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 4 1 ( 2 0 1 6 ) 1 6 3 1 6 e1 6 3 2 1

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journal homepage: www.elsevier.com/locate/he

Determining hydrogen pre-cooling temperature

from refueling parameters

Jinsheng Xiao a,b,*, Xu Wang a, Pierre B
enard b, Richard Chahine b

a
Hubei Key Laboratory of Advanced Technology for Automotive Components and Hubei Collaborative Innovation
Center for Automotive Component Technology, School of Automotive Engineering, Wuhan University of Technology,
Hubei 430070, China
b
Hydrogen Research Institute, Universit
e du Qu
ebec a
 Trois-Rivieres, QC G9A 5H7, Canada

article info abstract

Article history: Compressed hydrogen storage has a requirement on the temperature: for safety reasons,
Received 24 January 2016 the final gas temperature is not allowed to exceed 85
C during filling. However, due to the
Received in revised form short time and the fast filling rate in practice, the final gas temperature rises sharply. To
4 June 2016 solve the issue, the hydrogen could be pre-cooled sometimes, but setting the pre-cooling
Accepted 8 June 2016 hydrogen temperature becomes a critical problem, we need to know whether the inflow
Available online 30 June 2016 hydrogen needs to be pre-cooled and what the pre-cooling temperature it should be. This
paper proposes a new analytical solution of pre-cooling hydrogen temperature from a
Keywords: simplified lumped parameter model. The effects of initial temperature, initial pressure and
Hydrogen storage the filling time on the inflow hydrogen temperature are studied, and three sets of equations
Refueling are proposed correspondingly. Further we use these equations to fit the published refer-
Fast filling ence data, the fittings show good agreement. The occasions where the hydrogen needs to
Pre-cooling be pre-cooled are presented. We suppose this study not only helps to choose the pre-
Temperature cooling hydrogen temperature, but also ensure the safety during the hydrogen filling.
Safety © 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.

would become brittle [2]. As a result of the materials' prop-

Introduction erty, the compressed hydrogen storage has a requirement on
the temperature: the final gas temperature is not allowed to
Hydrogen is acknowledged to be an alternative and a poten- exceed 85
C during refueling [3].
tial fuel in the future, and compressed hydrogen gas is widely To ensure the safety during the refueling, many re-
used in fuel cell vehicles [1]. In practice, due to the short filling searches have been done. Experiments were conducted by
time and the fast filling rate, the final gas temperature rises Liu, aiming to make clear the thermal behaviors of hydrogen
rather quickly. But the carbon fiber reinforced plastic com- storage [4]. A thermodynamic analysis was presented for a
posite (CFRP) materials used in the system are sensitive to the compressed gaseous hydrogen system [5]. Dicken et al.
temperature, when the temperature is too high, the materials studied the influences of the total fill time and the initial mass

* Corresponding author. Hydrogen Research Institute, Universite
du Que
bec a

 Trois-Rivieres, QC G9A 5H7, Canada. Tel.: þ1 819 376
5011x4478; fax: þ1 819 376 5164.

nard), Richard.Chahine@
E-mail addresses: Jinsheng.Xiao@uqtr.ca (J. Xiao), 357740742@qq.com (X. Wang), Pierre.Benard@uqtr.ca (P. Be
uqtr.ca (R. Chahine).
http://dx.doi.org/10.1016/j.ijhydene.2016.06.084
0360-3199/© 2016 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
 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 4 1 ( 2 0 1 6 ) 1 6 3 1 6 e1 6 3 2 1 16317

coefficients and the filling time can be also known by the use
Nomenclature of another fitted formula with 48 coefficients.
We developed the numerical solutions for the lumped
af heat transfer coefficient between hydrogen and
parameter thermodynamic models of adsorptive and cryo-
ambient fluid, W/m2/K
adsorptive hydrogen storage systems [12,13]. Based on the
As internal surface area of tank, m2
lumped parameter thermodynamic models, analytical solu-
cp constant-pressure specific heat, J/kg/K
tions are developed for chargeedischarge cycle of compres-
cv constant-volume specific heat, J/kg/K
sion hydrogen storage system [14] and adsorptionedesorption
h specific enthalpy of hydrogen, J/kg
cycle of adsorptive hydrogen storage system [15]. The simple
hin specific enthalpy of inflow H2, J/kg
uniform formula is inspired by the concept of the rule of
hout specific enthalpy of outflow H2, J/kg
mixture and its weighted factors are obtained from the
kp0 kp0 ¼ T=ðT0 pf Þ
analytical solution of lumped parameter thermodynamics
kp0f kp0f ¼ T=T0
model. The analytical solution of the hydrogen temperature in
kpf kpf ¼ Tp0 =T0
the tank is used to fit the experimental temperatures [16,17].
m mass of hydrogen mass in tank, kg
Estimation of final hydrogen temperature from refueling pa-
m0 initial hydrogen mass, kg
rameters based on the rule of mixtures is simple and practical
m_ mass flow rate, kg/s
for controlling the maximum temperature and for ensuring
m_ in hydrogen mass inflow rate, kg/s
hydrogen safety during fast filling process.
m_ out hydrogen mass outflow rate, kg/s
The SAE J2601 establishes the protocol and process limits
p0 initial pressure, MPa
for hydrogen fueling of light duty vehicles, it has been devel-
p0f p0f ¼ p0 =pf
oped to meet the performance objectives under all practical
pf final pressure, MPa
conditions based on a look-up table approach [18,19] and MC
Q_ heat inflow rate, Q_ ¼ af As ðTf  TÞ, W
Method [20,21]. The useful hydrogen fueling test data is
t time variable or fill time, s
_ s available at http://www.h2protocol.com/h2-fueling-data/ [22].
t* characteristic time, t* ¼ m0 =m,
These data would be used for further estimation of final
T temperature of hydrogen, K
hydrogen temperature or determination of pre-cooled
T* characteristic temperature, K
hydrogen temperature.
T0 initial temperature in tank, K
In the research of the development of hydrogen storage
Tf temperature of ambient fluid, K
system, in order to meet the requirement of the highest
T∞ inflow or outflow temperature, K
temperature limit (e.g. 85
C), cooling the hydrogen in
u specific internal energy, J/kg
advance has been proved to be an applicable way. However,
Greek symbols setting the pre-cooling hydrogen temperature has become a
a dimensionless heat transfer coefficient, critical problem, which should not only ensure the final
a ¼ af As =cv m_ temperature of hydrogen not to exceed the corresponding
g ratio of specific heats, g ¼ cp/cv limits, but also avoid making the pre-cooling temperature too
m fraction of initial mass, m ¼ m0/m low to waste energy. In this article, we fix the final tempera-
m0 m0 ¼ m1þa ture as the highest temperature limit (e.g. 85
C), express the
t dimensionless time, t ¼ t=t* pre-cooling temperature T∞ as the function of refueling pa-
rameters including initial temperature T0, initial pressure p0
and filling time t under different final pressures. For the three
cases, the deduced equations are used to fit the reference
on the temperature distribution and the temperature rise, data. The fittings show good agreement. Furthermore, the
and a three-parameter formula was proposed [6]. An experi- fitting result can be used for deciding whether the inflow
ment was carried out to investigate the discharge cycle of a hydrogen needs pre-cooling or not and how could it should
type III cylinder and a model was also presented [7]. The ef- be.
fect of mass flow rates and inlet gas temperatures on the end
state of charge was measured by Cebolla et al., then a
conclusion was drawn that the inlet gas temperature played Model for determining hydrogen pre-cooling
an important role on the final state of charge [8]. temperature
Monde et al. [9] took two different ways to deal with the
hydrogen gas and the tank wall, a lumped parameter model General mass and energy balance equations for charge/
was used to describe the thermal behaviors of hydrogen gas in discharge processes of high pressure hydrogen gas into/from a
the tank and a one-dimensional model was used for tank wall. tank are mostly written as [14].
Their simulation results were proved to agree with the gas
temperature profile obtained by BMW-Powertech tests [10]. dm
¼ m_ in  m_ out (1)
Monde et al. derived approximate equations to predict the dt
temperature of the pre-cooled hydrogen and the filling
d
time for a practical vessel [11], the pre-cooled hydrogen tem- ðmuÞ ¼ m_ in hin  m_ out hout þ Q_ (2)
dt
perature can be predicted by using a fitted formula with 36
16318 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 4 1 ( 2 0 1 6 ) 1 6 3 1 6 e1 6 3 2 1

Let us define m_ ¼ m_ in and mh

_ ¼ m_ in hin for charge process,
_ ¼ m_ out hout for discharge process. The
m_ ¼ m_ out and mh Determining hydrogen pre-cooling temperature
above equations can be written as from different refueling parameters

dm Determining from initial temperature and final pressure

¼ m_ (3)
dt
From the reference [11], the curves of inflow temperature T∞
d vs initial temperature T0 under each final pressure present
_ þ Q_
ðmuÞ ¼ mh (4)
dt linear trend, so we can fit these data as linear functions:

_ the solution of
Under constant charge or discharge rate m, T∞ ¼ a  bT0 (12)
_ Thus
mass balance equation (3) is simplified as m ¼ m0 þ mt.
Comparing Eq. (12) with Eq. (11), we have
the energy balance equation becomes
1 1þa a m0 1 þ a
du
 a¼ T  Tf ; b ¼ (13)
_
ðm0 þ mtÞ _ ¼ mh
þ mu _ þ a f As T f  T (5) 1m g
0 g 1  m0 g
dt
This formula is used to fit the reference data [11], as shown
For the case of constant inflow or outflow hydrogen tem- in Fig. 1. The values of fitted parameters of a and b for four final
perature T∞, the energy equation (5) can be written in the form pressures are shown in Table 1. For simplification, we can
of temperature: assume m0 zm for most cases. The known constants according
to the reference [11] are T ¼ 358.15 K, Tf ¼ 293.15 K. So, there
dT T*  T
¼ ð1 þ aÞ * (6) are three unknown parameters in the Eq. (13). We must fix one
dt t þt
of the three parameters in Eq. (13) and then we solve other two
where T* ¼ ðgT∞ þ aTf Þ=ð1 þ aÞ is a characteristic temperature, parameters by using two equations in Eq. (13). Table 2 gives
t* ¼ m0 =m_ is characteristic time, and a ¼ ðaf As Þ=ðcv mÞ
_ is a out the values of parameters m and g when a ¼ 0 and a ¼ 1.
dimensionless heat transfer coefficient which represents the Through the equations, whether the hydrogen need pre-
ratio of heat transfer ability afAs to heat capacity change cv m_ cooling or not could be determined if the real initial temper-
(W/K) of the system during charge and discharge processes. ature, finial pressure and ambient temperature are known. For
Using dimensionless time t ¼ t=t* , solution of Eq. (6) can be example, as shown in Fig. 1, assuming that the ambient
obtained as [14]. temperature is 300 K, when the finial pressure in the tank
reaches 50 MPa, a critical initial temperature T0 can be found
 1þa
T*  T 1 by ensuring the highest hydrogen temperature is 85
C. If the
¼ (7)
T*  T0 1þt real initial temperature T00 is higher than T0, the required
inflow temperature T∞ will be lower than the ambient tem-
Then, the solution can be expressed in the form of “rule of
perature (i.e. the source temperature), so the hydrogen needs
mixtures” [17]:
to be pre-cooled. On the opposite side, the hydrogen doesn't
T ¼ m0 T0 þ ð1  m0 ÞT* (8) need pretreatment.
According to the definition of m (m ¼ m0/m), the value of it is
where m0 ¼ m1þa ¼ ðm0 =mÞ1þa is the weighted factor. Inserting supposed to be less than one and more than zero, and the
the characteristic temperature T* ¼ ðgT∞ þ aTf Þ=ð1 þ aÞ into higher the final pressure, the less the value of it. The
Eq. (5), we obtain

T ¼ m0 T0 þ g0 T∞ þ a0 Tf (9) 320

310 pf=35MPa
where g0 ¼ gð1  m0 Þ=ð1 þ aÞ, a0 ¼ að1  m0 Þ=ð1 þ aÞ. So we can
express the hydrogen pre-cooling temperature as 300
50MPa
Inflow temperature (K)

1
 290
T∞ ¼ 0 T  a0 Tf  m0 T0 (10)
g 70MPa
280
i.e. 87.5MPa
270

260
1 1þa a m0 1 þ a
T∞ ¼ T  Tf  T0 (11) 250
1  m0 g g 1  m0 g

This means the hydrogen pre-cooling temperature can be 240

T0 T0'
determined by refueling parameters, such as final hydrogen 230
temperature T, ambient temperature Tf, initial temperature 250 260 270 280 290 300 310 320
T0, and other parameters m, a, and g, which are related to Initial temperature (K)
initial mass or initial pressure, final mass or final pressure,
mass flow rate, average pressure ramp rate or filling time, heat Fig. 1 e Effect of initial temperature on inflow temperature
transfer coefficient and tank structure. under different final pressures (Symbol: Data [11], Line:
Fitting).
 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 4 1 ( 2 0 1 6 ) 1 6 3 1 6 e1 6 3 2 1 16319

Table 1 e Fitted parameters (a, b) of the functions for 310 pf=35MPa

inflow temperature with initial temperature under
different final pressures. 300
50MPa
Final pressure Parameter Value Standard error 290

Inflow temperature (K)

pf (MPa)
280
35 a 871.18592 4.71569 70MPa
b 1.83822 0.01504 270
50 a 675.51797 2.47640
b 1.30209 0.00826 260
87.5MPa
70 a 560.32866 3.21561
b 0.98361 0.01125 250
87.5 a 492.92798 1.58431
240
b 0.82292 0.00560
p0 p0'
230
0 2 4 6 8 10 12 14 16 18 20
Initial pressure (MPa)
Table 2 e Fitted parameters (m, g) of the functions for
inflow temperature with initial temperature under Fig. 2 e Effect of initial pressure on inflow temperature
different final pressures.
under different final pressures (Symbol: Data [11], Line:
Final pressure Parameter Value when Value when Fitting).
pf (MPa) a¼0 a¼1
35 m 0.75570 0.64632
g 1.68281 1.98822 Table 3 e Fitted parameters of the functions for inflow
50 m 0.69035 0.56841 temperature with initial pressure under different final
g 1.71221 2.02295 pressures.
70 m 0.62870 0.50007
g 1.72147 2.03389 Final pressure Parameter Value Standard error
87.5 m 0.59792 0.46765 pf (MPa)
g 1.80702 2.13498 35 a 1.55886 0.53731
kp0f 1.25105 0.11919
g 1.66221 0.12868
monotonicity of m is good in Table 2. The g can be obtained 50 a 0.97218 0.07034
with two different ways. One uses the equation of state for kp0f 1.41422 0.02122
g 1.61013 0.01808
ideal gas, and the other uses the equation of state for real gas.
70 a 1.36409 0.13875
It turns out there exists deviation between them, whose value kp0f 1.35755 0.03225
fluctuates within a range of twenty percent. So we support g 1.78424 0.03709
that the values of g are reasonable in Table 2. 87.5 a 1.03855 0.21035
kp0f 1.48110 0.07122
g 1.80489 0.05928
Determining from initial pressure and final pressure

In the case of reference data [11], Tf ¼ T0, so Eq. (10) or Eq. (11) than the source temperature, so there is no need for us to pre-
can be simplified as cool the hydrogen. Otherwise, if the real initial pressure is
  lower than the critical initial pressure, the inflow hydrogen
1þa 1 m0 þ a needs to be pre-cooled.
T∞ ¼ T  T0 (14)
1  m0 g 1þa

According to the equation of state for ideal gas, for initial Determining from filling time and final pressure
state and end state, we have p0V ¼ n0RT0 and pfV ¼ nRT, then
we can obtain p0/pf ¼ n0T0/(nT). We define m ¼ m0/m ¼ n0/n, so As in Section Determining from initial pressure and final
we get m ¼ Tp0/(T0pf). We can further have m ¼ kp0 p0 , where pressure, we have m0 zm ¼ Tp0 =ðT0 pf Þ, we assume m ¼ kpf/pf,
kp0 ¼ T=ðT0 pf Þ, or m ¼ kp0f p0f , where kp0f ¼ T=T0 and p0f ¼ p0 =pf . where kpf ¼ Tp0/T0 ¼ 12.21. For the case of reference data [11],
For simplification, we also use m0 zm in Eq. (14). T ¼ 358.15 K, T0 ¼ 293.15 K, p0 ¼ 10 MPa, so kpf ¼ Tp0/T0 ¼ 12.21.
We use T ¼ 358.15 K, T0 ¼ 293.15 K to fit the data which We also assume the dimensionless heat transfer coefficient as
comes from the reference [11]. Fig. 2 shows good agreement. a ¼ ktt. Then Eq. (14) becomes:
The values of the corresponding fitting parameters are shown
in Table 3. In Fig. 2, the horizontal line represents the envi- . !
ronment temperature is 300 K. In order to achieve a certain 1 þ kt t 1 kpf pf þ kt t
T∞ ¼ . T T0 (15)
final pressure (for example, 35 MPa), a critical initial pressure 1  kpf pf g 1 þ kt t
p0 can also be obtained. According to the curve of 35 MPa,
when the real initial pressure p00 is higher than the critical Rearranging Eq. (15) gives the inflow temperature as a
initial pressure p0, the required inflow temperature is higher linear function of time:
16320 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 4 1 ( 2 0 1 6 ) 1 6 3 1 6 e1 6 3 2 1

applied to deduce the correlation between the inflow

310
temperature and the refueling parameters.
pf=35MPa
300 (2) The hydrogen pre-cooling temperature can be determined
directly by refueling parameters, such as final hydrogen
290
Inflow temperature (K)

50MPa temperature, ambient temperature, initial temperature,

280 and other parameters which are related to initial mass
or initial pressure, final mass or final pressure, mass
270 70MPa flow rate, average pressure ramp rate or filling time,
260
heat transfer coefficient and tank structure.
(3) The fitted formulas have simpler form, less parameters and
250
87.5MPa
more physical meanings. The formulas are used to fit
published reference data. These results show the effects
240
of initial temperature, initial pressure and filling time
t' t
230 on the inflow temperature respectively. The fittings
0 50 100 150 200 250 300 agree very well with the original data.
Filling time (s) (4) This work helps choosing the pre-cooling hydrogen temper-
ature and ensuring the safety during the filling. To ensure
Fig. 3 e Effect of filling time on inflow temperature under
that the final hydrogen temperature do not exceed
different final pressures (Symbol: Data [11], Line: Fitting).
85
C, the hydrogen needs to be pre-cooled in the oc-
casions of the real initial temperature being higher
than the critical initial temperature, the real initial
Table 4 e Fitted parameters of the functions for inflow
pressure being lower than the critical initial pressure
temperature with filling time under different final
pressures. and the real filling time being less than the critical
filling time.
Final pressure Parameter Value Standard error
(5) The formula used for fitting the reference data is based
pf (MPa)
on ideal gas assumption and single-zone (hydrogen gas)
35 kt 0.12300 0.00150
lumped parameter model. The real gas modification
g 1.66229 0.00413
50 kt 0.08112 0.00128
and dual-zone (hydrogen gas and tank wall) lumped
g 1.61835 0.00472 parameter model will be considered for widely repre-
70 kt 0.06626 9.4186E4 sentation of the reference (experimental or simulated)
g 1.63593 0.00345 data.
87.5 kt 0.06005 8.11192E4
g 1.71429 0.00313

.
kt ðT  T0 Þ T  T0 kpf pf
T∞ ¼  . t þ  .  (16) Acknowledgments
g 1  kpf pf g 1  kpf pf
We wish to thank the National Natural Science Foundation of
However, the data given in Fig. 3 show nonlinear behavior. China (NSFC Project No.51476120) and the Natural Sciences
So this formula has to be modified to well fit the reference and Engineering Research Council of Canada (NSERC) for their
data. Given that the reference data increase lower than the financial supports and Mr. Benjamin Angers for his technical
linear model, a fractal exponent on the time t is used for ex- assistance on the OriginPro 2015 software.
press the dimensionless heat transfer coefficient a ¼ kt t1=2 . For
the reference data [11], the fitted parameters are shown in
Table 4, and the fitted results are shown in Fig. 3. As it’s
shown, the fittings agree very well. references
In Fig. 3, the horizontal line represents the environment
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