international journal of hydrogen energy 34 (2009) 5476–5487

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Automotive hydrogen storage system using cryo-adsorption

on activated carbon

R.K. Ahluwalia*, J.K. Peng

Argonne National Laboratory, 9700 S Cass Avenue, Argonne, IL 60439, USA

article info abstract

Article history: An integrated model of a sorbent-based cryogenic compressed hydrogen system is used to
Received 28 March 2009 assess the prospect of meeting the near-term targets of 36 kg-H2/m3 volumetric and
Received in revised form 4.5 wt% gravimetric capacity for hydrogen-fueled vehicles. The model includes the ther-
27 April 2009 modynamics of H2 sorption, heat transfer during adsorption and desorption, sorption
Accepted 4 May 2009 dynamics, energetics of cryogenic tank cooling, and containment of H2 in geodesically
Available online 3 June 2009 wound carbon fiber tanks. The results from the model show that recoverable hydrogen,
rather than excess or absolute adsorption, is a determining measure of whether a sorbent
Keywords: is a good candidate material for on-board storage of H2. A temperature swing is needed to
Hydrogen storage recover >80% of the sorption capacity of the superactivated carbon sorbent at 100 K and
Cryo-adsorption 100 bar as the tank is depressurized to 3–8 bar. The storage pressure at which the system
Activated carbon needs to operate in order to approach the system capacity targets has been determined and
compared with the breakeven pressure above which the storage tank is more compact if H2
is stored only as a cryo-compressed gas. The amount of liquid N2 needed to cool the
hydrogen dispensed to the vehicle to 100 K and to remove the heat of adsorption during
refueling has been estimated. The electrical energy needed to produce the requisite liquid
N2 by air liquefaction is compared with the electrical energy needed to liquefy the same
amount of H2 at a central plant. The alternate option of adiabatically refueling the sorbent
tank with liquid H2 has been evaluated to determine the relationship between the storage
temperature and the sustainable temperature swing. Finally, simulations have been run to
estimate the increase in specific surface area and bulk density of medium needed to satisfy
the system capacity targets with H2 storage at 100 bar.
ª 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights
reserved.

1. Introduction refueling hydrogen at reasonable pressures and tempera-

Hydrogen-fueled fuel cell and internal combustion engine
vehicles are being developed as clean, efficient, advanced
technologies for automotive transportation of the future.
For the storage of adequate amount of hydrogen on-board
such vehicles, activated carbon (AC) and other sorption
media are being explored as one option of storing and
tures. In general, however, the storage capacities of such
materials, including the recently developed metal organic
frameworks [1,2], are less than 2 wt% at room tempera-
tures. It is well known that physisorption can be signifi-
cantly enhanced by operating at cryogenic temperatures
[3,4]. Superactivated carbon AX-21 has shown excess
adsorption of 5.4-wt% H2 at liquid nitrogen temperatures

* Corresponding author.
E-mail address: walia@anl.gov (R.K. Ahluwalia).
0360-3199/$ – see front matter ª 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.
doi:10.1016/j.ijhydene.2009.05.023
 international journal of hydrogen energy 34 (2009) 5476–5487 5477

Nomenclature1 DP pressure swing

r density
C specific heat
k Boltzmann constant Subscripts/Superscripts
m_ mass flow rate a absolute adsorption
P pressure c skeletal
T temperature ex excess
u internal energy H2 hydrogen
Dh heat of adsorption m medium
DT temperature swing r refueling
h enthalpy b bulk
m mass d discharge
N adsorption g gas
Q_ heat transfer rate in inlet
t time out outlet
V volume s structure

(77 K). MOF-177, Zn4O(1,3,5-benzenetribenzoate)2, has
shown an even higher uptake at 77 K: 7.5-wt% of excess H2
and 11.2-wt% of absolute H2 at 70 bar [1]. The purpose of
this paper is to assess the potential of meeting the early
gravimetric and volumetric capacity targets [5] for on-board
H2 storage systems with cryo-adsorption at moderate
pressures (up to 350 bar but preferably <100 bar). The
longer-term targets have not been considered specifically
since they are reportedly being revised in view of the data
from the field demonstration program and the early results
from projects on development of hydrogen storage mate-
rials [6].
Whereas physisorption offers advantages of on-board
reversibility and rapid sorption kinetics, operating at cryo-
genic temperatures poses certain challenges. Maintaining the
storage vessel at low temperatures requires use of vacuum
superinsulation and tank design features to minimize
conduction paths to the ambient. Application of vacuum
insulation is a time consuming and labor intensive process
that has not been automated for high-volume manufacturing.
Insulating the storage tank may significantly add to the
volume of the system, thereby, degrading the volumetric
hydrogen storage capacity of the system. Although these
physisorption materials have relatively low heats of adsorp-
tion (Dha), removing even small amount of heat during refu-
eling is difficult at cryogenic temperatures. This heat transfer
problem is exacerbated by the generally low thermal
conductivity of physisorption materials (especially as powder
and pellets), which, in turn, requires use of a heat-conducting
support or extended heat transfer surfaces that add to the
system weight and volume. Also, as discussed below,
a temperature swing may be needed to assist in desorbing H2
and this further increases the cryogenic cooling duty.
Our approach to assessing cryo-adsorption for hydrogen
storage was to evaluate the volumetric and gravimetric
capacity of an on-board H2 storage system that meets the
functional requirements of the vehicle and its power plant
(see Table 1). To be viable, the storage system must be capable
of being refueled at a minimum rate of 0.5 kg of H2/min (initial
1
Local variables used in Section 2 are identified within the text
for clairty.
2007 target) and be able to supply H2 at 0.02 g/s/kW minimum
full-flow rate (i.e., 1.6 g/s for an 80-kW fuel cell system) at
a minimum delivery pressure of 3–8 bar. We used AX-21 as the
model sorbent since its physical properties and adsorption
isotherms are well characterized. We considered the option of
cooling the storage tank with off-board liquid N2 during
refueling because liquid N2 can be readily available or
produced on-site. We also evaluated the alternative option of
adiabatically refueling the tank with liquefied H2. Finally, we
used the model sorbent as a benchmark to assess the
improvements in H2 uptake needed to satisfy the near-term
capacity targets for storage systems.
2. Storage system model
Benard and Chahine [7] have shown that the Ono-Kondo
lattice theory can be adapted to model the adsorption
isotherms for hydrogen uptake on superactivated carbon
substrates. We recast their equations for the experimentally
observable excess adsorption (Nex) in terms of the absolute
adsorption (Na) and the amount of gaseous hydrogen that can
be contained in the accessible pores of the crystal structure.
Nex ¼ Na  va rg
ðx1 þ x2 þ x3 Þ
Na ¼ Nmax
3
va ¼ Nmax =rmax (1)
where rmax is the maximum density corresponding to
a completely filled adsorption layer and Nmax is a prefactor
that is a measure of the maximum uptake. In the Ono-Kondo
theory, xi represents the molecular fraction per adsorption site
(xi¼ri/rmax, i ¼ 1, 2 or 3) on the ith layer that can be determined
from the following set of nonlinear equations.
x1 ¼ x3
  
x1 1  xg E  EA
ln þ z1 x1 þ z2 x2  z0 xg þ ¼0
xg ð1  x1 Þ kT kT
5478 international journal of hydrogen energy 34 (2009) 5476–5487

Table 1 – Selected DOE (FreedomCAR) hydrogen storage system targets [5].

Storage Parameter Units 2007 2010 2015

Specific energy kWh/kg (kg-H2/kg) 1.5 (0.045) 2 (0.06) 3 (0.09)

Energy density kWh/L (kg-H2/L) 1.2 (0.036) 1.5 (0.045) 2.7 (0.081)
Refueling rate kg-H2/min 0.5 1.5 2
Minimum full-flow rate (g/s)/kW 0.02 0.02 0.02
Minimum H2 delivery pressure atm 8 4 3
Loss of usable H2 (g/h)/kg-H2 1 0.1 0.1

 ! excess H2 adsorption for the range of pressures and temper-

x2 1  xg z0 E  z2 E
atures over which the data are available. The results are
ln þ x2  xg þ ðx3  2x2 þ x1 Þ ¼ 0 (2)
xg ð1  x2 Þ kT kT
consistent with the expectation that, at a given temperature,
where xg ¼ rg/rmax, z0, z1 and z2 are the coordination numbers Nex reaches a maximum value with increasing pressure,
(z1 ¼ 6, z2 ¼ 1, and z0 ¼ z1 þ 2z2), and E and EA are the interac- whereas Na approaches an asymptotic value as the pressure is
tion energy parameters. Benard and Chahine [7] have deter- increased. Also, the lower the temperature, the lower is the
mined the energy parameters E (0.4 kJ/mol) and EA (4 kJ/mol), pressure at which the maximum Nex occurs.
rmax (130 kg/m3), and Nmax (g-H2/kg-AC) by fitting the Ono-
Kondo equations to the adsorption data for superactivated 2.1. Dynamic model
carbon AX-21 with a specific area of 2800 m2/g and a bulk
density of 300 kg/m3. In developing the thermodynamic model for the storage
medium we assumed that the kinetic and potential energy of
Nmax ¼ 130:62  0:404T þ 1:295  104 T2 þ 1:313  106 T3 (3) H2 flowing in and out of the tank can be neglected, that the
pressure and temperature in the tank are uniform, and that
Although pressure does not appear explicitly in Eqs. (1)–(3),
the sorption kinetics are sufficiently rapid so that the H2 in the
it implicitly affects H2 adsorption through the parameter xg
bulk gas phase is in phase equilibrium with the H2 adsorbed
that is defined in terms of the gas density (rg). Fig. 1 shows that
on the activated carbon. Taking the contents of the storage
the Ono-Kondo theory is in agreement with the measured
tank inside the vacuum insulation as a control volume (i.e.,
carbon fiber, liner, sorbent, stored H2, heat-conducting
support and the components of the heat exchanger), the
60
following are the differential forms of the mass and energy
Excess Adsorption (g/kg)

50 balances for the open system.

77 K
dmH2
40 _ in
¼m _ out
H2  mH2 (4)
dt
30
d 
_ in
ms us þ mH2 uH2 ¼ m _ out _
H2 hin  mH2 hg þ Q in (5)
20 dt

10
where mH2 is the total mass and mH2 uH2 is the total internal
297 K energy of stored H2.
0
0 50 100 150 200 mH2 ¼ ma þ mg (6)
Pressure (bar)
mH2 uH2 ¼ ma ua þ mg ug (7)
90
Absolute Adsorption (g/kg)

80 77 K
ma ¼ mAC Na (8)
70
60 mg ¼ ½ð1  rb =rc ÞVm  Va rg (9)
50
where Vm is the volume of the storage media, and Va ¼ vamAC.
40
By referencing the internal energy of adsorbed H2 with respect
30 to the enthalpy of gas phase H2 and its heat of adsorption
20 (which is a function of H2 uptake) as
10 297 K
0 ua ¼ hg  Dha ; (10)
0 20 40 60 80 100 120 140 160 180 200
Pressure (bar) it can be shown that the total internal energy of stored H2 can
Fig. 1 – H2 uptake (excess and absolute) in AX-21 from 77 K be represented by the following equation.
to 297 K in increments of 20 K. Experimental data from
Ref. [6]. mH2 uH2 ¼ mH2 hg  ma Dha  ½ð1  rb =rc ÞVm  Va rg ; (11)
 international journal of hydrogen energy 34 (2009) 5476–5487 5479

Note that ua is an extensive property because it depends on dmH2

_ out
¼ m H2
H2 uptake. With the assumption of phase equilibrium, mH2 can dt
also be written as
dP
mH2 ¼ mAC Nex þ ð1  rb =rc ÞVm rg ; (12) ¼0
dt
which can be differentiated, rearranged, and combined with
Eq. (4) to produce the following alternate form of the mass dT Q_ in
¼h
  a  a i
dt vhg
ms Cs þ mH2 vT mAC Na vDh mAC vN Dha
conservation equation. P
vT P vT P

                
vNex r vrg dP vNex vNex r vrg dT
mAC þ 1  b Vm þ mAC _ out
m H2 ¼  mAC þ 1  b Vm (16)
vP T rc vP T dt vT P vT P rc vT P dt
   
r vrg dT
þ 1  b Vm ¼m_ in _ out
H2  mH2 (13) 2.3. Method of solution
rc vT P dt

We can similarly rearrange the energy equation, Eq. (5), as The ordinary differential equations in the dynamic model,
follows. Eqs. (13)–(16), were integrated by using the Adams-Bashford-

             
vhg vDha vNa r dP vhg vDha
mH2 mAC Na mAC Dha  1 b Vm Va þ ms Cs þmH2 mAC Na
vP T vP T vP T rc dt vT P vT P
 
vNa dT  
mAC Dha ¼m_ in _
H2 hin hg þ Q in ð14Þ
vT P dt

Equations (4), (13) and (14) can be used to determine the Molton method as implemented in the Gear package [8]. The
pressure, temperature and H2 disposition(mH2 , ma and mg) in equations were algebraically manipulated to calculate the
the tank for any operating condition such as refueling derivatives sequentially without having to perform iterations
_ out
ðm _ in
H2 ¼ 0Þ, discharge ðmH2 ¼ 0Þ and dormancy and boil-off. The [9]. The overall system parameters were first determined by
equations are equally applicable to adiabatic ðQ_ in ¼ 0Þ and obtaining steady-state solutions to Eqs. (4) and (5) which were
non-adiabatic conditions ðQ_ in s0Þ. The solution for the special coupled to the netting analysis for the dome geometry and
case of dormancy and boil-off is discussed below. carbon fiber thickness and heat transfer analysis for number
of layers of insulation. The Benedict–Webb–Rubin equation of
2.2. Dormancy and boil-off
state, as implemented in REFPROP [10], was deployed to
calculate the density, specific heat and enthalpy of liquefied
During dormancy, P < Pmax so that H2 does not have to be
and gaseous hydrogen. Where available, the algorithms in
vented and m_ in _ out
H2 and mH2 are both equal to zero. One can then
REFPROP were used to calculate the derivatives of H2 density
determine the increase in tank pressure and temperature
and enthalpy with respect to pressure and temperature. As
because of in-leakage of heat by solving the following set of
recommended in Barron [11], we used the Debye model to
equations.
estimate the specific heat of the vessel structural components
that are at or near the H2 storage temperature [9].
dmH2
¼0
dt
h vNex 

 i 3. Results and discussion
rb vrg
dP  mAC vT P þ 1  rc Vm vT P dT
¼ h  

 i
dt mAC vNex þ 1  rb Vm g
vr dt The cryo-adsorption hydrogen storage tank and the associ-
vP T rc vP
T ated internal and external components are shown in Fig. 2.

h
 vDha  vNa 
 i
vhg rb dP _
dT  mH2 vP T mAC Na vP T mAC vP T Dha  1  rc Vm  Va dt þ Q in
¼ h
     i (15)
dt ms Cs þ mH
vhg
mAC Na vDha mAC vNa Dha
2 vT
P
vT P vT P

Consider next the period in which the pressure inside the
tank has reached the set point of the relief valve, which then
lifts and begins to vent H2 to maintain P ¼ Pmax. For this
period m_ out
H2 can be determined by solving the following set of
equations.
Design and analysis parameters for the storage system are
summarized in Table 2. As shown in Fig. 2, we considered
a carbon fiber (CF) composite tank wound on a metal liner. The
composite is made of T700S carbon fiber impregnated with
32% resin by volume and has 2550 MPa tensile strength and
5480 international journal of hydrogen energy 34 (2009) 5476–5487

Carbon Activated Vacuum 1600 kg/m3 density. A netting analysis algorithm for geodesic
Shell Fiber Liner Carbon Foam Support Insulation winding pattern [12] was used to determine the optimal shape
of the dome and the thickness of the geodesic and hoop
windings in the cylindrical section for specified maximum
storage pressure and length-to-diameter ratio. In calculating
carbon fiber thickness, we applied a safety factor of 2.35 and
allowed for <100% translation strength. We assumed that the
carbon fiber translation strength can be linearly interpolated
between 82.5% at 350 bar and 63% at 700 bar and that it can be
extrapolated to pressures outside the 350–700 bar range.
We assumed that the sorbent is in the form of a powder
Relief Valve packed inside an Al alloy foam to compensate for its poor
Sensor P
thermal conductivity. An in-tank heat exchanger was
Pressure Heat Valve included to remove the heat of adsorption during refueling
Flow Regulator Exchanger and to provide the heat of desorption during discharge. The
Controller heat exchanger and manifolds are of Al 2024 construction
with the tube sizes and tube sheet thickness given in Table 2.
Shut-off LN2 LN2 We considered that the heat exchanger is cooled with off-
Valve out H2 in
in board liquid N2 during refueling and heated by forced
To
Engine convection (with the ambient as the heat source) during
hydrogen discharge. Multi-layer vacuum super insulation
Fig. 2 – Schematic of on-board cryo-adsorption system. (MLVSI) is used to minimize heat transfer from the ambient.
We assumed that the MLVSI consists of aluminized Mylar
sheets (28 layers/cm) with Dacron spacer [13]. The insulation
thickness was determined so as to limit the heat transfer to
1 W through the sheets at the storage temperature. We
assumed that an equal heat transfer rate occurs through other
conductive leakage paths.
A first-order analysis indicates that the size of the in-tank
Table 2 – Storage system parameters. heat exchanger is controlled by the heat transfer that needs to
Parameter Reference occur during refueling (hydrogen adsorption) rather than the
values heat transfer during discharge (hydrogen desorption). This is
because the tank must be refueled in 3–5 min, whereas it would
Sorbent Material Superactivated Carbon AX-21
Bulk density 300 kg/m3 take nearly an hour to discharge the tank at the full-flow rate of
Skeletal density 2300 kg/m3 1.6 g/s (the automotive application would rarely, if ever,
Specific area 2800 m2/g require this high a hydrogen delivery rate on a sustained basis).
Thermal conductivity 0.1 W/m K Accordingly, the required heat transfer area must be deter-
Heat Transfer 40-PPI Al 2024 Foam 2-wt% mined to accommodate the average heat transfer rate given by
Support Thermal conductivity 2.4 W/m K
the following difference equation derived from Eq. (4).
Contact resistance 1000 W/m2 K
Thermal U-Tube Heat Exchanger 1     
Material of construction Al 2024 alloy Q_ in ¼ _ in
ms us þ mH2 uH2 2  ms us þ mH2 uH2 1  m H2 hin (17)
tr
Tube ID/OD 9.5/11.9 mm
Tube sheet thickness 0.9 mm where the subscript 2 denotes the conditions after the tank
Insulation Multi-Layer Vacuum Aluminized Mylar has been fully refueled and the subscript 1 denotes the
Super Insulation sheets with conditions after the tank has been completely discharged.
Dacron spacer
Note that care must be exercised in writing the difference
Layer density 28 cm1
equation because ua is an extensive property and the specific
Density 59.3 kg/m3
Pressure 105 torr heats of structural elements are strong functions of
Effective conductivity 5.2  104 W/m K temperature.
Tank T700S Carbon Fiber In conducting system analysis, we made an allowance of
Tensile strength 2550 MPa 30 kg and 25 L for weight and volume of miscellaneous
Density 1600 kg/m3 components that are unlikely to change with the different
L/D 3
operating conditions varied in this study. Piping, pressure
Liner
Material Al 2024 alloy
relief valve, pressure regulating valve, check valve, pressure
Thickness 2.4 mm and temperature sensors, fill valve, shut-off valve, vent valve,
Shell housing for cryogenic valves, heat exchanger for raising the
Material Al 2024 alloy temperature of discharged H2 to the allowable inlet tempera-
Thickness 3 mm ture of the fuel cell system, tank support stand, and the N2/air
System Miscellaneous weight 30 kg
blower (not shown in Fig. 2) were all considered to be ex-vessel
Miscellaneous volume 25 L
miscellaneous components.
 international journal of hydrogen energy 34 (2009) 5476–5487 5481

3.1. Medium storage density

Storage Density in Medium (kg/m3)

70

Fig. 3 presents the calculated hydrogen storage density of AX- 60

Recoverable Gas
21 medium at 100 K and compares it with the density of 50
compressed H2 at the same temperature. 48 kg/m
40
Recoverable Medium
rH2 ¼ rb Nex þ ð1  rb =rc Þrg
30
Fig. 3 indicates that the fraction of the total stored H2 that is
20
adsorbed on activated carbon decreases as the pressure is AX-21
Storage T = 100 K
increased. A breakeven point is reached at 525 bar, at which 10
Minimum P = 8 bar
pressure the storage capacity of the medium (i.e., sorbent and
0
void space) is the same with or without the sorbent. At 0 50 100 150 200 250 300 350 400 450 500
a pressure above the breakeven point, the storage capacity is Storage Pressure (bar)
actually higher if the sorbent is removed from the tank. The
Fig. 4 – Isothermal recoverable H2 storage density in AX-21
breakeven pressure is a function of the storage temperature;
with a minimum discharge pressure of 8 bar.
the higher the storage temperature, the higher is the break-
even pressure. Fig. 3 also includes the capacity of the storage
medium needed to satisfy the initial system target of 36 kg/m3
with an assumed volumetric efficiency of 75%, defined as the 3.2. System storage capacity
ratio of the medium volume to the total volume. At the 75%
volumetric efficiency (which as the subsequent analysis Fig. 6 presents the calculated volumetric and gravimetric
indicates may be difficult to achieve in practice and is a func- capacity of the complete AC storage system. The design and
tion of the storage pressure), H2 has to be stored at a pressure operating conditions are 5.6-kg recoverable H2, 8-bar
higher than 210 bar in order to achieve 36 kg/m3 system minimum discharge pressure, 100-K storage temperature, 50-
volumetric capacity. At 210 bar and 100 K, we calculate that K temperature swing and 11.2-min refueling time. Fig. 6
24.7% of stored H2 is sorbed on activated carbon and the indicates that the system gravimetric capacity initially
remaining 75.3% is present in the bulk gas phase. increases with increasing storage pressure, reaches a plateau,
Fig. 4 shows that the isothermal H2 storage density based and then declines as the pressure is raised to >400 bar. The
on the amount of hydrogen that can be recovered by reducing system volumetric capacity shows a somewhat different
the tank pressure to 8 bar. On a recoverable basis, the break- trend in that it approaches an asymptotic value at pressures
even pressure decreases to 140 bar and, at 75% volumetric >500 bar. Under the conditions of Fig. 6, the AC system can
efficiency, 36 kg/m3 storage density is achieved at a lower achieve a gravimetric capacity of 4.5 wt% at storage pressures
pressure without the sorbent in the tank. between 275 and 400 bar but the system cannot achieve a 36-
Fig. 5 shows that the recoverable H2 storage density of AX- kg/m3 volumetric capacity. Because our interest is in evalu-
21 medium can be enhanced by allowing the tank tempera- ating cryo-adsorption at moderate pressures, the subsequent
ture to rise during discharge, referred to here as a temperature discussion is limited to H2 storage at pressures less than
swing (DT ). With a DT of 50 K, the breakeven pressure 350 bar.
increases to 350 bar. Also, a recoverable system storage Fig. 7 shows the weight and volume distribution of the AC
density of 36 kg/m3 can be reached at 260 bar storage pressure, system at 350-bar storage pressure. We calculate that the
which is somewhat lower than the storage pressure needed system has 29% gravimetric efficiency, defined as the weight
without the sorbent in the tank. Under these operating of the storage medium divided by the total weight of the
conditions, AX-21 stores 16.8% of recoverable H2 at 100 K, with system. The containment (liner, carbon fiber and shell)
the majority of the recoverable H2 being in the gas phase.
Storage Density in Medium (kg/m3)

70
Storage Density in Medium (kg/m3)

80
60
70
50
60
48 kg/m3
50 40 Recoverable Medium
3
Medium 48 kg/m
40 30

30 20 AX-21
Storage T = 100 K
Gas Recoverable Gas
20 10 Minimum P = 8 bar
AX-21 T Swing = 50 K
Storage T = 100 K
10 0
0 50 100 150 200 250 300 350 400 450 500
0
0 50 100 150 200 250 300 350 400 450 500 550 600 650 700 Storage Pressure (bar)
Storage Pressure (bar)
Fig. 5 – Recoverable H2 storage density with 50-K
Fig. 3 – H2 storage density ðrH2 Þ in AX-21 medium at 100 K. temperature swing, Pmin [ 8 bar.
5482 international journal of hydrogen energy 34 (2009) 5476–5487

a constant 14.1 kW), nearly 53% of which is the heat of

System Volumetric Capacity (kg/m3)

System Gravimetric Capacity (wt%)

45
40
2007 Target
35
Gravimetric
30
25
Volumetric
20
15
AX-21
Storage T = 100 K
10
Minimum P = 8 bar
5 ΔT = 50 K
0 0.0
0 50 100 150 200 250 300 350 400 450 500 550 600
Storage Pressure (bar)
Fig. 6 – System volumetric and gravimetric capacity, 100 K
storage temperature, DT [ 50 K, Pmin [ 8 bar.
accounts for 36% and the heat transfer components (foam,
heat exchanger and manifolds) account for 10% of the overall
weight of the system. We also calculate that, at 350 bar storage
pressure, the system has 58% volumetric efficiency, which is
much less than 75% volumetric efficiency assumed in
Sections3.1 and 3.2. Among the balance-of-system compo-
nents, the multi-layer vacuum super insulation and the
carbon fiber are the two largest components, accounting for
nearly 20% of the total volume.
3.3. Refueling and discharge dynamics
Fig. 8 presents the variations of pressure and temperature
with the amount of stored H2 for a scenario in which the tank
is refueled to its maximum capacity (5.6 kg recoverable H2 at
350 bar and 100 K, with a 50-K temperature rise to 150 K at the
end of the hydrogen discharge) in 11.2 min after being
completely discharged to 8 bar. The results can be reinter-
preted for pressure and temperature dynamics by calculating
time from the amount of stored H2 and the H2 refueling rate.
We assumed that H2 is supplied at 25% overpressure and 100 K
and that liquid N2 is circulated through the heat exchanger
tubes to cool the tank internals and to remove the heat of
adsorption. In this scenario, the refueling rate is limited by the
rate of heat transfer. The total cooling duty is 9.4 MJ (at
5.5
adsorption, 37% is the PV work, 7% is the sensible cooling of
5.0
the in-tank structures (heat exchanger tubes, plenum, foam,
4.5
AC medium and liner), and the remaining 3% is due to the
4.0
3.5
cooling of the residual H2 that was in the tank at the start of
3.0 the refueling.
2.5 Fig. 9 presents the variations of pressure and temperature
2.0 as functions of stored H2 for two discharge scenarios, one in
1.5 which heat is supplied at a constant rate of 1.7 kJ/g of H2
1.0 removed, and the second in which the heating is not initiated
0.5 until the tank pressure has decreased to 8 bar. As above, the
results can be reinterpreted for pressure and temperature
dynamics by calculating time from the amount of stored H2
and the H2 discharge rate. The total heat duty is the same in
both scenarios. The first scenario has the advantage of a lower
heating rate (2.6 kW) that may be accommodated with the
heat exchanger designed for refueling with liquid N2. Note
that the tube-side heat transfer coefficient with gas recircu-
lation during discharge will be much smaller than the boiling
heat transfer coefficient obtained with liquid N2 circulated
during refueling. The second scenario maintains the tank at
lower temperatures during discharge and would lead to longer
dormancy. However, the peak heat rate for the second
scenario may be as high as 15 kW, which would be difficult to
accommodate with the heat exchanger that has been sized for
refueling.
3.4. Dormancy and H2 loss
Fig. 10 presents the dormancy (time before any H2 needs to be
vented) and H2 loss from a fully charged tank assuming that
the relief valve is set to lift at 25% above the maximum storage
pressure. It is convenient to express the dormancy in terms of
the cumulative heat leakage into the tank (Wd or Watt-day,
1 Wd ¼ 86.4 kJ) and H2 loss as g/h/W. Fig. 10 indicates that
there is no venting of H2 until a heat input of 18 Wd (1.6 MJ)
has occurred (over 9 days at 2 W heat transfer rate) and the
temperature has risen by 16 K. Hydrogen then vents at an
initial rate of 0.8 g/h/W, which rate decreases with time as the
amount of H2 in the tank decreases. Even if the tank warms to
the ambient temperature (i.e., no more heat in-leakage), there
is nearly 3 kg of H2 still remaining in the tank at 440 bar, i.e.,
the maximum H2 loss is limited to 50% of the initial charge.

Volume Distribution
Weight Distribution
Misc
Manifold
Misc 14%
1%
24% Medium
HXT
29%
1%
Manifold
1% MLVSI
12%
HXT
Shell Medium
4%
Foam 3% 58%
MLVSI
1% 5% CF
Shell Liner 8%
11% 6% Liner
CF Foam
19% 2% 1%

Fig. 7 – System weight and volume distribution, Pmax [ 350 bar, other conditions as in Fig. 6.
 international journal of hydrogen energy 34 (2009) 5476–5487 5483

160 400 450 1.0

P 0.9
140 350 400
Temperature

Boil Off Rate (g/h/W)

350 0.8
120 300
Temperature (K)

Pressure (bar)
0.7

P (bar), T (K)
300
100 250 Boil Off Rate 0.6
250
80 200 0.5
200
60 150 T 0.4
Pressure 150
0.3
40 100
100 Storage Pressure = 350 bar 0.2
20 50 Storage Temperature = 100 K
50 Vent Pressure = 440 bar 0.1
0 0 0 0.0
0 1 2 3 4 5 6
0 20 40 60 80 100 120 140 160 180 200
Mass of H2 in Tank (kg) Cumulative Heat Transfer (Wd)
Fig. 8 – Dynamics of H2 refueling of a fully depleted tank Fig. 10 – Thermodynamics of H2 storage and dormancy,
with constant cooling rate, initial conditions: P [ 8 bar, initial conditions: P [ 350 bar, T [ 100 K.
T [ 150 K.

H2 is withdrawn from the cylinders, cooled to 100 K in the off-

Dormancy and the temperature at which the tank begins to board heat exchanger, and supplied to the on-board tank.
vent hydrogen are also a function of the initial amount of H2 Liquid N2 (denoted as LN2 in Fig. 12) is pumped to the on-board
stored, as shown in Fig. 11. The dormancy is seen to increase tank to remove the heat of adsorption and cool the internal
to >200 Wd (from 18 Wd) and the vent temperature to >200 K structures. An excess of liquid N2 is supplied to the on-board
(from 116 K) if the tank is initially only half full. tank to maintain two-phase flow in the in-tank heat
The calculated dormancy of the cryo-adsorption system is exchanger tubes and to prevent dryout (which would decrease
quite comparable to the dormancy of the cryo-compressed the available cooling rate). The liquid N2 that boils off is
system operating under similar conditions [9]. However, the replenished with makeup liquid N2 to precool H2 in the off-
cryo-adsorption system has longer dormancy than the board heat exchanger.
conventional low-pressure liquid H2 system because of its The off-board refueling system configuration shown in
larger thermal capacity, the storage medium’s heat of Fig. 12 was selected to keep the consumption of liquid N2 to
desorption, absence of phase change and the consequent a minimum by discharging N2 at a temperature only 20 K
rapid expansion, and storage in a pressure vessel. below the ambient. This also reduces the size of the in-tank
heat exchanger by pre-cooling H2 in the off-board heat
3.5. H2 refueling system exchanger.
We estimated that the off-board heat exchangers account
We have estimated the electrical energy needed to store H2 at for 62% of the 4.5 MJ/kg-H2 or 10.9 kg-LN2/kg-H2 overall cryo-
350 bar and 100 K using the off-board refueling system shown genic cooling duty. Liquid N2 is generally produced by air
in Fig. 12. The analysis assumed that a distributed steam liquefaction and separation [11]. Using a figure of merit of
methane reformer equipped with pressure swing adsorption 0.205 for a commercial liquid N2 unit appropriate for a refuel-
for H2 purification supplies H2 at 20 bar, and that all cryogenic ing station [14], we calculated the electrical energy
cooling is accomplished using liquid N2. The refueling system
compresses H2 to 440 bar using a multi-stage compressor
Dormancy (W.d), Initial H2 Stored (%)

train, and stores it in a bank of compressed H2 cylinders. The

200 200
180 Storage Pressure = 350 bar 190
Storage Temperature = 100 K
Vent Temperature (K)

180 400 160 Vent Pressure = 440 bar 180

160 350 140 170
Constant Heat Rate
Dormancy 160
140 120
300 Vent Temperature
Temperature (K)

Pressure (bar)

Temperature 100 150

120
250
80 140
100
Variable Heat Rate 200 60 130
80 Ha Stored
150 40 120
60
Pressure 20 110
40 100
Constant Heat Rate Variable Heat Rate 0 100
20 50 0 50 100 150 200 250 300 350 400

0 0 Initial Pressure (bar)

0 1 2 3 4 5 6
Mass of H2 in Tank (kg) Fig. 11 – Duration of dormancy and tank temperature at
which H2 is vented, as a function of the amount of H2
Fig. 9 – Dynamics of H2 discharge under scenarios of stored in the tank at 100 K at the beginning of the
constant and variable heat rates. dormancy period.
5484 international journal of hydrogen energy 34 (2009) 5476–5487

support. The first set of simulations indicates that the engi-

H2,20 bar 440 bar
300 K
EM
Compressor Train
Heat
Exchanger
100 K
LN2+ N2 N2
77.4 K
LN2 Makeup
LN2 LN2
On-Board 77.4 K
AC Tank
Fig. 12 – Refueling system with off-board liquid N2 cooling.
requirement to be w1 kWh/kg-N2 or 10.9 kWh/kg-H2, which
may be compared to the 7–14 kWh/kg-H2 electricity
consumption for centralized H2 liquefaction plants [15]. We
conclude that producing liquid N2 by air liquefaction is not an
especially attractive route for cryogenic cooling of the on-
board H2 storage system. Other options of producing liquid N2
by indirect routes (e.g., employing cryogenic He to cool N2 in
a closed cycle) may need to be investigated.
3.6. Engineered activated carbon
We have used the integrated model to determine the attri-
butes that an engineered sorbent must have to achieve 4.5-
wt% H2 gravimetric capacity and 36 kg-H2/m3 volumetric
capacity for the system. We assumed that the H2 is to be
stored at 100 bar and that off-board liquid N2 is available to
cool the storage tank during refueling at a rate of 0.5 kg-H2/
min. We further assumed that the sorbent has thermody-
namic properties of AX-21 but advances are made to fabricate
this storage medium with higher surface area and bulk
density, so that Eqs. (1) and (2) describe the adsorption
isotherms for the engineered activated carbon with Nmax
given by Eq. (3), after applying a scaling factor for the
enhanced surface area.
Table 3 summarizes results from two sets of simulations,
one with and the other without a conductive heat transfer
neered AC will need to have a specific area greater than
Off-Board
H2 Storage 6824 m2/kg and a bulk density greater than 544 kg/m3. An
engineered AC with these attributes will have 107 g-H2/kg
excess sorption at 100 K and 100 bar. As a comparison, AX-21
N2 has excess sorption of 44 g-H2/kg under the same conditions
280 K
of pressure and temperature. Our simulations showed that
the storage system with the engineered AC will adsorb 76.6%
of total H2 and that 76.7% of sorbed H2 is recoverable within
the operating envelope of pressures and temperatures. We
calculated that the on-board cooling duty increases to 2.8 MJ/
kg-H2 from 2 MJ/kg-H2 for AX-21. The excess sorption
requirement decreases to 94 g-H2/kg if the minimum delivery
pressure is 4 bar, and to 90 g-H2/kg if the minimum delivery
pressure is further lowered to 3 bar, as specified in the 2010
and 2015 storage system targets, respectively (see Table 1).
The second set of simulations was run assuming that the
thermal conductivity of the medium is improved to 2.5 W/m.K
(the value for 2-wt% Al foam) so that the conductive heat
transfer support can be discarded. The results in Table 3
indicate that eliminating the heat transfer support reduces
the specific area and excess adsorption requirements by
9–10%, although the bulk density has to increase by about 8%.
Increasing surface area represents one approach to
enhancing sorption capacity. Our simulations show that the
surface area and bulk density must be increased simulta-
neously. To achieve such increases, a materials breakthrough
will be needed because the conventional experience shows
that any increase in surface area results in a decrease in the
material’s bulk density, and vice-versa. For example, consol-
idating AX-21 from 300 to 700 kg/m3 has resulted in decreasing
the specific area from 2800 to 2000 m2/g. An alternative
approach to enhancing a material’s sorption capacity is to
increase its H2 binding energy (i.e., increase Dha). We will
report on system level analysis of cryo-adsorption with higher
binding energy materials (such as MOFs) in a future
publication.
3.7. Adiabatically refueled system
We have also assessed the option of adiabatically refueling the
storage system with liquefied H2 (LH2) as a means of over-
coming the inefficiency of cooling it with liquid N2. This option
may be attractive in that an off-board coolant is not required

Table 3 – Material attributes needed to meet 2007 system capacity targets (100 bar, 100 K, DT [ 50 K).
Designation Minimum Pressure Specific Area Bulk Density Nex H2 in AC Recoverable H2 in AC Cooling Duty
2
Bar m /kg kg/m3 g-H2/kg % % MJ/kg-H2

With Foam (Low Conductivity AC)

AX-21 8 2800 300 44 39.4 76.7 2.0
EAC-11 8 6824 544 107 76.6 76.7 2.8
EAC-21 4 5968 551 94 74.5 85.4 2.7
EAC-31 3 5736 553 90 62.7 88.3 2.6
Without Foam (AC Conductivity ¼ 2.4 W/m K)
EAC-12 8 6222 587 98 76.8 76.7 2.7
EAC-22 4 5445 594 85 74.6 85.4 2.6
EAC-32 3 5238 596 82 73.9 88.3 2.6
 international journal of hydrogen energy 34 (2009) 5476–5487 5485

leading to a simplification of the forecourt layout and the a 60

refueling process. An in-tank heat exchanger, however, is still

Temperature Swing (K)

needed to effect a temperature swing and assist in desorbing 50
the H2 and maintaining the tank pressure at or above the
40
minimum specified H2 discharge pressure. The average heat
transfer rate during the discharge can be determined from the 30
following difference equation.
20
1     
Q_ in ¼ ms us þ mH2 uH2 2  ms us þ mH2 uH2 1 10
td
Z
1 2 out 0
þ m_ H2 hout dt (18)
td 1 100 105 110 115 120 125 130 135 140 145 150
Storage Temperature (K)
where the subscript 2 denotes the conditions after the tank
has been completely discharged and the subscript 1 denotes
b 40
the conditions after the tank has been fully refueled. We have

Excess Adsorption (g/kg)

assumed that a heat transfer coefficient of 100 W/m2 K can be 35
Excess Adsorption
obtained with forced air convection on the tube-side (may 30
require use of extended surfaces). The power consumed by 25
the blower is not included in the results discussed below. 20
Recoverable

Fig. 13a shows the relationship between the storage

15
temperature and the temperature swing that can be accom-
modated if the tank is refueled adiabatically with liquid H2 at 10

20 K pumped to 350 bar. There exists a minimum storage 5

temperature (w105 K) that can be maintained with adiabatic 0
100 105 110 115 120 125 130 135 140 145 150
refueling. This minimum temperature depends on the oper-
Storage Temperature (K)
ating pressures but is primarily a function of the amount of H2
adsorbed, the extent to which H2 is desorbed within the
pressure and temperature swings, and the heat of adsorption.
c
SystemVolumetric Capacity (kg/m3)

System Gravimetric Capacity (wt%)

Fig. 13a shows that the temperature swing that can be sus- 28.4 4.8
tained with adiabatic refueling increases with the storage 28.2
Volumetric
4.7
temperature, from 0 for 105 K storage temperature to >50 K
28.0 4.6
for 150 K storage temperature.
27.8
Fig. 13b displays the sorption capacity of AX-21 under 4.5
27.6
adiabatic refueling conditions. The excess sorption capacity is 4.4
27.4
a function of the storage pressure and temperature, and it 4.3
27.2
decreases monotonically as the storage temperature Gravimetric
27.0 4.2
increases. The recoverable sorption capacity, however, is also
26.8 4.1
influenced by the allowable swings in pressure and tempera-
ture; it actually increases with temperature over the range 26.6 4.0
100 105 110 115 120 125 130 135 140 145 150
105–150 K because of the relationship between the tempera- Storage Temperature (K)
ture swing and storage temperature. Fig. 13b indicates that the
recoverable fraction of excess sorbed H2 increases from w18% Fig. 13 – Performance of cryo-adsorption storage system
at 105 K (DT ¼ 0 K, DP ¼ 342 bar) to w88% at 150-K storage with adiabatic liquid H2 cooling as a function of storage
temperature (DT ¼ 53 K, DP ¼ 342 bar). Above 150 K, the temperature, Pmax [ 350 bar: a) Temperature swing, b)
recoverable sorption capacity decreases with increasing Excess and recoverable H2, c) System volumetric and
temperature because the excess sorption capacity decreases gravimetric capacity.
faster than the increase in the recoverable fraction.
Fig. 13c shows that there is an optimum storage tempera-
ture (w115 K, DT ¼ 5.5 K) at which the AC storage system has
the highest volumetric capacity under adiabatic refueling because of higher storage temperature (115 K vs. 100 K) and
conditions (DP ¼ 342 bar). There is also a similar, and nearly smaller temperature swing (5.5 K vs. 50 K).
coincidental, optimum temperature for the system gravi- As a reference point, we have evaluated the gravimetric and
metric capacity as well. At these optimum temperatures, volumetric capacity of the cryo-compressed system (no
excess adsorption accounts for nearly 18.5% of the total stored sorbent) that stores gaseous H2 under the same operating
H2 and 8.8% of recoverable H2. Because of the relatively small conditions as in Fig. 13. We have made an additional assump-
amount of sorbed H2, the optimum temperature for system tion that a shell-side (outside the heat exchanger tubes) heat
capacity is lower than the temperature at which the recover- transfer coefficient of 10 W/m2 K can be obtained with natural
able sorbed amount is highest (150 K in Fig. 13 b). Also, the convection of H2 in the storage tank. Fig. 14 presents the
volumetric and gravimetric capacities are both lower with temperature swing attainable with liquid H2 refueling as
adiabatic LH2 refueling than with off-board LN2 refueling a function of the storage temperature (350 bar peak and 8 bar
5486 international journal of hydrogen energy 34 (2009) 5476–5487

temperatures as a way of meeting the automotive hydrogen

a
180 storage targets for volumetric and gravimetric capacity and
other operating requirements. Our principle conclusions are
160
Temperature Swing (K)

summarized below.
140
120
 The suitability of a particular sorbent is best determined by
100 the recoverable hydrogen capacity of the material and the
80 system. The recoverable capacity depends on the storage
60 pressure and temperature, and also on the pressure and
40 temperature swings. Our analyses show that without
a temperature swing, >80% of the sorption capacity of AX-21
20
at 100 K and 100 bar is irrecoverable if the minimum
0
50 55 60 65 70 75 80 85 90 95 100 delivery pressure is 3–8 bars.
Storage Temperature (K)  For a hydrogen storage temperature of 100 K and an allow-
b able temperature rise of 50 K, our analyses show that the
use of a sorbent such as AX-21 does not enhance the
System Volumetric Capacity (kg/m3)

System Gravimetric Capacity (wt%)

40 8.0
hydrogen storage capacity over that of just the cryo-
39 7.8
compressed H2 gas at the same temperature and pressure.
38 7.6
 For the conditions considered in our analyses, a fully
Gravimetric
37 7.4
charged AC storage system has dormancy of 18 Wd (i.e., 9
36 7.2 days at 2 W heat in-leakage rate). Even under prolonged
35 7.0 conditions of non-use of the H2, the storage system will
Volumetric
34 6.8 retain half of the total amount of H2 in full tank.
33 6.6  For a cryo-adsorption hydrogen storage system that uses
32 6.4 off-board liquid N2 to cool the dispensed H2 and remove the
31 6.2 on-board heat of adsorption during vehicle refueling, our
30 6.0 analyses show that to produce the requisite amounts of
60 65 70 75 80 85 90 95 100
Storage Temperature (K) liquid N2, approximately 11 kWh of electricity would be
consumed per kilogram of H2 dispensed to the vehicle. We
Fig. 14 – Performance of cryo-compressed storage system also analyzed an alternative, adiabatic refueling option with
with adiabatic liquid H2 cooling as a function of storage liquefied H2, which may simplify the on-board and off-board
temperature, Pmax [ 350 bar: a) Temperature swing, b) hydrogen storage systems, if liquefied H2 is available at the
System volumetric and gravimetric capacity. fueling station.
 We have also estimated that for an AX-21-like sorbent,
increases of 140% in the specific surface area and 80% in the
minimum pressure). As expected, the minimum storage
bulk density would be needed to make such materials
temperature is lower and the attainable temperature swing is
suitable for the automotive hydrogen storage application.
much larger than with the sorbent in the tank (Fig. 13a). We
calculate that the cryo-compressed system can reach a peak
gravimetric capacity of 7.8 wt% H2 and a volumetric capacity of
39.4 kg/m3 at 60-K storage temperature (DT ¼ 75 K). In a sepa- Acknowledgements
rate study [16], we have reported comparable system capacities
of 6.7 wt% and 34.3 kg/m3 for the Lawrence Livermore National This work was supported by the U.S. Department of Energy’s
Laboratory’s 2nd Generation cryo-compressed system [17–19] Office of Energy Efficiency and Renewable Energy. Dr. Sunita
with aluminum alloy (rather than stainless steel) shell and use Satyapal of the Office of Hydrogen, Fuel Cells, and Infra-
of thinner insulation. We calculate higher volumetric and structure Technologies was the Technology Development
gravimetric capacities for the cryo-compressed system than Manager for this study. The authors thank Dr. Romesh Kumar
for the cryo-adsorption system because the operating pressure of Argonne National Laboratory for many useful discussions
is much above the breakeven pressure and the temperature and helpful suggestions. Argonne National Laboratory, a U.S.
swing is larger. Department of Energy Office of Science laboratory, is operated
by UChicago Argonne, LLC, under Contract No. DE-AC02-
06CH11357.
4. Summary and conclusions

We have formulated an integrated system model that

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