i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1

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Heat and gas transport properties in pelletized

hydrideegraphite-composites for hydrogen storage
applications

Carsten Pohlmann a, Lars Röntzsch b,*, Thomas Weißgärber b, Bernd Kieback a,b
a
Institute for Materials Science, Dresden University of Technology, Helmholtzstr. 7, 01069 Dresden, Germany
b
Fraunhofer Institute for Manufacturing Technology and Advanced Materials IFAM, Winterbergstr. 28, 01277 Dresden, Germany

article info abstract

Article history: Metal hydrides are suitable for the compact, efficient and safe storage of hydrogen.
Received 6 September 2012 Considering hydride-based hydrogen storage tanks, the enhancement of the heat and gas
Received in revised form transport properties of the hydride bed is crucial for increased (un-)loading dynamics of the
26 September 2012 tank.
Accepted 27 September 2012 In this contribution, pelletized composites of different hydrogen storage materials
Available online 9 November 2012 (lithium amide, sodium alanate, magnesium hydride and transition metal hydride
Hydralloy C5) with expanded natural graphite (ENG) are discussed. The materials were
Keywords: admixed with up to 25 wt.% ENG and compacted at compaction pressures up to 600 MPa.
Hydrogenation behavior The resulting hydride-ENG pellets exhibit an increased effective thermal conductivity
Sodium alanate which can be tuned in a wide range. The pellets have an increased volumetric H2 storage
Lithium amide capacity compared to loose hydride powders. High gas permeability in radial direction and
Magnesium hydride sufficient thermal conductivity (>10 W m
1 K
1) in combination with a stable pellet
Hydralloy structure indicate a high potential to use suchlike prepared hydride-ENG composites for
Thermal conductivity hydrogen storage applications with high loading dynamics.
Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights
reserved.

1. Introduction capacities of hydrogen in metal hydrides, those solid-state

A change of paradigm in the energy sector is currently taking
place in many industrial countries. Because renewable energy
sources gain increasing importance, they need to be accom-
panied by environmentally friendly energy storage and energy
distribution technologies [1,2]. In this respect, hydrogen is
a clean, safe and carbon-free energy carrier for portable, mobile
as well as stationary applications [3e7]. A key challenge for
establishing a hydrogen-based energy cycle is yet its efficient,
compact and safe storage [8]. Due to high hydrogen storage
storage materials have attracted increasing attention within
recent years [9,10]. Extensive research has been carried out on
various hydrogen storage materials in order to meet the targets
given by the US Department of Energy1 regarding hydrogen
storage density, safety, efficiency, and materials costs.
From the viewpoint of hydride-based hydrogen storage
tanks, an important aspect is the improvement of the heat
transfer characteristics inside the hydride bed, thereby,
advancing the (un-)loading dynamics of the storage tank. In
that respect, only a few studies were conducted, which can be

* Corresponding author. Tel.: þ49 351 2537 411; fax: þ49 351 2537 399.
E-mail address: Lars.Roentzsch@ifam-dd.fraunhofer.de (L. Röntzsch).
1
http://www1.eere.energy.gov/hydrogenandfuelcells/storage/current_technology.html.
0360-3199/$ e see front matter Copyright ª 2012, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijhydene.2012.09.159
1686 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1
divided into two groups: Firstly, the enhancement of the
thermal conductivity through auxiliary metal structures
[11e15], and secondly, the preparation of hydrideegraphite
composites with increased effective thermal conductivity
[15e20]. The latter method allows to tailor the thermal
conductivity very accurately and to create even anisotropic
heat conduction properties which are favorable for tubular
storage modules. Furthermore, increased volumetric storage
capacities are achieved via compaction.
The goal of this study is the development of two-component
composite materials consisting of hydrides (majority phase)
and graphite (minority phase) in order to obtain an effective
heat conductivity much larger than that of pure hydride
powder beds. A reasonable target is to achieve an effective heat
conductivity of the hydrideegraphite composite of at least
10 W m
1 K
1 using less than 25 wt.% graphite.
Furthermore, it is important to guarantee sufficient gas
permeability, mechanical stability and stable storage capacity of
the pellet throughout cyclic hydrogenationedehydrogenation.
In order to cover a broad range of possible applications and
temperature regimes, a lightweight metal hydride (Mg90Ni10
alloy with hydrogen sorption temperatures around 300  C), two
complex hydride systems (sodium alanate, lithium amide with
hydrogen sorption temperatures around 140  Ce250  C) as well
as one transition metal hydride (MneTieV alloy also known as
Hydralloy C5 with hydrogen sorption temperatures around
20  Ce60  C) are examined and compared.
2. Experimental
The lightweight as well as the transition metal hydride mate-
rials are prepared in their metallic state. Since melt-spinning
proved to produce suitable nanocrystalline magnesium-
based materials for hydrogen storage [21,22], a melt-spun
Mg90Ni10 is used as starting material. For this purpose,
Mg90Ni10 master alloy ingots (99.9% purity) were produced and
melt-spun under argon atmosphere. Afterward, the resulting
ribbons were repeatedly chopped (Retsch SM 2000) into flakes.
The transition metal hydride granules (Hydralloy C5: 51 wt.%
Mn, 28 wt.% Ti, 14 wt.% V, 3 wt.% Fe, 3 wt.% Zr) were pre-
treated via high-energy rotating disk milling producing a fine
powder. In contrast to that, the complex hydrides are prepared
in their hydrogenated state via high-energy ball milling [23].
The first system based on NaAlH4 has improved intrinsic
sorption kinetics due to an addition of 4 mol% CeCl3. The
second system is a 2:1 molar mixture of LiNH2 and MgH2. It is
assumed to be the optimal composition in terms of hydrogen
storage capacity and limited ammonia generation [24].
All mixtures were admixed with ENG (delivered by SGL
Carbon). The ENG is of high purity (highest amounts of
impurities: Fe < 150 ppm and Si < 100 ppm) and not pre-
treated in any way in the as-delivered state. Furthermore, we
examined a radial thermal conductivity of about
370 W m
1 K
1 of neat ENG-pellets in our previous work [20].
Thereafter, they are uniaxial compacted into cylindrical
pellets. Table 1 gives the used compaction pressures and the
ENG contents for the various systems. Compactions pressures
are chosen based on the results of previous experiments
concerning mechanical stability. In the case of the transition
Table 1 e ENG contents and compaction pressures for the
various systems.
Material system ENG contents Compaction
[wt.%] pressures [MPa]
Mg90Ni10 5, 10, 25 150, 300, 600
NaAlH4 5, 10, 25 200, 300, 400
LiNH2eMgH2 5, 10, 25 200, 300, 400
Hydralloy C5 2.5, 5, 12.5 75, 150, 300, 600
metal hydride the weight fractions of ENG were decreased by
50% due to a higher mass density of the base material.2
The geometric density of the pellets is determined in order
to calculate the residual porosity. Thermal conductivity is
distinguished in axial and radial directions by cutting the
pellets into two slices with 2 mm in thickness using an
Accutom 5. These slices were examined using the flash
method (Netzsch LFA 447 NanoFlash) determining tempera-
ture diffusivity. From that, the respective thermal conduc-
tivity can be deduced. Furthermore, cross-sections of each
specimen are prepared for metallographic examination.
Thermogravimetry (TG) under hydrogen gas using
a magnetic suspension balance (Rubotherm) was performed in
order to investigate the stability of the pellets during cyclic (de-)
hydrogenation. Gas permeability in radial direction was deter-
mined only for the magnesium-based pellets using a specially
designed measuring cell (cf. Fig. 1). This was achieved by
pushing a constant mass flow of nitrogen through the pellet
from the center radially outwards. Thereby, an increase of gas
pressure in the central hole of the pellet can be measured which
relates to the gas permeability of the pellet in radial direction.
According to the integration of the Forchheimer equation in
radial direction, the mass flow Q and the difference between the
squared gas feeding pressure p21 and the squared outside pres-
sure p22 fits a parabolic polynomial (cf. Equation (1)) [16]:
     
R$T h r2 1 1 1 1
p21
p22 ¼ $ $ln $ $Q þ b$
$Q 2 (1)
M h$p r1 k 2$p $h r1 r2
2 2
where p1 is the feeding pressure, p2 is the outside pressure, R is
the universal gas constant, T is the absolute temperature, M is
the molar mass of nitrogen, h is the viscosity of nitrogen, h, r1
and r2 are the dimensions of the pellet, Q is the nitrogen mass
flow, k is the gas permeability and b [m
1] is a parameter
weighing the influence of turbulences in the gas flow. Fig. 1
provides an example of suchlike fitted curves including
a schematic drawing of a pellet with indicated measuring
variables. From the coefficients of the parabola (linear part)
the gas permeability can be deduced straightforwardly.
3. Results and discussion
3.1. Mg90Ni10-ENG pellets
In our previous works [20,25] the as-compacted state of pellets
prepared from melt-spun Mg90Ni10 and ENG was examined. It
2
Since ENG volume fraction strongly influences the overall
thermal conductivity, it was anticipated to keep it similar to the
other systems.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1
p2 = 1 bar
r known from the literature where powdery magnesium hydride
p1
Q flakes are mainly orientated in this plane. Gas flow resistance
1.38×10 Q + 4.64×10 Q
Fig. 1 e Example of a quadratic fit to determine the gas
permeability including a schematic drawing of a pellet
where measured pressures ( p1 and p2) and the mass flow
(Q) are depicted.
was found that the heat transfer characteristics and porosities
can be tailored in a wide range adjusting compaction pressure
and ENG content. First (de-)hydrogenation experiments were
conducted as reported previously [25]. From those results,
a series of cyclic hydrogenations with pellets containing no
ENG with a residual porosity of 40 vol.% were designed. In
principle, three states are of high interest: the pellet in its as-
compacted state, after cyclic hydrogenation in its hydroge-
nated and in its dehydrogenated state. From those three states
the thermal conductivity, gas permeability and phase align-
ment (microstructure) was determined. Fig. 2 shows the
pellets, micrographs of their cross-sections and the according
thermal conductivities, gas permeabilities, porosities and
metallic fractions of all three states.
The as-compacted state shows all properties as expected
from the previous experiments (cf. [20,25]). The pellet exhibits
a as-compacted b hydrogenated c dehydrogenated
6 W·m ·K 11 W·m ·K
k 4.95×10-1 m 2.13×10-1 m
8 cycles
62 vol.% 6 vol.%
38 vol.% 22 vol.%
100 µm 100 µm 100 µm
Fig. 2 e Properties of the Mg90Ni10-pellets without ENG in
their (a) as-compacted, (b) hydrogenated and (c)
dehydrogenated state after cycling.
1687
a relatively high gas permeability of 4.95  10
13 m2 which is
almost two orders of magnitude higher compared to values
was used. There, Chaise et al. [16] calculated values around
1  10
15 m2. This is caused by the strong dimensional aniso-
tropy of the used magnesium alloy flakes (form factor). Gas flow
easily penetrates the pellet in the radial direction since the
would be much higher in axial direction which, however, is not
of importance considering tubular tank architecture.
The hydrogenated pellet (after 8 cycles of (de-)hydrogena-
tion) showed a maximum uptake of hydrogen of about 5 wt.%
which is below its theoretical maximum (about 5.6 wt.%). A
residual metallic fraction is visible in the micrograph (cf.
Fig. 2(b)). Some flakes show internal metallic residues. The
total amount of metallic fraction was determined to about
6 vol.%. Further examination has to clarify this phenomenon.
It may be possible to improve the activation process of the
pellet. Another approach is to reduce thickness of the melt-
spun ribbons in order to decrease the diffusion path of
hydrogen. The gas permeability of the hydrogenated pellet
decreased (2.13  10
14 m2) due to decreasing porosity but still
remains at a high level. The thermal conductivity increased to
11 W m
1 K
1 which is evident considering the following: At
first, porosity is reduced which eventually leads to increased
heat conduction. Secondly, during the activation process of
the pellet the initially amorphous flakes crystallize which also
changes their intrinsic thermal conductivity. It increases from
about 15 W m
1 K
1 to 120 W m
1 K
1 [20]. The residual
metallic fraction strongly contributes to the higher thermal
conductivity in the hydrogenated state.
The dehydrogenated pellet recovered a porosity of 40 vol.%
which proves a good reversibility of the process with dimen-
sionally stable pellets. Due to the volume contraction during
dehydrogenation, void spaces form at the particles surfaces
which results in increased porosity. However, porosity is not
distributed as it was in the as-compacted state. Now a macro-
porosity between particles and a micro-porosity (roughened
ribbon surfaces) has formed. This results in higher resistance
to the gas flow through the pellet. Therefore, gas permeability
cannot be restored to its value in the as-compacted state. It
further decreased to 1.35  10
14 m2. Yet, a higher level
compared to MgH2-powder is maintained [16]. Thermal
conductivity slightly increased to 28 W m
1 K
1. Again, this is
caused by the effect of higher intrinsic thermal conductivity in
the metallic state.
In conclusion, it was shown that pellets based on a melt-
spun Mg90Ni10 alloy exhibit dimensional stability and suffi-
28 W·m ·K cient gas permeability throughout cyclic hydro-
1.35×10-1 m genationedehydrogenation. Yet, thermal conductivity
59 vol.%
41 vol.%
strongly varies. Once a complete hydrogenation can be
ensured, the effective thermal conductivity decreases drasti-
cally. However, pellets with ENG may assure high thermal
conductivities in the hydrogenated state.
3.2. Complex hydride-ENG pellets
After retrieving the volume fractions of all phases present
(hydride, ENG and porosity), it is possible to calculate volu-
metric as well as gravimetric storage densities of the pellets.
1688 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1

volumetric hydrogen content

[g l ]
-1

gravimetric hydrogen content

[wt.%]

Fig. 3 e Calculated hydrogen storage capacities of the

complex hydride-ENG pellets.

To determine the maximum gravimetric and volumetric

hydrogen storage density the theoretical storage densities of
the according hydride are multiplied by its mass and volume
fraction in the pellet, respectively. For NaAlH4, a maximum
gravimetric H2 storage density of 5.6 wt.% is assumed [26].
Doping NaAlH4 with 4 mol% CeCl3 reduces the maximum
gravimetric H2 storage density to 4.7 wt.%. The LiNH2eMgH2
mixture (2:1) has a maximum gravimetric H2 storage density
of 5.6 wt.% [27]. The maximum volumetric storage densities
are determined by multiplying the gravimetric densities with
the mass density of the according hydride. This results in 74 g-
H l
1 and 81 g-H l
1 for the NaAlH4e and the LiNH2eMgH2-
based systems, respectively. The thereby calculated hydrogen
storage densities are plotted in Fig. 3. These values represent
the maximum hydrogen content of each pellet which is the Fig. 5 e Micrographs of (a) the NaAlH4e and (b) the
upper limit of the amount of hydrogen that can be used LiNH2eMgH2-based pellets with 5 wt.% ENG each (arrows
practically. The available amount is reduced due to incom- indicate direction of compaction).
plete decomposition, e.g. at higher hydrogen backpressure. In
order to compare the storage densities of such pellets with
about 26 and 22 vol.% was found which results in a volumetric
commonly used loose hydride powders, the apparent density
storage density of 19 g-H l
1 and 18 g-H l
1 for the NaAlH4e
of the loose powders was determined according to DIN ISO
and LiNH2eMgH2-based powders, respectively. These values
3923/1. As a result, a hydride powder volume fraction of only
illustrate the enormous advantage of compaction regarding
volumetric hydrogen storage density.

Fig. 4 e Thermal conductivities of the NaAlH4e (black) and Fig. 6 e Porosity vs. compaction pressure of the Hydralloy-
the LiNH2eMgH2-based (gray) pellets. ENG pellets.
 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1
Table 2 e Thermal conductivities of the Hydralloy-ENG pellets.
Compaction 75 MPa 150 MPa
pressure
ENG content lrad ENG content lrad ENG content lrad ENG content
[wt.%] [W m
1 K
1] [vol.%] [W m
1 K
1] [vol.%] [W m
1 K
1] [vol.%]
2.5 3.7 4.4 2.4 4.7
5 14.4 9.0 15.9 9.7
12.5 60.0 20.2 62.8 22.2
The radial thermal conductivities of the complex hydride
pellets are shown in Fig. 4. As expected from the magnesium-
based system, a remarkable degree of anisotropy between
heat conduction perpendicular (radial) and parallel (axial) to the
direction of compression was examined. In both systems, the
radial thermal conductivity increases with increasing ENG
content. The radial thermal conductivities gather in a corridor
from 2 W m
1 K
1 to 40 W m
1 K
1. Due to the strong anisotropic
effect introduced by the ENG3 the axial thermal conductivity
remains at a low level of about 1 W m
1 K
1. From that the
ENG content is considered to be a suitable control parameter to
tune the thermal conductivity in a wide range. In that respect,
Hassel et al. [15] recently reported that ENG is more effective in
increasing the thermal conductivity compared to aluminum
powder. Our results, however, indicate a stronger increase in
thermal conductivity at comparable ENG-contents which
further illustrates the high potential outlined by Hassel et al.
The thermal conductivity in radial direction exceeds the
stated target in the hydrogenated state. Since dehydrogenation
should lead to higher intrinsic thermal conductivity of
the hydrogen storage material in the pellet (transition to the
metallic state), sufficient heat transfer throughout cyclic
dehydrogenationerehydrogenation can be assumed.
Optical micrographs of the NaAlH4e and the LiNH2eMgH2-
based pellets with 5 wt.% ENG compacted at 200 MPa are given
in Fig. 5. Both hydride phases appear grayish, ENG is black and
the very bright areas are metallic residues (aluminum or
magnesium, respectively). Porosity may be present between
hydride particles, at ENG-hydride phase boundaries as well as
within ENG. Generally, ENG shows a strong anisotropic
alignment, where graphite veins are mostly radially orien-
tated. This explains the strong influence on the radial thermal
conductivity (cf. Fig. 4). With increased ENG content the
degree of percolation of the ENG network increases and the
mean distance between single ENG veins decreases which
causes the almost linear gain in radial thermal conductivity.
3.3. Hydralloy-ENG pellets
In order to produce pellets which have a similar range of
porosity as the magnesium-based system4 another
3
The ENG is mainly radially aligned and, furthermore, also
shows high intrinsic anisotropic heat conduction behavior (high
thermal conductivity along graphene planes).
4
Both systems start from their dehydrogenated (metallic) state,
so that porosity inside the pellet is needed to compensate
swelling during hydrogenation. Thus, a comparable range of
porosities is reasonable.
1689
300 MPa 600 MPa
lrad ENG content
[W m
1 K
1] [vol.%]
7.4 5.0 9.0 5.3
23.6 10.2 22.9 10.5
56.5 23.4 58.5 24.4
compaction pressure of 75 MPa has been applied. Fig. 6 depicts
the achieved porosities for all ENG contents and compaction
pressures. As expected from our previous works [20,25] the
ENG increases compressibility (lubricant effect of ENG) which
results in lower porosities at equal compaction pressures.
Table 2 states the radial thermal conductivities of all
Hydralloy pellets. The axial thermal conductivities remain
constant at low levels. Again, a strong degree of anisotropy
between heat conduction perpendicular (radial) and parallel
(axial) to the direction of compression was found. Compared
to the complex hydride systems similar values can be ob-
tained at equal ENG volume fractions (cf. Fig. 4). Again, this
indicates the importance of the ENG contribution to the
effective thermal conductivity. From that, it is reasonable to
assume that if the ENG shows a high anisotropic alignment, it
becomes a control parameter to tune the thermal conductivity
of a powder-based low heat conducting material admixed
with ENG and compacted into pellets. On the contrary,
the melt-spun magnesium-based pellets exhibit a much
stronger dependence of their effective thermal conductivity
on porosity [20,25].
A first hydrogenation experiment was carried out with
a Hydralloy pellet containing 5 wt.% ENG compacted at
150 MPa. Initially an activation process followed by 15 cycles
at 50  C and 7 cycles at 20  C was investigated. From Fig. 7 it
is evident that even after the activation process of the
Hydralloy pellet a further improvement in sorption kinetics
as well as in hydrogen capacity takes place. However, after
the second cycle no significant changes occur. A hydro
hydrogen content [wt.%]
number
of cycles
cycle
cycle
cycle
Fig. 7 e Hydrogen de- and absorption behavior of
a Hydralloy-ENG pellet with 12.5 wt.% ENG compacted at
75 MPa.
1690 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 3 8 ( 2 0 1 3 ) 1 6 8 5 e1 6 9 1
genation rate of about 0.08 wt.% per minute is achieved with
a maximum hydrogen upload of 1.42 wt.%. The pellet
expanded in axial direction by about 10% which is attributed
to a non-optimal volume fraction of porosity in the as-
compacted state. At this point it becomes evident that
more residual porosity in the as-compacted state is needed
to compensate the material swelling during hydrogenation.
In this regard, a cycled pellet with optimized porosity needs
to be examined concerning its change in porosity, thermal
conductivity and also gas permeability due to the hydroge-
nation procedure. Future investigations will focus on that
issue; yet, our findings presented here have already indicated
the high potential of pelletized Hydralloy-ENG mixtures to be
used in tubular tank modules.
4. Conclusions
Mg90Ni10-ENG pellets have been investigated concerning their
changes in properties throughout cyclic (de-)hydrogenation. It
was found that the pellets maintain their mechanical
stability and sufficient gas permeability (varies between
1.35  10
14 m2 and 2.13  10
14 m2). However, both the
hydrogenated and the dehydrogenated state exhibit a clear
difference in radial thermal conductivity.
A characterization of the as-compacted state of the
complex hydride-ENG systems concerning thermal conduc-
tivity, phase alignment and distribution was presented. Both
exhibit a similar range of thermal conductivity of about
2 W m
1 K
1 to 40 W m
1 K
1 with only insignificant depen-
dence on compaction pressure. High anisotropic alignment of
the ENG phase in the pellet is essentially responsible for these
characteristics.
Hydralloy C5 was mixed with ENG (up to 12.5 wt.%) and
compacted (up to 600 MPa) into cylindrical pellets. Compared
to the complex hydride systems, similar values were reached
at equal ENG volume fractions. First experiments on the (de-)
hydrogenation behavior have shown an increase in sorption
kinetic and storage capacity during the first cycles after
activation.
From that it is reasonable to use the described processing
route to fabricate a variety of solid-state hydrogen storage
materials. All three material systems have proven wide
tunable ranges of radial thermal conductivity and high
mechanical stability. First cyclic (de-)hydrogenation experi-
ments indicate high potential to use suchlike prepared
hydrogen storage materials for tubular tank architectures.
Acknowledgment
This work has been performed in the framework of the
European Centre for Emerging Materials and Processes Dres-
den (ECEMP) which is funded by the European Union and the
Free State of Saxony. The authors would like to acknowledge
financial support from the Fraunhofer Attract program, the
GCSFP-Project (contract no. 03BV108B) and the International
Research Initiative (IRI) of E.ON. The preparation and delivery
of the ball-milled complex hydride powders by J.J. Hu and M.
Fichtner is gratefully acknowledged. Furthermore, the authors
would like to thank J. Meinert for helpful discussions and Th.
Hutsch for experimental support.
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