningbo 315100, China;
b
School of Civil Engineering and Architecture, Jiangsu University of Science and Technology, Zhenjiang
212003, China;
c
School of Environment and Technology, University of Brighton, Cockcroft Building 616, Lewes Road,
Brighton, U.K., BN2 4GJ
d
Department of Civil Engineering, University of Nottingham Ningbo China, Ningbo, 315100, China.
e
Ningbo Nottingham New Materials Institute, University of Nottingham Ningbo China, Ningbo, China
*Corresponding authors: [email protected]; [email protected]

Abstract

Adopting a holistic review approach, this study started from the scientometric analysis

by analyzing the mainstream journals, keywords, scholars, publications, and institutions

active in the research of cement composites reinforced with graphene oxide (GO). Further

statistical summary of research themes and in-depth discussion addressed the current research

findings and gaps in terms of workability, mechanical properties, durability, and other issues

when adding GO into cementitious materials. Recommendations for future research were

provided, including but not limited to the necessity to study the long-term mechanical

properties of cement composites reinforced with GO, and the application of GO in concrete.

Keywords: Scientometric analysis; Science mapping; cement composites; Graphene oxide;

mechanical properties; durability

1. Introduction

The properties of cement pastes are believed to have the most important influence on the

cement-based composites (e.g., concrete) [1], As the cement hydration products, crystal

shapes and numbers, if controlled properly, could lead to great improvements in properties of

cement pastes [2]. Graphene oxide (GO) is a graphene derivative, consisting of several layers

of wrinkled two-dimensional carbon sheet with various oxygen-containing functional groups

1
such as hydroxyl, carboxyl, and epoxy groups on its surface or between the inter-sheet layers

[3] GO has been adopted by researchers [1,4-6] in controlling the formation of crystals in

the cement hydration process. To improve the mechanical properties of concrete, adding fiber

reinforced polymer (FRP) has been a widely adopted approach [7,8]. GO, as a promising

option of a nano-reinforcement in cement composites,[9,10] has been studied as a

complement to FRP [11]. For example, GO was added in cementitious adhesive to enhance

the bonding between NSM FRP and concrete substrate [7]. As a novel class of two-

dimensional nanoscale material [12], GO has attracted attention due to its high specific

surface area, dispersibility in water, high aspect ratio and superior mechanical performance

[13,15]. Another advantage of using GO is its lower cost by being synthesized in large

quantities from inexpensive nature graphite flakes [9]. GO has been studied in the form of

nanosheets,[9,12,16] which could be compounded by Hummer’s method.[16] GO nanosheets

provides a new method and direction towards the cement modification [16]. More research

[4,17-21] in GO-reinforced cementitious composites have been found in recent years.

Although it remains a relatively new research area in cement composites, the booming

trend can be expected. There has been so far limited investigation on the current research

status of applying GO in cementitious composites, specifically: 1) what have been the main

research themes (e.g., mechanical properties); 2) what are the current research gaps (e.g.,

understanding of the mechanism of how GO affects the cement hydration); 3) what should be

studied in the future for applying GO in cementitious composites. More research related to

GO-reinforced cement composites remain to be performed, such as properties of composites

containing recycled aggregates and GO as recommended by Long et al.[22]. There is a need

for a holistic review to shed light on the state-of-the-art research on GO-reinforced

cementitious composites. Adopting a comprehensive review approach consisting of a

scientometric analysis with science mapping technology followed by the in-depth discussion,

2
this study aims to achieve these following objectives: 1) to identify the influential publication

sources, frequently studied themes (i.e., keywords), productive scholars and institutions, as

well as literature with highest impacts in the field of GO-reinforced cement composites; 2) to

analyze the ongoing mainstream research focuses (e.g., microstructure); 3) to address the

current research gaps and to provide recommendations for the near-future research in cement

composites reinforced with GO. This review-based study provides the long-term direction of

how the emerging GO can be applied in material and structural engineering to meet the

modern construction needs.

2. Methodology

This review-based study incorporated a scientometric review [23-25] and follow-up in-

depth discussion of the ongoing research themes in GO-reinforced cementitious materials.

The rationale of adopting scientometric review is that multiple previous review-based studies

in the fields of construction engineering, management, and materials [26] may be relying on

subjective judgements which might be unreliable [27]. The scientometric analysis is able to

prevent this subjectivity and tends to be more unbiased [28]. In this study, the scientometric

review started from keyword search in Scopus, which was defined by AghaeiChadegani et al.

[29] as the database with a wider coverage of journals and more recent publications compared

to other search engines (e.g., Web of Science). Scopus has also been recommended by other

studies [30,31] as the search engine of literature. The keyword search in Scopus was set as

denoted below:

TITLE-ABS-KEY ("graphene oxide" AND (cement OR "cement paste" OR "cement

composites" OR "cementitious materials"))

The keywords input in the search included different types of construction materials with

cement in the mix design, such as mortar and concrete. The type of documents in the search

was set limited to journals, excluding conference proceedings. Conference papers have been

3
published in a larger number but with limited contribution to literature review considering the

extra amount of complexity added to analyze them [32]. After these key journal articles were

downloaded from Scopus, their abstracts were read by the research team members in this

study to ensure that all articles fall into the research of cement composites reinforced by GO.

Science mapping was involved in the scientometric analysis. It describes and evaluates

research policy purposes and process immense reservoirs of bibiometric data [33]. Science

mapping also displays the structural and dynamic aspects of a scientific research [34], and

represents spatially how disciplines, fields, and individual publications or authors related to

one another [35]. The text-mining tool, VOSViewer [36], was adopted to assist the science

mapping. Following the recommendations of Hosseini et al.[28]and Park and Nagy [37],

VOSViewer was utilized to to achieve these objectives: 1) to import the literature sample

downloaded from Scopus; 2) to identify the mainstream journal sources that publish research

outputs of GO-reinforced cementitious materials; 3) to analyze research words that have been

more widely studied; 4) to identify key researchers, articles, and institutions that contribute to

the academic community. Clusters and inter-relatedness among keywords, researchers,

articles, and institutions are also to be analyzed through science mapping. The information of

influential studies, scholars, and keywords provides the big picture on the latest movement of

academic research in a certain domain (e.g., GO-reinforced cement composites). It prevents

researchers in the global academic community or those who are interested in the academic

domain from being isolated.

Following the scientometric analysis, a further in-depth discussion was performed to

provide insights on the current research themes, gaps, and recommended future directions in

GO-reinforced cementitious materials. The discussion divided the existing research into a few

categories based on the scientometric analysis results. Existing findings and gaps within each

category were described leading to future work.

4
3. Scientometric analysis

Totally 113 relevant journal articles were selected following the literature search in

Scopus using the methods described in Section 2. Compared to other research themes in

cement composites, such as TITLE-ABS-KEY (“recycled aggregate” AND “cementitious

materials”) which resulted 611 relevant journal articles, the significantly smaller amount of

articles found in Scopus indicates that GO-reinforced cementitious composites remain a

relatively new research area. These articles are further analyzed according to the following

subsections in terms of the overall literature sample, publication source, research keywords,

productive and influential scholars, articles with highest impacts on the research community,

and institutions active in GO-reinforced cementitious composites.

3.1. Overall literature sample

The overall literature sample is illustrated in Fig.1 according to the yearly publication

from 2011 to 2018.

Note: the number of publication in 2018 is based on literature published up to 10 February 2018. Therefore,
publications in 2018 are not completely counted.
Fig.1. Summary of publication years of journal articles focusing on graphene oxide applied in
cement composite

The first relevant article was found in 2011, and few articles were found before 2014.

Most studies were published after 2015 and increased significantly since then. The current

number of publications in 2018 in incomplete (i.e., up to early February of 2018). But it can

5
be expected that more literature will be published in the follow-up years.

3.2. Analysis of publication sources

Sources of these 113 articles were analyzed using Vosviewer as the science mapping

visualization tool. Setting the minimum number of articles and minimum citations of a source

to be 2 and 5 respectively in Vosviewer, totally 13 journals met the thresholds as visualized in

Fig.2.

Note: The names of journals may not be completely displayed in VOSViewer. The full names of these journals
can be found in Table 1.
Fig.2. Science mapping of sources of publications in GO-reinforced cement composites

The size of nodes and fonts in Fig.2 indicate the impact of these journal sources. The

thickness of the connection lines shows the inter-relatedness between two journals. For

example, it can be found from Fig.2 that publications from Construction and Building

Materials and Cement and Concrete Composites have been highly mutually cited. The colors

of nodes in Fig.2 show the clusters of journals which indicate that journals within the same

cluster tend to be more inter-related based on their mutual citations. For example, Gongneng

Cailiao/Journal of Functional Materials, Xinxing Tan Cailiao/New Carbon Materials, and

Magazine of Concrete Research tended to form their own cluster with less connection to

other journals visualized in Fig.2. Generally, it can be seen that Construction and Building

Materials is the most influential journal in the research of GO-reinforced cement composites.

6
It has also strong and wide connections with most other journals in this field. The more

quantitative analysis of the influence of these journals is provided in Table 1.

Table 1.
Statistical analysis of journals in GO-reinforced cement composites

Journal source Total Number Citations Avg. Average

link of pub. citations
strength journal Year
articles
Carbon 13 4 51 2017 12.8
Cement and Concrete
Composites 37 4 93 2016 23.3
Cement and Concrete
Research 19 2 32 2016 16.0
Composite Structures 9 2 5 2017 2.5
Composites Part A: Applied
Science And Manufacturing 24 2 6 2017 3.0
Construction and Building
Materials 117 34 361 2016 10.6
Fuhe Cailiao Xuebao/Acta
Materiae Compositae Sinica 1 2 8 2015 4.0
Gongneng Cailiao/Journal Of
Functional Materials 7 7 18 2015 2.6
Journal of Materials in Civil
Engineering 11 4 46 2016 11.5
Journal of Physics And
Chemistry of Solids 19 3 29 2016 9.7
Magazine of Concrete
Research 6 2 15 2014 7.5
RSC Advances 37 5 61 2016 12.2
Xinxing Tan Cailiao/New
Carbon Materials 10 2 19 2016 9.5
Note: Avg. Pub. Year stands for the average year that the given item (e.g., Journal) publishes the research theme
of graphene oxide in cement composites. The same abbreviation applies to the follow-up tables in this paper.

The impacts of a given journal are measured by their total link strength to other peer

journals in Table 1, number of articles published, total citations received, and average citation

per article. The average publication year is also listed in Table 1 to show the recentness of

articles in the journal. Consistent to the visualization displayed in Fig.1, Construction and

Building Materials ranks in the top in terms of the total link strength, number of publications,

and total citations. It should be noticed that the average citation may vary from other

measurements. It can be told that journals with highest citation per article related to GO-

7
reinforced cement composites are: Cement and Concrete Composites, Cement and Concrete

Research, Carbon, RSC Advances, and Journal of Materials in Civil Engineering. It is

inferred that though with fewer articles published compared to Construction and Building

Materials, these journals have made significant contributions to the research community in

publishing research findings in GO-reinforced cement composites.

3.3. Keyword analysis

Keywords represent the core contents of existing studies and depict the research areas

within a certain domain [38]. From totally 232 keywords extracted through Scopus database,

the researchers set the minimum number of occurrences at 3 using Author Keyword. By

removing generic keywords including graphene, graphene oxide, cement, cement paste,

cement composites, cementitious materials, and further combining keywords with the same

semantic meanings (e.g., strength, mechanical properties, and mechanical strength), totally

13 keywords were identified. Fig.3 displays these major keywords and their inter-relatedness.

Note: NSM stands for near-surface mounted

Fig.3. Co-occurrence of keywords

It can be found in Fig.3 that mechanical properties and microstructure have been the two

main research focuses. The connection line shows that microstructure study is highly related

to the hydration of cement, including the early-age hydration [39,40]. The co-occurrences

between microstructure and hydration can be found in numerous studies [1,41-42]. In

comparison, durability has not been sufficiently studied. The existing studies [15,44,45] of

8
durability have more been based on GO in the form of nanosheets. Studies [46,47] of

mechanical properties were more closely co-occurring with dispersion and the form of GO in

carbon nanotubes. Dispersion problem of GO nanosheets in alkaline cement matrix is another

issue that restricts the further application of GO [49]. The cluster analysis also shows that

these keywords (i.e., concrete, fatigue, NSM or near-surface mounted, bond, and FRP) [50-

53]tended to form their own inter-related network with weaker connections to the remaining

keywords. The more quantitative measurements of keywords are provided in Table 2.

Table 2.
Statistical summaries of keywords studied in cement composites reinforced by GO
Total link Avg. Pub. Average
Keywords strength Occurrences Year* citations
Bond 3 3 2017 1.7
Carbon Nanotubes 3 3 2017 5.0
Concrete 8 8 2017 2.5
Dispersion 2 3 2017 6.7
Durability 3 3 2016 4.7
Electrical Resistivity 3 3 2017 5.0
Fatigue 3 3 2017 0.7
FRP 7 7 2017 1.4
Hydration 9 12 2015 13.3
Mechanical Properties 20 33 2016 7.1
Microstructure 22 28 2016 10.6
Nanosheets 6 9 2016 4.6
NSM 7 7 2017 1.4

Consistent to the visualization in Fig.3, mechanical properties and microstructure top

Table 2 by their total ink strength and occurrences. However, it is also noticed that cement

hydration is the keyword that have received the most attention in the research of composites

reinforced by GO, followed by microstructure, which is highly related to the study of

hydration. Hydration is also the research topic that has been published earlier, with the

average publication year in 2015, compared to other newly emerging keywords which are

mostly published around 2017 (e.g., concrete and dispersion).

3.4. Authorship analysis

9
 Awareness of existing scientific collaboration networks in a research field enhances the

access to specialties and expertise, improves productivities, and prevent scholars’ isolation

within the academic community [28]. Science mapping was applied to study the most

productive researchers and the collaboration among them. Among the totally 335 authors

identified in VOSViewer, the researchers further set the minimum number of publications and

the minimum number of citations of an author to be 3 and 30 respectively. A total of 21

authors met the thresholds. Among them, the most productive authors are visualized in Fig 4.

Fig.4. Productive scholars in the research of GO-reinforced cementitious composites

The collaboration network can be found from the clusters and connections lines shown in

Fig.4. These most productive scholars (e.g., Duan W.H., Mohammed A., and Lv S.) all have

established their research collaboration network. Strong collaborations among researchers can

10
be found through science mapping. For example, Lu Z. and Li Z have co-authored in multiple

publications [42,54-56]. Lv S. has been leading the research within the cluster in multiple

research outputs [4-6,15,41,44-45,57-59]. Quantitative measurements provided in Table 3

offer more insights on the impact of these scholars.

Table 3.
Quantitative analysis of scholars active in the research of GO-reinforced cementitious
composites
Total link Avg. pub. Average
Author strength Publications Citations Year citation
Duan W.H. 202 10 174 2016 17.4
Hou D. 65 3 54 2016 18.0
Korayem A.H. 83 3 123 2015 41.0
Kothiyal N.C. 50 4 35 2016 8.8
Li D. 64 3 107 2016 35.7
Li X. 163 9 96 2017 10.7
Li Z. 180 9 90 2016 10.0
Liu J. 155 8 168 2015 21.0
Liu Y. 125 6 138 2016 23.0
Lu C. 69 3 43 2015 14.3
Lu Z. 151 8 85 2016 10.6
Lv S. 145 8 155 2015 19.4
Ma Y. 98 5 142 2014 28.4
Mohammed A. 84 13 44 2017 3.4
Nazari A. 58 5 33 2016 6.6
Qiu C. 68 4 111 2014 27.8
Sanjayan J.G. 122 7 54 2017 7.7
Sharma S. 50 4 35 2016 8.8
Sun T. 92 5 131 2014 26.2
Wang J. 39 4 58 2016 14.5
Zhou Q. 115 6 155 2014 25.8

According to Table 3, most productive scholars measured by total link strength, number

of publications, and total citations include Duan W.H., Li Z., Liu J., Lu Z., Lv S., Sanjayan

J.G., and Zhou Q. The average citation per publication differs from other measurement items

in Table 3. Korayem A.H. and Li D., although with only three journal articles published, top

the average citation among all scholars, indicating the significance of their research in

reinforcing cement composites with GO. Other scholars with significant contribution to the

research community include Ma Y., Qiu C., Sun T., Zhou Q., and Liu Y., most of whom fall

11
into the cluster of Lv S shown in Fig.4. The average publication year indicates that scholars

that have been active and productive with more recent publications, including Li X.,

Mohammed A., and Sanjayan J.G.

3.5. Citation of articles

Journal articles that have received the highest citations were summarized. Setting the

minimum number of citations of a journal article at 20, totally 19 out of 113 articles were

extracted. Among them articles received highest citations are visualized in Fig.5.

Note: Only the first author of each selected article is displayed in VOSviewer.
Fig.5. Mapping of most influential articles in GO used in cement composites

The connection lines in Fig.5 identify the inter-relatedness of articles. The number of

citations of these most influential articles are listed in Table 4.

Table 4.
Articles that have received highest citations by February 2018

Article Title Citation

12
 Effect of graphene oxide on the rheological properties of cement
Shang et al. (2015) pastes [60] 22
Graphene oxide-deposited carbon fiber/cement composites for
Chen et al. (2015) electromagnetic interference shielding application [11] 36
Horszczaruk et al. Nanocomposite of cement/graphene oxide - Impact on hydration
(2015) kinetics and Young's modulus [61] 24
Mechanical properties and microstructure of a graphene oxide-
Pan et al. (2015) cement composite [62] 71
Mechanism of cement paste reinforced by graphene oxide/carbon
Lu et al. (2015) nanotubes composites with enhanced mechanical properties [47] 30
Enhanced properties of graphene/fly ash geopolymeric composite
Saafi et al. (2015) cement [17] 30
Influence of graphene oxide as dispersed phase in cement mortar
matrix in defining the crystal patterns of cement hydrates and its
Sharma and Kothiyal effect on mechanical, microstructural and crystallization properties
(2015) [63] 23
Effect of GO nanosheets on shapes of cement hydration crystals and
Lv et al. (2014) their formation process [1] 31
Effect of graphene oxide nanosheets of microstructure and
Lv et al. (2013) mechanical properties of cement composites [59] 89
Graphene oxide/ferrofluid/cement composites for electromagnetic
Singh et al. (2011) interference shielding application [64] 76

It can be found from Table 4 that articles with highest citations basically focus on the

research of cement hydration, mechanical properties, micro-structure and related mechanism

within GO-reinforced cement composites.

3.6. Research institutions

Institutions with high impacts on the research community of GO-reinforced cement

composites were summarized. Setting minimum number of publications and minimum

number of citations to be 2 and 10 respectively in VOSViewer, 10 out of 223 institutions were

extracted as shown in Fig.6.

13
Note: The names of institutions may not be completely displayed in VOSViewer. The full names of these
institutions can be found in Table 5.
Fig.6. Science mapping of institutions active in the research of GO-reinforced cement
composites

Three main clusters are identified in Fig.6. International collaboration among institutions

can be found in each of the three clusters, for example, the collaboration between Hong Kong

and mainland of China, between China and U.S., as well as among China, Australia, and U.S.

According to the node size and thickness of collection lines, Monash University Australia and

Shanxi University of Science and Technology China have been most productive in the

research of GO-reinforced cement composites. Quantitative measurements of the research

impacts of these institutions are provided in Table 5.

Table 5.
Measurements of research impacts of institutions in GO-reinforced cement composites
Total Number
link of Total Avg. pub. Average
Institution strength articles Citations year citation
Beijing University of Civil
Engineering and Architecture
China 6 2 19 2016 9.5
Hong Kong University of Science
and Technology 18 2 43 2016 21.5
Jiangsu Subote New Material Co.,
Ltd. China 19 4 22 2017 5.5
Michigan Technological
University United States 9 2 28 2016 14.0
Missouri University of Science
and Technology United States 14 3 24 2017 8.0

14
 Monash University Australia 40 7 129 2016 18.4
Shaanxi University of Science
And Technology China 28 7 170 2014 24.3
Southeast University China 19 4 22 2017 5.5
Taiyuan University of
Technology China 19 3 21 2017 7.0

Five out of the totally ten research-active institutions listed in Table 5 come from the

mainland of China, the rest institutions are from U.S., Australia, and Hong Kong respectively.

Consistent with the findings in Fig.6, Monash University Australia and Shanxi University of

Science and Technology China top Table 5 based on their total link strength, number of

publications, and total citations. Both universities are also among the institutions with highest

average citation. Shanxi University of Science and Technology China is also the institution

with longer history of established research profile in GO-reinforced cement composites.

Other institutions have been more recently involved in the same research area, such as

Missouri University of Science and Technology United States and Southeast University

China.

4. Discussion and findings

Compared to other more widely studied area in construction materials (e.g., recycled

aggregate concrete), the limited studies (i.e., 113 journal articles found in Scopus) of GO

applications in cementitious materials indicate that GO reinforced cement composites is a

relatively new research direction. The first journal article in GO reinforced cement

composites was published in 2011 and few studies were found before 2014. Since 2015, these

studies have been skyrocketing year by year, indicating the emerging research direction of

adopting GO to reinforce cementitious materials, due to its extraordinary properties [54].

However, barriers that restrict GO’s real-world application have not been well addressed,

such as agglomeration [48]. GO have been studied in multiple forms and sizes, such as

nanosheets [65], nanoplatelets [66], and aggregates [56]. Currently the research in cement

15
composites reinforced by GO is still at the early stage. The main themes and future research

directions can be summarized in terms of the cement composites’ workability, the formation

mechanism and performance control of hydration products’ microstructure, mechanical

properties of cement composites, durability, and volume stability.

4.1. GO types and preparation

GO exists in multiple forms, such as GO nanosheets [4] and GO nanotubes [67]. These

commonly studied GO types and the method of their preparation are summarized in Table 6.

Table 6.
Summary of literature on preparing various types of GO
Type of GO Method of preparation Reference
GO In-situ reduced GO Saafi [17]
The combination of modified silica fume and GO by
GO-encapsulated silica fume
electrostatic action to form suspension using magnetic Shang [60]
(GOSF)
stirring
Single-walled GO-carbon Adopting Hummers method, GO being composited with
Li [67]
nanotubes single-walled carbon nanotubes
GO-deposited carbon fiber (GO- Using electrophoretic deposition and GO being prepared
Chen [11]
CF) adopting the Hummers method
Polycarboxylate (PC) and GO
nanosheet composites（GON- The copolymerization caused by GO nanosheet and the
monomers of polycarboxylic acid-based water-reducer Lv [4]
PCS）
Synthesis of chemically functionalized GO through the
GO and Polyetheramine (GOM) Wang [68]
reaction of Polyetheramine and GO

4.2. Cement composites’ workability

The fast movement and increasing applications of high-rise and long-span structures

require a better concrete performance. Self-compacting concrete has been successfully

applied in practice. Nevertheless, multiple studies [55,62,69-71] indicated that GO would

reduce the fluidity of the cement slurry and increase its viscosity, further affecting concrete

workability. Wang et al.[69] found that cement slurry’s fluid loss would reach 70%, with its

viscosity increased by 1,850% when cementitious materials were added with 0.05% GO by

weight. GO is a two-dimensional carbon allotrope [12] and GO sheets tend to be hydrophilic

[72]. Therefore, GO increased cement pastes’ viscosity due to its two-dimensional planar

honeycomb lattice [73]microstructure, high specific surface area, and hydrophilic feature

16
[5,6,74]. Although there have been studies [68,75] attempting to improve the rheological

properties of cement-based composites, the problem of slump loss has not been completely

solved. Coarse aggregate in ready-mix concrete would further increase the internal friction

resistance, causing difficulties in construction. Further research is needed to explore the

feasibility of adopting the modern molecular cutting and grafting technology and applying

GO in multi-functional chemical admixture in improving concrete workability and reducing

slump loss. There is a large potential for applying GO-reinforced cementitious composites

(e.g., concrete). More research is needed in improving the workability of concrete containing

GO, for example, applying the self-assembly or morphological technologies [88] to

incorporate GO in chemical admixture to improve concrete workability.

4.3. Formation mechanism of cement hydration products

Hydration products determine the performance of cement-based composites. Research

[1,4-6]has shown that GO has a significant effect in the cement hydration products. Lv et al.

[5] observed that at the existence of GO, the hydration products tended to be well-ordered

crystalline or petal-like shapes as shown in Fig.7.

Fig.7. Cement hydration products in crystalline or petal-like shapes

The pores were more uniform and smaller as GO had the sheet layers with higher

strength and toughness, and hence enhancing the growth of cement hydration products. Jiang

17
and Wang [77] and Wang et al.[69] supported the finding of Lv et al.[5].However, the

research of Horszczaruk et al.[61] showed that the addition of GO did not cause significant

differences in the formation and shapes of hydration products. Cui et al.[78] further disagreed

with Lv et al.[5]that the crystalline or petal-shaped substances were not part of hydration

products, but just calcium carbonate due to the carbonation reaction when preparing the

sample of cement composites. The understanding of the formation mechanism and shapes of

hydration products were further explored by Lv et al.[44,57] focusing on controlling the

shapes of hydration products by doping GO nanosheets. The formation mechanism of cement

hydration products involving GO is illustrated in Fig.8.

Fig.8. The formation mechanism of hydration products in well-ordered crystalline or

petal-like shapes (adapted from Lv et al.[44]).

Future research can target on altering the microstructure of cement composites reinforced

by GO in order to achieve the desired performance of composite materials. Further research

can also be performed to simulate the hydration process using molecular dynamics method

18
adopted by Hou et al.[79] and Fan et al.[80], and to establish a microstructure model of

hydration products.

4.4. Mechanical properties

The mechanical properties of cement composites reinforced with GOs have been

relatively more widely studied compared to other themes (e.g., durability). Unlike the

formation mechanism of hydration products which have raised more arguments in the

research community, existing studies [5,6,46,69,81-83]have generally agreed that GO

improves the mechanical properties of cementitious composites. However, there are

inconsistencies of the increase rate by adding GO. An analysis of these studies [11,41,60,62]

revealed a wide range of strength increase rate of GO-reinforced composites, from 15% to

160% in compressive strength increase, and 18% to 185% in split tensile strength increase.

This wide range of strength increase rate could be partly explained by the mixture percentage

differences of GO in cement composites (i.e., from 0.02% to 4 %) as well as the preparation

of GO samples [84], such as GO sheets or single wall carbon nanotubes [67], graphene oxide

encapsulated silica fume [60], and GO-deposited carbon fiber [10] [11]. Besides the dosage of

GO additives, other factors such as surface chemistry, size, charge, and defects of graphene

structures [85] could also affect the resulted mechanical performance of cement composites.

The longer-term mechanical properties of cement composites reinforced with GO has not

been sufficiently studied. The researchers are also concerned on the reduction of the long-

term strength of cement composites due to the delayed formation of calcium alum under high

temperature. The effects of high temperature in properties of concrete containing GO has

raised research attention [86]. Few studies can be found so far addressing the issue of whether

GO could prevent this long-term strength loss. The other concern is whether GO could

enhance the resistance to material fatigue in cement composites, as material fatigue is a

widely concerned issue.

19
 4.5. Durability

Compared to the mechanical properties, durability of GO-reinforced cement composites

have not been sufficiently studied. The durability issue of cementitious materials covers a

wide scope, including reinforcement corrosion caused by chloride or carbonation, freeze-

thaw cycle, and alkali aggregate reaction, etc. GO can be directly correlated with the

corrosion resistance of gephene-reinforced concrete [87]. Mohammed et al.[14] found that

GO could reduce the penetration depth of chloride ions. The reduced penetration depth could

be explained by the inter-connected GO layers which form the sponge-shaped structure to

capture chloride ions [14]. Tong et al.[87] found that the anti-freezing performance of GO-

reinforced mortar was worse than the standard mortar, possibly due to the absorption and

desorption of nano-level pores within mortar. Lv et al.[44] revealed that GO-reinforced

composites could reduce the permeability depth by 72%, improve the dynamic modulus of

elasticity by 78% after 100 freeze-thaw cycles, and decrease the 28-day’s carbonation depth

by 66%. The improved durability by adding GO nanosheets into cement composites was due

to the orderly formed crystal-like hydration products which reduced the cracking and

hazardous pores in the microstructure [44]. Despite of these few studies, there have been so

far limited investigation in these common durability issues for GO-reinforced cement

composites. Specifically, limited studies have focused on analyzing the mechanism and

establishing the theoretical models within durability issues. More studies can be performed to

address the GO performance in an alite or alkailine paste as it has been found by Ghazizadeh

et al.[88] that GO would be reduced with its functional groups at a high PH.

4.6. Other research themes

The volume stability of cementitious composites affects the cracking sensitivity of

concrete structure in terms of autogenous shrinkage, plastic shrinkage, drying shrinkage, and

temperature deformation and creep. The mechanisms of these deformations, although

20
varying, are related to the microstructural change within cement composites, change of

hydration products’ density, and viscous flow. Adding GO into cement composites would

significantly affect the pore structure and hydration of cement composites, leading to the

further effects on volume stability. Nevertheless, there have been few studies investigating

the volume stability of GO-reinforced cement composites. It should also be noticed that most

existing studies focused on applying GO into cement slurry or mortar, but with limited

studies of GO applications in concrete. As concrete is the most widely used construction

materials [89], more studies on GO applied in concrete should be conducted in the future.

Future research directions in GO-reinforced concrete should be extended from the

perspective of material properties to structural application, and ultimately leading to the

application of GO-reinforced concrete in construction practice.

5. Conclusions

Aiming to investigate the current status of research in graphene oxide-reinforced

cementitious composites and provide the corresponding research directions, this review-based

study adopted a holistic approach incorporating both scientometric analysis and in-depth

review of existing literature. The research in graphene oxide-reinforced cementitious

composites is a relatively new yet emerging area in modern cementitious materials. The first

publication in this area was found in 2011, and only 113 journal articles were found up to

February 2018. The research in graphene oxide-reinforced cement composites has gained

increasing popularity especially since 2015. It is expected that more near-future studies will

be published in this area. The scientometric analysis revealed that:

 Construction and Building Materials was the most influential journal in publishing

studies related to graphene oxide-reinforced cement composites based on its total link

strength, number of articles published, and citations;

 mechanical properties and microstructure were the most frequently studied keywords.

21
 Microstructure has been found with high inter-relatedness with cement hydration. In

comparison, other areas have not been sufficiently researched, including durability,

cement hydration, dispersion of GO, and material fatigue;

 most influential and productive scholars in the area of graphene oxide-reinforced cement

composites were identified, including Duan W.H., Lv S., Mohammed A., Li X., Li Z.,

Liu, J., and Lu, Z. The research network led by Lv S. had significant contribution to the

academic field, with multiple researchers receiving high citation rates per publication;

 journal articles receiving the highest citations and institutions active in the research of

graphene oxide-reinforced cement composites were also identified to provide a macro

picture of the scholarly community worldwide.

Further in-depth review of literature indicated that the formation of differently-shaped

cement hydration products has not been well understood. There have been arguments among

researchers regarding how graphene oxide would affect the cement hydration products.

Multiple other themes remain to be explored, such as the microscopic mechanical properties

of hydration products from cement composites reinforced with graphene oxide. More

research has focused on the mechanical properties of graphene oxide-reinforced cement

composites, but the durability issue remain under-studied. Recommendations for near-future

research are provided below:

 effective method in improving the workability of cementitious materials when reinforced

with graphene oxide;

 further studies of the formation mechanism of cement hydration products, and how to

adapt the microstructure of graphene oxide-reinforced cement composites to achieve

desired properties of composites;

 studies on the long-term mechanical properties of graphene oxide-reinforced cement

composites;

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 durability evaluation of graphene oxide-reinforced cement composites based on different

graphene oxide types (e.g., nanosheets, nanotubes, and graphene oxide with fiber, etc.);

 volume stability issue within graphene oxide-reinforced cement composites;

 experimental studies and applications of graphene oxide in concrete from both the

material and structural perspectives.

Acknowledgement

The authors wish to acknowledge the financial support of National Natural Science
Foundation of China (Grant No. 51778577), National Science and Technology Support
Program of China (Grant No. 2015BAL02B03) and Ningbo the Benefit of People Program
from the Ningbo Science and Technology Bureau (Contract No. 2015C50049).

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