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A lumped-parameter model for cryo-adsorber
hydrogen storage tank
V. Senthil Kumara,*, K. Raghunathana, Sudarshan Kumarb
aIndia Science Lab, General Motors R & D, Creator Building, International Technology Park, Bangalore 560066, IndiabChemical and Environmental Sciences Lab, General Motors R & D, 30500 Mound Road, Warren, MI 48090, USA
a r t i c l e i n f o
Article history:
Received 24 March 2009
Received in revised form
30 April 2009
Accepted 1 May 2009
Available online 2 June 2009
Keywords:
Hydrogen storage modeling
Cryogenic adsorption
Metal-organic frameworks
a b s t r a c t
One of the primary requirements for commercialization of hydrogen fuel-cell vehicles is
the on-board storage of hydrogen in sufficient quantities. On-board storage of hydrogen by
adsorption on nano-porous adsorbents at around liquid nitrogen temperatures and
moderate pressures is considered viable and competitive with other storage technologies:
liquid hydrogen, compressed gas, and metallic or complex hydrides. The four cryo-
adsorber fuel tank processes occur over different time scales: refueling over a few minutes,
discharge over a few hours, dormancy over a few days, and venting over a few weeks. The
slower processes i.e. discharge, dormancy and venting are expected to have negligible
temperature gradients within the bed, and hence are amenable to a lumped-parameter
analysis. Here we report a quasi-static lumped-parameter model for the cryo-adsorber fuel
tank, and discuss the results for these slower processes. We also describe an alternativesolution method for dormancy and venting based on the thermodynamic state description.
2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights
reserved.
1. Introduction
One of the primary requirements for thecommercialization of
hydrogen fuel-cell vehicles is the on-board hydrogen storage
for a range of about 500 km, see Satyapal et al. [1]. On-board
storage of hydrogen by adsorption at low temperatures(around 77 K, liquid nitrogen temperature) and moderately
high pressures (less than 60 bar) is considered viable and
competitive with other storage technologies: liquid hydrogen,
compressed gas, and metallic or complex hydrides, see Zhou
[2]. Nano-porous metal-organic frameworks (MOFs) as adsor-
bents offer good gravimetric capacity and fast and reversible
kinetics. For example, MOF-5 has a reversible maximum
excess adsorption capacity of about 6 wt% at 77 K, see Zhou
et al. [3]. MOF-5 is the adsorbent considered in this report to
study the fuel tank performance.
In this work we assume that the operating pressure of the
cryo-adsorber fuel tank is 20 bar. We assume that liquid
nitrogen at 77 K is available as a coolant at the fuel station.
Hence, the lowest temperature of the cooled hydrogen feed
gas is about 80 K. The four processes occurring in a cryo-
adsorber fuel tank are:
Refueling A depleted fuel tank at low pressure (say 1.1 bar)
and higher temperature (say 120 K) is charged with
hydrogen. Heat released during adsorption is removed by
the recirculation of cool hydrogen gas entering at 80 K.
Discharge When the vehicle is in motion, the fuel-cell stack
demands are met by desorbing hydrogen from the cryo-
adsorber bed. Desorption is enhanced by therecirculation of
hot hydrogen gas. The tank pressure eventually drops to
1.1 bar.
* Corresponding author. Tel.: 91 80 41984567; fax: 91 80 41158262.E-mail addresses: [email protected], [email protected] (V. Senthil Kumar).
A v a i l a b l e a t w w w . s c i e n c e d i r e c t . c o m
j o u r n a l h o m e p a g e: w w w . e l s e v i e r . c om / l o c a t e / h e
0360-3199/$ see front matter 2009 International Association for Hydrogen Energy. Published by Elsevier Ltd. All rights reserved.doi:10.1016/j.ijhydene.2009.05.025
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Dormancy & Venting While the vehicle is parked, its pres-
sure builds up to vent pressure, say 25 bar, due to contin-
uous heat leak into the fuel tank, and gas is vented to the
fuel cell or atmosphere. The process of venting is also called
boil-off, by analogy with liquid hydrogen storage systems.
The time period until the start of venting is called
dormancy.
These fuel tank processes occur over different time scales:
refueling over a few minutes, discharge over a few hours,
dormancy over a fewdays, andventing overa fewweeks. When
themoleculartransportprocessesare fast, slower processeslike
discharge, dormancy and venting are expected to have negli-
gible internal gradients and are generally amenable to a lum-
ped-parameter analysis. In thisreport we describe a quasi-static
lumped-parameter model for the cryo-adsorber fuel tank, and
present the results for these slower processes. The fastest fuel
tank process, refueling, requires higher dimensional models to
describe the temperature gradients occurring within the bed,
and these are being currently developed.
Section 2 describes the adsorption datafor MOF-5. Section 3describesa fuel tank designconsidered in this study. Section 4
identifiesthe assumptions involved in the model development
and Section 5 presents the quasi-static lumped-parameter
model for the cryo-adsorber. The simulation results for
dormancy, venting and discharge are presented in Sections 6
8, respectively. While some of the thermophysical properties
are directly taken fromexisting databases, someare computed
in this work; these details are given in the appendix.
2. Adsorption data
Zhou et al. [3] have reported the adsorption data for MOF-5
powder over a wide range of temperature and pressure. Over
the range of 60125 K temperature and 130 bar pressure, their
excess adsorption data canbe fitted to a Langmuir isotherm of
the following form:
qT; P qmbP
1 bP; (1)
b b0 exp
B
T
; (2)
qm qm0
fT; (3)
where we have assumed
fT 1 AT2: (4)
For the hydrogen adsorption data in AX-21, Benard and
Chahine [4] use
fT 1 AT: (5)
However, for the MOF-5 data in the considered range of
temperature and pressure, we find that equation (4) gives
a good fit. Fig. 1 shows the Langmuir fit for data in the range
130 bar and 60125 K, with the following parameters :b0 2.8164 10
3 bar1, B 332.0158 K, qm0 11.7134 102
kg H2/kg MOF and A 131.3231 106 K2. At 20 bar and 77 K,
these parameters give q* 0.0532 kg H2/kg MOF.
ForMOF-5 powderZhou et al. [3] reporta skeletal density of
about 1.78 g/cc and 66.2% porosity. Due to thelack of densified
MOF-5 adsorption data, we assume that MOF-5 pellets have
same density as the powder. Hence, solid density
rs 1780 kg/m3, pellet porosity 3p 0.662, and pellet density
rp rs
1 3p
601:64 kg=m3: (6)
Assuming a dense random packing of spheres gives a bed
porosity of3b 0.36, bed density
rb rp1 3b 385:05kg=m3 (7)
and total porosity
Nomenclature
T, P Temperature and pressure, K, bar
ms, Vb Skeletal mass and volume of the adsorbent bed,
kg, m
3
mw Mass of tank wall, typically steel, kg_mf; _m Inlet and outlet gas mass flow rates, kg/s
3p, 3b, 3t Pellet, bed and total porosities, 3t 3b (1 3b)3p,
m3/m3
rs, rp, rb Skeletal, pellet and bed densities, rp rs(1 3p),
rb rp(1 3b), kg/m3
rg, vg Gas density and specific volume vg 1/rg, kg/m3,
m3/kg
mg, kg, ks Gas viscosity, gas thermal conductivity and
adsorbent thermal conductivity, Pa s, W/m/K,
W/m/K
dp Pellet diameter, m
U Superficial bed velocity, m/shg Convective heat transfer coefficient on the surface
of a pellet, W/m2/K
Nu, Bi, Re, Pr Nusselt, Biot, Reynolds and Prandtl numbers
vw; vs Mean specific volumes of the steel and
adsorbent, m3/kg
aPg; kTg Isobaric thermal expansion coefficient and
isothermal compressibility, 1/K, 1/barHg, Hq, Hs, Hw Specific enthalpy of gas, adsorbate, adsorbent
(solid) and steel components (wall), J/kg
CPg, CPs, Cpw Specific heat capacity of gas, adsorbent and
steel, J/kg/K_Ql; _Qh Heat leak rate, heat addition rate into the
tank, W
q, q* Excess adsorbate concentration and its
equilibrium value, kg H2/kg adsorbent
qm, b The two Langmuir adsorption isotherm
parameters, kg/kg, 1/bar
DHa Heat of adsorption, J/kg H2 adsorbed
Hsys Enthalpy of the inner thermal masses, J
TN Ambient temperature, KReff Effective resistance for heat leak into the
inner thermal masses, K/W
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3t 3b 1 3b3p 0:7837: (8)
For MOF-5 Panella et al. [5] report a heat of adsorption of
3.8 0.8 kJ/mol, Dailly et al. [6] report 4.1 kJ/mol, Kaye and
Long [7] report 4.75.2 kJ/mol, and Zhou et al. [3] report an
initialheat of adsorption of about 4.8 kJ/mol. Here we assume
a constant average heat of adsorption DHa 4.0 kJ/mol.
3. Fuel tank design
A lumped-parameter model does not distinguish between
different packed bed designs. Hence for illustration we
assumea longitudinal packed bed as shown in Fig. 2. A header
distributes the hydrogen feed stream to a packed bed of cryo-
adsorbent pellets. The bed adsorbs hydrogen, the unadsorbed
gasflow gets collected andflows outof the tank. Hydrogen gas
flowing out of the tank can be cooled and recirculated for
further adsorption.
The adsorbent bed is designed for an assumed 5 kg total
hydrogen capacity at 20 bar and 77 K, with 20% excess bed
mass allowed to provide for operating temperatures higher
than 77 K. Total hydrogen in the fuel tank, at any temperature
and pressure, is the sum of hydrogen in the adsorbed and gas
(in bed voids and pellet pores) phases. Thus,
mH2 T; P msqT; P Vb3trgT; P: (9)
At 20 bar and 77 K, rg 6.4851 kg/m3. Using these values in
Equation (9) gives an adsorbent mass of 75.3 kg. Allowing
a 20% excess gives ms 90.37 kg and Vb 0.2347 m3 234.7 l.
The bed volume will be significantly lower for densified
adsorbent pellets.
4. Model assumptions
In the next section we develop a quasi-static lumped-param-eter model for the cryo-adsorber, andhere we justify or list the
assumptions of quasi-static behavior and lumping. Quasi-
static behavior implies local thermal and mass equilibrium at
any time i.e. the transient system passes through a series of
equilibrium states. The adsorbents typicallyoffer largespecific
internal surface area, leading to intimate gassolid contact.
Hence, at any location within the bed, there is negligible
temperature difference between the solid and the gas i.e.
Ts r!; tzTg r
!; thT r!; t; (10)
and the adsorbate loading is close to its equilibrium value i.e.
q r!
; tzq
T r!
; t; P r!
; t: (11)These near-equalities can be easily demonstrated using
heat and mass transfer correlations for packed beds, see for
example Wakao et al. [8] and Wakao and Funazkri [9]. These
quasi-static approximations are implicitly assumed for
example in the work of Mota et al. [10]. The advantages of
quasi-static approximation are the following: when local
thermal equilibrium prevails a single energy balance can be
used to describe both solid and gas phases; when local mass
equilibrium prevails, we can replace dq/dt (usually described
using a linear driving force model) by dq*/dt. When the fuel
tank processes are quasi-static, to design or simulate the fuel
tank, only adsorption isotherms and heat capacity of the
adsorbent need to be measured at different temperatures.A lumped-parameter model involves intra-pellet lumping
andacross-the-bedlumping of temperature, pressure andsolid-
phase concentration fields. The intra-pellet lumping of
temperature and concentration can be systematically justified
by a Biot number analysis. For example at 80 K and 20 bar, the
hydrogen gas thermal conductivity is 0.061663 W/m/K, NIST
web book [11]. Then, for a 0.5 mm diameter pellet, in the stag-
nant gas limit from Nu hgdp/kg 2 we get the convective heat
transfer coefficient as hg 246.65 W/m2/K. Huang et al. [12]
report an effective thermal conductivity ofksz 0.32 W/m/K for
MOF-5. Using all these data we compute the Biot number of
a spherical pellet as Bi hgdp/6ks 0.0642. Since the computed
Biot number is lower than 0.1, we can safely assume that the
pellets are thermally thin i.e. the intra-pellet temperature
gradients are negligible, see Incropera et al. [13].
Fig. 2 Fuel-tank details: longitudinal (left) and cross-
sectional (right) views.
Fig. 1 Langmuir fit (lines) for MOF-5 excess adsorption
data (symbols) of Zhou et al. [3].
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The pressure drop across a bed of highly porous pellets is
often negligible, and it can be easily shown using an Ergun
equation analysis or see for example the results of Sankararao
and Gupta [15], justifying an across-the-bed pressure lumping.
For example at 80 K and 20 bar, the hydrogen gas density and
viscosity are 6.2069 kg/m3 and 3.7453 106 Pas, NIST web book[11]. We assume a particle diameter of dp 0.5 mm and a bed
porosity of 3b 0.36. For a particular design of 0.5467 m diam-
eter, a 60 g/s flow of 80 K 20 bar gas corresponds to a superficial
velocity of U 0.041181 m/s. Using these values in the Ergun
equation DP/L amgU brgU2, where a 1501 3b
2=33bd2
p and
b 1:751 3b=33bdp, Bird et al. [14], gives DP/L 0.013 bar/m,
which is negligible compared to the feed pressure of 20 bar.
Across-the-bed lumping of temperature and concentration
fields is intuitively assumed for the slower tank processes:
discharge, dormancy and venting. For a fast process like
refueling, however, we anticipate significant temperature
gradients within the bed for which higher dimensional
models are being currently developed.
5. Model development
The quasi-static lumped-parameter model contains transient
mass and energy balances, resulting in two equations. For
a given bed and feed flow (when present), there are three
unknowns: the tank temperature, pressure and mass outflow
rate. Closure is achieved by specifying one of these three
unknowns:
1. During discharge the mass outflow rate is specified by the
fuel-cell demand. Hence, the model is solved for tempera-ture and pressure.
2. During dormancy the outflow is zero by definition. Hence,
the model is solved for temperature and pressure.
3. The vent is typically operated by a pressure controller.
Therefore neglecting valve transients, venting can be
treated as an isobaric process. Hence, the model is solved
for mass outflow rate and temperature.
5.1. Transient mass balance
The rate of change of hydrogen content of the tank balances
the net flow into the tank. Hence the transient mass balance
for hydrogen is given by
dmH2dt
_mf _m: (12)
Using Equation (9) we get
msdqdt
Vb3tdrgdt
_mf _m: (13)
Now, expressions are developed for the two time deriva-
tives in the above equation. Assuming that the gas phase is in
equilibrium at the corresponding temperature and pressure
gives
rgt rgTt; Pt: (14)
Then,
drgdt
vrg
vT
P
dTdt
vrg
vP
T
dPdt
: (15)
The isobaric temperature derivative of density is related to
the isobaric thermal expansion coefficient aPg according to
aPg 1vg
vvgvT
P
1rg
vrg
vT
P
(16)
The isothermal pressure derivative of density is related to
the isothermal compressibility factor according to
kTg 1
vg
vvgvP
T
1rg
vrg
vP
T
; (17)
see Smith et al. [18], page 62. Using these results, the time
derivative of density is given by
drgdt
rgaPgdTdt
rgkTgdPdt
: (18)
The quasi-static approximation for the adsorbateconcentration
qt qTt; Pt (19)
gives
dqdt
dq
dt
vq
vT
P
dTdt
vq
vP
T
dPdt
: (20)
The temperature-dependence ofq* comes from that of the
two Langmuir parameters: b(T ) and qm(T ). Using Equations (2)
and (3), and simplifying give
vqvT
P q
f0TfT
B
1 bPT2!: (21)
The pressure dependence of q* is only due to the explicit P
terms. Hence, from Equation (1) we get
vq
vP
T
q
1 bPP: (22)
Using Equations (21) and (22) in (20) we get
dq
dt q
f0T
fT
B
1 bPT2
!
dTdt
q
1 bPP
!
dPdt
: (23)
Using equations (18) and (23) in equation (13) and rear-
ranging, the transient mass balance takes the form
a11dTdt
a12dPdt
b1; (24)
with
a11 msq
f0T
fT
B
1 bPT2
! Vb3trgaPg; (25)
a12 msq
1 bPP Vb3trgkTg; (26)
and
b1 _mf _m: (27)
Note that the dimensions of a11, a12and b1 are mass/
temperature, mass/pressure and mass/time, respectively.
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5.2. Transient energy balance
The thermal masses associated with the fuel tank are the gas
phase, adsorbed phase, adsorbent, pressure vessel including
the bed restrainers and other bed internals, insulation layer,
outer shell and ambient, as shown in Fig. 2. The insulationlayer isolates the inner thermal masses (gas, adsorbed phase,
adsorbent, and pressure vessel) from the outer ones (shell and
ambient). When the fuel-tank processes are slow, a single
lumped temperature can be used for the inner thermal
masses. Sircar [16] shows that any adsorption measurement
directly gives only the Gibbsian surface excess adsorption and
not the absolute adsorption, and suggests using mass and
energy balances with excess adsorption to simulate practical
adsorption systems. The transient energy balance for the
inner thermal masses (system) is given by
dHsys
dt _mfHgTf; Pf _mHgT; P _Ql Vb3t
dP
dt: (28)
Computation of Hsys is elaborated in the appendix. Each
term in the above equation is analyzed below, and the time
derivatives of temperature and pressure are collected
explicitly.
The differential change in the enthalpy of inner thermal
masses is defined as
dHsysT;P dmwHw dmsHs d
msqHq
d
Vb3trgHg: (29)
All the steel components in the inner thermal masses
(distribution tubes, restrainers, holding plates and pressure
vessel) are accounted as a steel wall of mass mw. For
a particular design for example we had mwz 125 kg. Adsor-bate enthalpy is obtained from the definition of heat of
adsorption as
Hq Hg DHa: (30)
This study assumes a constant average heat of adsorption,
independent of temperature and pressure. Hence, dHq dHg,
and
dHsysT; P mwdHw msdHs
msq Vb3trg
dHg
ms
Hg DHadq Vb3tHgdrg: (31)
And its time derivative is
dHsysdt
mwdHw
dt ms
dHsdt
msq Vb3trg
dHgdt
ms
Hg DHadq
dt Vb3tHg
drgdt
: (32)
Substituting equation (32) in equation (28), and collecting
the terms containing Hg(T, P) on one side and the remaining
time derivatives on another side gives
mwdHw
dt ms
dHsdt
msq Vb3trg
dHgdt
msDHadqdt
Vb3tdPdt
_mfHg
Tf; Pf
_m Vb3t
drgdt
msdqdt
HgT; P _Ql:
(33)
From the mass balance equation (13), note that the coeffi-
cient ofHg(T, P) in the above equation is _mf. Then,
mwdHw
dt ms
dHsdt
msq Vb3trg
dHgdt
msDHadqdt
Vb3tdPdt
_mfHg
Tf; Pf
HgT; P
_Ql: 33
Note that the reference state used in computing the gas
phase enthalpy does not determine the system evolution,since the gas enthalpy appears as a difference between two
states on the right hand side of equation (34). Hence, as
expected, the energy balance and the results deriving from it
are independent of the reference state used in computing the
gas phase enthalpy.
Now, using quasi-static approximations, all the time
derivatives are expressed in terms of the time derivatives of
temperature and pressure. For the time derivatives ofrg and q
equations (18) and (23) are used. The time derivative ofHg(T, P)
is expanded as
dHgdt
vHgvT
P
dTdt
vHgvP
T
dPdt
; (35)
see for example Section 2.1 of Ahluwalia and Peng [17].
Using the thermodynamic identities
vHgvT
P
T
vSgvT
P
Cpg (36)
and
vHgvP
T
vg T
vSgvP
T
vg T
vvgvT
P
vg1 aPgT
; (37)
see Smith et al. [18], page 191 we have,
dHgdt
CPgdTdt
vg1 aPgTdPdt
: (38)
For the solid phases (pressure vessel and adsorbent),
neglecting the thermal expansion of the material, similar
equations are written as
dHwdt
CPwdTdt
vwdPdt
; (39)
and
dHsdt
CPsdTdt
vsdPdt
; (40)
Using equations (18), (23), (38)(40) in equation (34), and
rearranging the transient energy balance is in the form
a21dTdt
a22dPdt
b2; (41)
with
a21 mwCpw msCps
msq Vb3trg
CPg
msqDHa
f0T
fT
B
1 bPT2
!; (42)
a22 mwvw msvs
msqvg Vb3t
1 aPgT
msqDHa1 bPP
Vb3t; (43)
and
b2 _mfHg
Tf; Pf
HgT; P
_Ql: (44)
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Note that the dimensions of a21, a22 and b2 are energy/
temperature and energy/pressure and energy/time
respectively.
We assume that the heat leak has the form
_Ql TN T=Reff (45)
We have assumed a typical value of Reff 74.0K/W, so that
the heat leak into the tank during typical dormancy condi-
tions is about 3 W. Engineering calculations show that with
a 1-inch multi layer vacuum super insulation and good
mechanical design such values ofReffare realistic.
5.3. Solution procedures
Solving equations (24) and (41) simultaneously, gives
dTdt
b1a22 b2a12
a11a22 a21a12 f1T; P; (46)
and
dPdt
b1a21 b2a11a11a22 a21a12
f2T; P: (47)
Among the coefficients appearing in these two equations
only b1 contains _m. Suppose _m is known (as in the case of
discharge from the fuel-cell operation requirement or during
dormancy where it is zero by definition), these two coupled
first order differential equations are solved with initial condi-
tions T(t 0) T0 and P(t 0) P0, to give the temperature and
pressure evolution T(t) and P(t). For the isobaric processes of
venting, equation (47) gives the isobaric criterion as
b1a21 b2a11: (48)
Using the expression for b1 in the isobaric criterion and
rearranging gives the isobaric mass outflow as
_m _mf a11a21
b2: (49)
Equation (46) is solved with the above isobaric flow rate to
get T(t). This formulation allows an elegant implementation
of isobaric or isothermal processes, by setting f1 or f2 to zero
respectively, although for an arbitrary process neither of
them is zero. For an isobaric process, instead of deriving an
expression for the time derivative of pressure and then
setting it to zero, one could directly get an expression for _mby setting the pressure derivative to zero during the deriva-
tion. Such a procedure is mathematically identical to the
above method. We prefer the model described by equations
(46) and (47) since it gives a unified formalism for all the fuel
tank processes.
6. Dormancy
In a parked vehicle, continuous heat leak into the fuel tank
causes the hydrogen pressure to build up and gas is vented to
the fuel cell. The time period until the start of venting is called
dormancy. Let T0 and P0 respectively be the temperature and
pressure of the tank at the beginning. Let the vent pressure be
Pvent 25 bar. During dormancy, there is no flow into or out of
thetank i.e. _mf _m 0. Hence, the model equationsreduce to
b1 0, b2 _Ql. Therefore,
dTdt
_Qla12
a11a22 a21a12(50)
and
dPdt
_Qla11
a11a22 a21a12: (51)
Note that both dT/dt, and dP/dt are proportional to _Ql. The
temperature and pressure evolution equations are solved
simultaneously with the initial conditions T0, P0 and the time
taken for the tank to reach the vent pressure gives the
dormancy. Figs. 3 and 4 show that a full tank (5 kg load),
starting at T0 85.6 K and P0 20 bar (for a given pressure and
hydrogen load the corresponding equilibrium temperature
can be got from equation (9)) reaches the vent pressure in 3.5
days, and the temperature at that time is 90.4 K.
An alternate, quick but approximate, method to estimate
dormancy is as follows: The hydrogen content of the tank at
the beginning of the dormant phase is mH2 T0; P0. Let the
temperature of the tank at the end of the dormant phase be
Tvent. By definition, hydrogen is not lost from the tank during
dormancy. Hence, Tvent is computed by solving the equation
mH2 T0; P0 mH2 Tvent; Pvent: (52)
Neglecting the temperature variation ofReff, the arithmetic
average heat leak during dormancy is
C _QlD TN T0 Tvent=2=Reff: (53)
For dormancy, setting_
mf _
m 0 in the transient energybalance equation (28), and integrating over the dormant
period gives
HsysTvent; Pvent HsysT0; P0 C _QlDDtdorm Vb3tPvent P0: (54)
The appendix details the computation of Hsys(T, P). Since
Tvent is already known, this equation is solved for Dtdorm. Note
that this equation is exact with a time-averaged heat leak. But
Fig. 3 Pressure evolution during full load dormancy, with
a 1-inch multi layer vacuum super insulation. The point
marks the end of dormancy.
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 4 ( 2 0 0 9 ) 5 4 6 6 5 4 7 5 5471
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