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Understanding Low Energy Nuclear Reactions

Conference Paper · March 2009

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Antonella De Ninno
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Understanding Low
Energy Nuclear
Reactions
Antonella De Ninno
ENEA Frascati, Rome (Italy)
The Pd/H(D) system
The Pd/H(D) system is the first, historically, that attracted
research activities (Graham, 1866) because it represents one
of the most transparent and instructive models for a metal-
hydrogen system.
Electrolytic loading is one of the well known method to store
hydrogen or deuterium inside a lattice.
High pressures have been also used in order to increase the
density in a solid and improve the interaction between
particles, because of the decrease of the distance.
Palladium hydride
When hydrogen dissolved into metals, it occupies the
interstitial positions and expands the lattice.
This process generates a corresponding stress field, so that
diffusion equation became:

cV
J = − D(∇c − ∇σ )
RT
It has been shown that a strain field can stop the diffusion.
In the α+β region, the lattice parameter mismatch at the border
between the two phases generates a very strong localised
stress field which is unfavorable for diffusion.

However, co-existance can be avoided by selecting an

appropriate path on the p-c-T diagram.

(A. De Ninno et al., J. of Alloys and Compounds 253-254 (1997) 181)

Influence of the Pd microstructure

It can be observed the presence of a maximum loading ratio

depending on the metal microstructure.
Thermo-mechanical working and in particular cold-working
followed by thermal treatment can be used to have different
grain size in Pd samples.
There is an “optimum” grain size due to the competition between
the mechanical energy loaded in the lattice (Gorskji effect) and
the accumulation of h(d) ions at the border of the grains.
The loading ratios obtained at different machining shows a
maximum at almost the same grain size (50-60 microns)

(De Ninno et al. ICCF7 Vancouver, 1998)

 0.95

0.9
loading ratio D/Pd
0.85

0.8

0.75

0.7

0.65

0.6
20 50 55 100 150
grain size (mm)
 A conceptual discontinuity
In a paper of 1994 (Il Nuovo Cimento, vol. 107 A, n.1, pp. 143-
156), M. Fleischmann, S. Pons and G. Preparata wrote:
“The hydrogen in the palladium lattice is present as protons and
the second surprising feature is that the extremely dense
proton plasma is present in an electron concentration of 600-
1000M……we are driven to the conclusion that a satisfactory
explanation of the stable existence of the dense plasma
must be based on an appropriate many-body model”

Other surprising features are the very high diffusion coefficients

( of the order 10-7 cm2s-1 for hydrogen in the α phase) and
the fact that the diffusion coefficient are in the order
DD+>DH+>DT+ different from which can be expected on the
basis of a simple classical model of diffusion.
Another important observation is the measurement of very high
equilibrium H/D separation factor for hydrogen and
deuteruim dissolution into palladium cathodes at high
negative overpotentials.
The interpretation of this fact requires the assumption that the
species behave as classical oscillators in the lattice, i.e. they
are virtually unbound.

(B. Dandapani, M. Fleischmann, J. of Electroanal. Chem. 39 (1972) 323)

Born-Haber cycle
The rational chemical design of high-efficiency Hydrogen
Storage Metals has to take into account the vast difference in
properties between H+I and H-I.

z H-I → H0 + e- (ΔH° = + 0.75 eV)

z H+I + e- → H0 (ΔH° = - 13.60 eV)
z 2H0 → H2 (ΔH° = - 4.52 eV)
z H-I + H+I → H2 (ΔH° = - 17.37 eV)
The heat of formation of the metal hydride, ΔHf , can be determined
from calorimetric experiments or derived from PcT-measurements.
However, if these experiments are unavailable we may derive it by
constructing a Born-Haber thermodynamic cycle
Me(s) n/2H2(g) MeHn(s)
+
Sublimation Dissociation
enthalpy enthalpy of H2
Me(g) nH (g)
Total crystal lattice energy

Ionization Electronic affinity

potential of H atom
Men+(g) nH -(g)
+

Born-Haber cycle for the formation of solid binary metal hydride from
solid metal and gaseous hydrogen
An hydrogen atom (or molecule) must find very strong electric
fields in order to maintain itself in the ionized state (or to
dissociate into two ions).
The electric field inside the lattice must be able to produce a
very high energy (13.6 eV over distances in the order of the
Bohr radius 0.57 Å).
Clearly this requires a very peculiar electron distribution !
The (1,1,0) plan of the Pd lattice

Pd site
octahedral site

tetrahedral site

η
ξ
Possible plasma oscillations of
d-electrons shells

d-electrons shell

disk of “static” charge

The profile of the electrostatic potential in
the η-direction
eV eV

a0= 0.7Å
η

the plasma of d-electrons generates a screened

elecrostatic potential at tetrahedral sites
The problem of delocalization of
protons/deuterons
We have to face the problem of the delocalization inside the
lattice of deep electrostatic holes:

z High diffusion coefficient

z Inverse isotopic effect
z High chemical potentials

Many-body interactions must come into play and supply the

energy required to raise the nuclei to highly excited states
As delocalization depends on the occupancy by the
protons of highly excited states of the well, this
configuration must be very energetically
advantageous.
It becomes clear that collective phenomena must
come into play in order to supply the energy
required.
Pd hydride (or deuteride) is a so
peculiar system and it looks like a
“solid plasma”
How to increase the loading
In case deuterons are in a collective state, an externally
applied potential V(r) changes the energy of the state
by the quantity Z*eV, and, accordingly, the chemical
potential
G G
μ [V (r )] = μ (0) + Z *eV (r )

Where Z* is the screening factor.

De Ninno et al. ICCF8, Lerici (Italy) 2000

 0.15 β phase
0.10
γ phase
• From the very beginning we
0.05 have an exothermic
z To increase the
Chemical potential μ

0.00 • When the concentration

(spontaneous) absorbtion of
Δμ
Inovercome
case we the want to increase
-0.05 external potential
hydrogen
further the
value of 0.6
(deuterium).
•H(D)/Pd,
A fairly itconcentration,
extra energy we
became
small
(eV)

-0.10
-0.15 Δμ To decrease the
zcan choose
needs to increase
advantageous between twotothe
slightly
to switch
Δx strategies
concentration
another phase.to about 0.65
μest -0.20
Δx
Δμ internal potential
-0.25 Δx

-0.30
-0.35

0 0.2 0.4 0.6 0.8 1.0

x = [D]/[Pd]
“Preparata Effect”

equilibrium
equilibrium
 Equilibrium
(h2 = h1)
Equilibrium
h1 (h2 > h1) h2
 Vl Longitudinal voltage
(NOT an electrotransport)

anode Pd specimen (film or wire)

V ac Transverse voltage
x
 Pre-loading Super-critical phase
Beginning

[D] = 0.7 [Pd]

Loading
of cycle

[D] = [Pd]
[D] = 0

A. De Ninno, E. Del Giudice, A. Frattolillo, G. Preparata, A. Rizzo, Experimental

Evidence of 4He Production in a Cold Fusion experiment, ENEA
RT/2002/41/FUS
 50
40
V cathode
30

(Volt)
20
10
0
0 5000 10000 15000 20000 25000
2.2
2.0
1.8
1.6
R/R0

1.4
1.2
1.0

0 5000 10000 15000 20000 25000

50
40
30
Cell Current
(mA)

20
10
0
0 5000 10000 15000 20000 25000

(De Ninno et al. ICCF9 Beijing, 2002)

Cell current Icell, voltage across the cathode, Vcathode ,and normalized
resistance R/R0 vs time. The Icell and the related Vcathode increase induce a
sudden drop in R/R0 corresponding to an increase of loading from x=0.7 to x >
1 within a few seconds.
 de-loading
1.6 loading (Icell OFF)
(Icell ON)
1.5

1.4
R/R0

1.3

1.2
III load-deload cycle
1.1

1.0
60 0 10000 20000 30000 40000
50
DeltaP (mWatt)

40
30
20
10
0
-10
-20
0 10000 20000 30000 40000

A. De Ninno et al. ICCF9 Beijing, 2002

Why we can measure 4He in high
loading experiments

As well as the incoherent fusion mechanism “in vacuo” that

involve deuterons pairs, we focus our attention tothe
existence of coherent mechanisms in condensed matter
Collective mechanism can explain the experimentally observed
transition

d + d → Pstate → 4He + energy

dd fusion in vacuum

3H + 1H1
1
2H + 2H1 4He n +
1 2 +
n
+ + n +
n n + n
+ n n
+
3He + 1n0
2

0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0

Time (×10-21 s)
dd fusion in condensed matter
z In condensed matter the boiling
He nucleus can release its
energy to the e.m. field

z If such a process is quick

enough, it is not forced to break
n +
into fragments + n

z We can thus observe 4He atoms

and heat

0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0

Tempo (×10-21 s)
The production of 4He unaccompanied by γ-rays demands a
very fast (t <10-21 sec) energy transfer to the lattice electrons.
Suppose that a fusion be a physical event localized at a
definite site in the lattice. In order to reach the nearest atom
at a distance of about 1 Å the velocity v of the energy transfer
should be about 300 c !
According to universal accepted principles of physics it is
impossible to transfer the energy of a fusion dd -> 4He
(without γ rays) to the lattice.
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LENR cannot be localized events