H2 Liquefaction - Cryogenic V14 - HYSYS (Aspentech)

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Integrated Cryogenic Process in

Hydrogen Liquefaction Plants
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Contents
Abstract..................................................................................................... ii
1 Background .......................................................................................... 1
2 Process Description ................................................................................ 1
3 Model Description .................................................................................. 1
4 Simulation Results ................................................................................. 2
5 Conclusion ............................................................................................ 6
Abstract
This HYSYS example models the integrated cryogenic process in large-scale hydrogen
liquefaction plants (100 tonne/day). A novel large-scale plant for hydrogen liquefying
is proposed. In the precooling section of the process, a new mixed refrigerant (MR)
refrigeration cycle, combined with a Joule-Brayton refrigeration cycle, precool
gaseous hydrogen feed from 25 C to the temperature -182.8 C. A new refrigeration
system with six simple Linde-Hampson cascade cycles cools low-temperature
gaseous hydrogen from -182.8 C to temperature -253.0 C. Ortho-para hydrogen
conversion is modeled with Chemistry.
It can be used as a starting point for more complex models for process design and
optimization, debottlenecking, and plant and equipment design.
ii
1 Background
In Paris, December 2015, the Paris Agreement among 195 nations was fulfilled with
commitment of reaching the two degrees global warming target and reduce the global
greenhouse emissions per capita with 8% in 2025 and 9% by 2030. The growth of
demand forecast for a green and clean energy carrier, points in direction of hydrogen,
as an energy commodity for decarbonization of the next-generation transport sector,
as well as to the power generation industry.
Hydrogen from a gravimetric point of view, conceals large amounts of energy. To

store and transport the extensive energy amount, hydrogen gas density must be
increased significantly to compete with other energy storage alternatives, such as
state-of-the-art batteries. The two methods of high-density storage of hydrogen are
by liquefaction or compression.
2 Process Description
The integrated cryogenic process is an overall process for hydrogen liquefaction
plants. The process flow diagram indicated in Figure 1 shows it includes three
sections: pre-cooling, cryogenic, and liquefaction. Two combined MR refrigeration
systems pre-cool feed hydrogen (stream H1) to -182.8 C (stream H5) in pre-cooling
section. Six Joule-Brayton cascade systems cool the pre-cooled feed equilibrium
hydrogen gas from -182.8 C to -238.4 C (stream H8) in cryogenic section. In the
end, system depressurized the deep cooled hydrogen at a temperature -253.0 C
passing the valve from 21 bar to 1.01325 bar.
This HYSYS example models the integrated cryogenic process in large-scale hydrogen
liquefaction plants (100 tonne/day). It can be used as a starting point for more
complex models.
The model includes the following key features:
 Main MR refrigeration system
 Auxiliary MR refrigeration system
 Six Joule-Brayton cascade systems
 LNG heat exchangers model precooling/cryogenic
 Ortho-para hydrogen conversion
3 Model Description
The integrated cryogenic process in hydrogen liquefaction plants is modeled using
HYSYS as shown in Figure 1.
In this simulation, Hydrogen Package fluid package is adopted for the overall process
modeling. The main large-scale hydrogen liquefaction process configuration includes
four independent stages:
 Isobaric pre-cooling (ambient to about 90 K)
1
 Isobaric cryogenic cooling (about 90 K-35 K)
 Depressuring to 1atm (21 bar to 1 atm)
Figure 1: Integrated Cryogenic process in hydrogen liquefaction plants in HYSYS
As shown in Figure 1, the plant includes three main sections: pre-cooling, cryogenic,
and depressurization. Two combined MR refrigeration systems pre-cool feed
hydrogen (stream H1) to -182.8 C (stream H5) in pre-cooling section. The main MR
system has a common heat exchanger (HX3) with auxiliary MR system. The main MR
system pre-cools feed hydrogen to -107.3 C (stream H4), and continuing, auxiliary
MR system makes it cooler to -182.8 C. In cryogenic section, six Joule-Brayton
cascade systems cool the pre-cooled feed equilibrium hydrogen gas from -182.8 C to
-238.4 C (stream H8). In the end, system depressurized the deep cooled hydrogen
at a temperature -253.0 C passing the valve from 21 bar to 1.01325 bar. The final
output is 99.86% para-hydrogen at -253.0 C and 1.01325 bar condition (stream H9),
that is enough to be kept for use.
4 Simulation Results
The chemistry parameter settings are shown in the following Table 1. The design and
assumption data of the plant are given in Table 2. The para-hydrogen composition
change between temperature 20-300 K is shown in Table 3. The MR composition and
stream results of the pre-cooling section are shown in Table 4 and 5. The refrigerant
composition of JB cycles streams and stream results of the cryogenic section are
shown in Table 6 and 7. The para-hydrogen concentration of H2 streams, from feed
to the product is shown in Table 8.
2
Table 1: Chemistry parameter settings
Reaction Type Stoichiometry

1 Equilibrium H2-PARA <--> H2-ORTHO
2 Dissociation H2 --> H2-PARA
Equilibrium Constants
ln(Keq)=A+B/T+C*ln(T)+D*T
A 5.18192049
B -195
C -0.61661082
D 0.000318
Keq Basis Mole fraction
Table 2: Design and assumption data of the plant
Parameter Condition(s)
Ambient temperature 25 C
Feed 25 C and 21 bar, pure hydrogen
Product 1.01325 bar, 99.86% saturated para liquid
hydrogen
Product flows rate 1.157 kg/s (100 tonne/day)
Pressure drop 0
Isentropic efficiency:
Compressors 80%
Expanders 80%
Equation of state Hydrogen Package
Table 3: Para-hydrogen composition between temperature 20-300 K
H2 Temp [K] Para-H2 H2 Temp [K] Para-H2 H2 Temp [K] Para-H2

10 - 110 0.3668 210 0.2644
20 0.9984 120 0.3446 220 0.2612
30 0.9679 130 0.3270 230 0.2584
40 0.8760 140 0.3129 240 0.2561
50 0.7529 150 0.3015 250 0.2541
60 0.6396 160 0.2922 260 0.2524
70 0.5501 170 0.2845 270 0.2510
80 0.4830 180 0.2781 280 0.2497
90 0.4331 190 0.2728 290 0.2487
100 0.3955 200 0.2682 300 0.2478
3
Table 4: MR composition of the pre-cooling section of the plant
Components Composition by mole (%)

M7 stream A1 stream
Hydrogen 0.0000 1.0000
p-Hydrogen 0.0000 0.0000
Nitrogen 0.1218 0.0000
Methane 0.1917 0.0000
n-Butane 0.0219 0.0000
n-Pentane 0.1778 0.0000
Propene 0.1189 0.0000
Ethane 0.1916 0.0000
Refrig-14 0.0892 0.0000
i-Butane 0.0227 0.0000
Propane 0.0497 0.0000
Helium 0.0000 0.0000
Neon 0.0000 0.0000
Ammonia 0.0148 0.0000
Table 5: Stream results of the pre-cooling section
Temperature Pressure Mass flow Temperature Pressure Mass flow

Stream Stream
(T [K]) (P [Bar]) (m [kg/s]) (T [K]) (P [Bar]) (m [kg/s])
H1 298.15 21.00 1.157 M15 166.35 13.93 9.528
H2 227.48 21.00 1.157 M16 165.52 2.04 9.528
H3 165.40 21.00 1.157 M17 166.15 13.93 14.182
H4 165.85 21.00 1.157 M18 84.65 13.93 14.182
H5 90.36 21.00 1.157 M19 85.28 2.04 14.182
M1 279.30 2.04 2.773 M19a 85.28 2.04 0.000
M1a 279.30 2.04 34.347 M19b 85.28 2.04 14.182
M1b 279.97 13.93 2.773 M14 233.15 13.93 9.528
M2 337.24 5.92 34.347 M15 166.35 13.93 9.528
M3 296.15 5.92 34.347 M16 165.52 2.04 9.528
M4 296.15 5.92 4.096 M17 166.15 13.93 14.182
M4a 296.15 5.92 30.251 M18 84.65 13.93 14.182
M4b 296.66 13.93 4.096 M19 85.28 2.04 14.182
M5 345.26 13.93 30.251 M19a 85.28 2.04 0.000
M6 325.62 13.93 37.120 M19b 85.28 2.04 14.182
M7 298.15 13.93 37.120 A1 296.85 0.46 1.450
M8 298.15 13.93 13.410 A2 340.18 0.67 1.450
M9 298.15 13.93 23.710 A3 295.15 0.67 1.450
M10 225.14 13.93 13.410 A4 335.78 0.96 1.450
M11 223.17 2.04 13.410 A5 298.15 0.96 1.450
M12 233.15 13.93 23.710 A6 86.55 0.96 1.450
M13 233.15 13.93 14.182 A7 72.92 0.46 1.450
M14 233.15 13.93 9.528 A8 85.48 0.46 1.450
4
Table 6: Refrigerant composition of JB cycles streams of the cryogenic section
Components Composition by mole (%)

Ja1 Jb1 Jc1 Jd1 Je1 Jf1
Hydrogen 0.000 0.472 0.472 0.360 0.472 1.000
Helium 1.000 0.528 0.528 0.640 0.528 0.000
Table 7: Stream results of the cryogenic section
Temperature Pressure Mass flow Temperature Pressure Mass flow

Stream Stream
(T [K]) (P [Bar]) (m [kg/s]) (T [K]) (P [Bar]) (m [kg/s])
H5 90.36 21.00 1.157 Jc7 47.29 2.15 1.256
H6 53.85 21.00 1.157 Jc8 89.63 2.15 1.256
H7 44.11 21.00 1.157 Jd1 297.15 0.71 3.803
H8 34.79 21.00 1.157 Jd2 426.99 1.68 3.803
Ja1 297.15 14.00 2.660 Jd3 295.15 1.68 3.803
Ja2 358.28 20.49 2.660 Jd4 424.07 3.95 3.803
Ja3 295.15 20.49 2.660 Jd5 298.15 3.95 3.803
Ja4 355.95 30.00 2.660 Jd6 51.35 3.95 3.803
Ja5 298.15 30.00 2.660 Jd7 34.29 0.71 3.803
Ja6 50.00 30.00 2.660 Jd8 34.93 0.71 3.803
Ja7 56.18 14.00 2.660 Je1 297.15 0.70 2.888
Ja8 63.45 14.00 2.660 Je2 394.27 1.40 2.888
Jb1 297.15 4.99 1.948 Je3 295.15 1.40 2.888
Jb2 338.92 6.85 1.948 Je4 391.75 2.79 2.888
Jb3 295.15 6.85 1.948 Je5 298.15 2.79 2.888
Jb4 336.39 9.38 1.948 Je6 39.15 2.79 2.888
Jb5 298.15 9.38 1.948 Je7 27.88 0.70 2.888
Jb6 78.15 9.38 1.948 Je8 37.65 0.70 2.888
Jb7 66.86 4.99 1.948 Jf1 297.15 0.50 3.400
Jb8 76.65 4.99 1.948 Jf2 412.03 1.29 3.400
Jc1 297.15 2.15 1.256 Jf3 295.15 1.29 3.400
Jc2 418.85 5.00 1.256 Jf4 409.40 3.31 3.400
Jc3 295.15 5.00 1.256 Jf5 298.15 3.31 3.400
Jc4 416.10 11.61 1.256 Jf6 33.05 3.31 3.400
Jc5 298.15 11.61 1.256 Jf7 20.43 0.50 3.400
Jc6 69.05 11.61 1.256 Jf8 31.05 0.50 3.400
5
Table 8: Para-hydrogen concentration of H2 streams
Stream Para (%) Stream Para (%)

H1 24.80 H6 70.68
H2 25.91 H7 82.63
H3 28.79 H8 99.09
H4 28.75 H9 99.86
H5 43.16
5 Conclusion
An innovative large-scale conceptual plant for producing 100 tonne/day of liquid
hydrogen is proposed and investigated. A complex multi-component refrigerant with
10 components is introduced for the new combined mixed refrigerant refrigeration
system in the pre-cooling section of the plant. It consisted of 13.81% nitrogen,
21.69% methane, 1.94% n-butane, 9.47% n-pentane, 12.69% propene, 21.33%
ethane, 10.08% refrig-14, 2.15% i-butane, 5.25% propane, and 1.60% ammonia.
The product liquid hydrogen of pre-cooling section is cooled from feed hydrogen in
25 C and 21 Bar to -182.8 C. Six cascade combined Joule-Brayton cycles with
different mixed refrigerants, deep cooled pre-cooled hydrogen to -238.4 C
temperature. Finally, feed hydrogen passed EX-L at a temperature -253.0 C.
6
References
[1] M Asadnia, M Mehrpooya. A novel hydrogen liquefaction process configuration
with combined mixed refrigerant systems. International Journal of Hydrogen
Energy, May 2017

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j

Integrated Cryogenic Process in

Hydrogen from a gravimetric point of view, conceals large amounts of energy. To

The model includes the following key features:

 Main MR refrigeration system

 Auxiliary MR refrigeration system

 Six Joule-Brayton cascade systems

 LNG heat exchangers model precooling/cryogenic

 Ortho-para hydrogen conversion

Figure 1: Integrated Cryogenic process in hydrogen liquefaction plants in HYSYS

Reaction Type Stoichiometry

Table 2: Design and assumption data of the plant

Table 3: Para-hydrogen composition between temperature 20-300 K

H2 Temp [K] Para-H2 H2 Temp [K] Para-H2 H2 Temp [K] Para-H2

Components Composition by mole (%)

Table 5: Stream results of the pre-cooling section

Temperature Pressure Mass flow Temperature Pressure Mass flow

Components Composition by mole (%)

Table 7: Stream results of the cryogenic section

Temperature Pressure Mass flow Temperature Pressure Mass flow

Stream Para (%) Stream Para (%)

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