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Progress in Chemistry 2021, Vol. 33 Issue (12): 2215-2244 DOI: 10.7536/PC201128 Previous Articles   Next Articles

• Review •

Current Status of Hydrogen Production in China

Junwen Cao, Wenqiang Zhang, Yifeng Li, Chenhuan Zhao, Yun Zheng, Bo Yu()   

  1. Institute of Nuclear and New Energy Technology, Tsinghua University, Beijing 100084, China
  • Received: Revised: Online: Published:
  • Contact: Bo Yu
  • Supported by:
    the National Natural Science Foundation of China(91645126); the National Natural Science Foundation of China(21273128); the Tsinghua University Initiative Scientific Research Program(2018Z05JZY010); the Tsinghua-MIT-Cambridge Low Carbon Energy University Alliance Seed Fund Program(201LC004)
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Hydrogen energy is an efficient and clean secondary energy that plays an irreplaceable role in realizing "carbon neutral". With the continuous expansion of hydrogen production scale and the reduction in hydrogen production cost, hydrogen energy will become a competitive alternative energy, which can further promote the transformation of China’s energy structure, reduce carbon emissions, and improve China’s energy security and resilience. China is the world’s largest producer of hydrogen, and there are three main industrial hydrogen production routes in China: fossil fuel reforming, industrial by-product hydrogen and the electrolysis of water. Other new hydrogen production technologies, such as hydrogen production from solar photolysis, hydrogen production from biomass, hydrogen production from thermochemical circulation, etc., have attracted extensive attention and investigations. In addition, hydrogen production system is complex, which is difficult for modeling and optimization. Accordingly, artificial intelligence (AI) shows unique advantages in the prediction, evaluation and optimization for hydrogen production system, which is promising and attractive. Based on the recent progress, this article summarizes several critical hydrogen production technologies into four main categories, and further proposes some perspectives for the future development of hydrogen supply structure in China. Finally, this article also reviewes the latest application of artificial intelligence in hydrogen production system to provide new insights for the development of hydrogen production technology in China.

Contents

1 Introduction

2 Hydrogen production from conventional fossil fuel reforming

2.1 Hydrogen production from coal

2.2 Hydrogen production from natural gas

3 Industrial by-product hydrogen

3.1 Pressure swing adsorption

3.2 Low temperature separation

3.3 Membrane separation

3.4 Metal hydride separation

4 Hydrogen production from water electrolysis of clean energy

4.1 AEC

4.2 PEMEC

4.3 SOEC

5 Hydrogen production from other new technologies

5.1 Hydrogen production from solar photolysis of water

5.2 Hydrogen production from biomass fermentation

5.3 Hydrogen production from thermochemical conversion of biomass

5.4 Hydrogen production from thermochemical cycle

6 Comparison of different hydrogen production methods

7 Application of artificial intelligence in hydrogen production system

8 Conclusion and outlook

Key words: hydrogen production, fossil fuel reforming, industrial by-product hydrogen, electrolysis of water, hydrogen production from other new technologies, artificial intelligence
Fig.1 Comparison of hydrogen energy industry chain at home and abroad
Table 1 The main recation of coal gasification to produce hydrogen
Reaction type Reaction equation Reaction heat ΔH 298 K,
kJ·kg-1·mol-1		 equilibrium constant
800 ℃ 1300 ℃
heterogeneous reaction
combustion C+O2=CO2 -406 430 1.8×1017 1.5×1013
partial combustion 2C+O2=CO -246 372 1.4×1017 4.56×1015
Carbon reacts with water vapor C+H2O=CO+H2 +118 577 0.807 1.01×102
Boudouard reaction C+CO2=2CO +160 896 0.775 3.04×102
hydrogenation reaction C+2H2=CH4 -83 800 0.466 1.08×10-2
homogeneous reaction
Hydrogen combustion reaction 2H2+O2=2H2O -482 185 2.2×1017 4.4×1011
CO combustion reaction 2CO+O2=2CO2 -567 326 2.4×1015 4.9×1010
water-gas reaction CO+H2O=CO2+H2 -42 361 1.04 0.333
Methanation reaction CO +3H2=CH4+H2O -206 664 0.577 1.77×10-4
Fig.2 The process of coal gasification to produce hydrogen[15]
Table 2 Basic information of four common gasifiers
Shell gasifier[21] GSP gasifier[22] Texaco gasifier[25] Tsinghua gasifier[24]
Gasification form Dry powder gasification Dry powder gasification Coal water slurry gasification Coal water slurry gasification
Gasification conditions High temperature and pressure High temperature and
pressure		 High temperature and pressure High temperature and pressure
Advantages High suitability of coal;
High gas production efficiency;
Small oxygen production equipment;
High power generation efficiency;
Good environmental performance		 Long life;
Less investment in syngas reprocessing;
Low investment;
Gases are suitable for the manufacture of synthetic ammonia		 Low methane content;
High suitability of coal;
Small operation risk;
All sewage can be used to make coal water slurry;
Simple structure, low operating cost;
Simple ash removal
system		 High safety of ignition system;
Obvious investment advantages; Wide adaptability of coal ;High gasification efficiency; Low operating cost; Water saving, environmentally friendly
Disadvantages Large investment in equipment;
Complex structure of gasifier and waste boiler		 Low single furnace
production capacity;
The long-term operation effect is poor		 High oxygen consumption;
Narrow adaptability of raw
materials;
Refractory material has short life		 -
Table 3 Comparison of main characteristics of several typical hydrogen production reactors from natural gas[37]
Fixed bed Fluidized bed Membrane reactor Plasma reactor Solar reactor Microchannel reactor
Reactor structure Relatively simple Simple Complicated Complicated Very complicated Very complicated
Operation difficulty Simple Relatively simple Complicated Simple Very complicated Very complicated
Advantage Easy operation;
Low processing
cost		 Uniform distribution of temperature and concentration Catalytic reaction and separation coupling;
High conversion rate;
High purity hydrogen		 Strong adaptability of raw materials;
good processing
flexibility		 Pollution-free Large specific surface
area, short transfer
distance and low transfer
resistance
Disadvantage Fly temperature;
Channel flow		 Serious backmixing Metal film is limited by
high temperature
durability;
Non-metallic films are limited by selectivity		 Poor selectivity;
High energy
consumption		 Low energy
utilization efficiency;
High fluctuation due to weather influence		 High number
magnification cost;
Poor uniformity of fluid
distribution in parallel
operation
Table 4 The sequence of catalyst activity obtained by experimental or theoretical calculation under different conditions
Catalytic activity Carrier
(Theoretical calculation)		 External environment ref
Rh, Ru > Ni, Pd, Pt > Re > Ni0.7Cu1.3 > Co Al2O3 or MgO 500 ℃, 1 bar Rostrup-Nielsen[50]
Rh-Ru > Ni > Ir > Pd ~ Pt >> Co ~ Fe - 350 ~ 600 ℃, 1 bar Kikuchi et al.[51]
Pd MgO 550 ℃, 1 bar Rostrup-Nielsen et al.[52]
Ru > Rh > Ir > Pt > Pd MgO 600 ~ 900 ℃, 1 bar Qin et al.[53]
Ni ZrO2/CeO2, Al2O3 600 ℃ Wei and Iglesia[54⇓⇓⇓~58]
Ru ~ Rh > Ni ~ Ir ~ Pt ~ Pd ZrO2, Al2O3, MgAl2O4 500 ℃, 1 bar Jones et al.[59]
Ru > Rh > Ni > Ir > Pt ~ Pd Theoretical calculation 500 ℃, 1 bar Jones et al.[59]
Rh > Pt > Ni Theoretical calculation 600 ℃, PH2O-0.25 bar, $P_{H_2}$-0.4 bar, PCO-0.2 bar, $P_{CH_4}$-0.2 bar German et al.[43]
Pt > Ni > Rh Theoretical calculation 600 ℃, $P_{H_{2}O}$-0.25 bar, $P_{H_2}$-0.4 bar, PCO-0.2 bar, $P_{CH_{4}}$-1.5 bar German et al.[43]
Fig.3 The number of the by-product hydrogen from coke enterprises and chlor-alkali industry in China[61]
Table 5 The composition of different by-product hydrogen sources[62⇓⇓~65]
Volume fraction (%) P(MPa)
H2 CH4 CO CO2 N2 H2S O2 Cl2
Coke oven gas 55 ~ 60 23 ~ 27 6 ~ 9 - 2 ~ 5 0.5 ~ 3.0 - - ~0.03
Methanol exhaust 50 ~ 60 20 ~ 25 5 ~ 10 10 ~ 15 - - - - 5 ~ 7
Synthetic ammonia tail gas 50 ~ 60 15 ~ 20 - - 15 ~ 20 - - - 10 ~30
Exhaust gas from chlor-Alkali industrial (after alkali washing) ~98 <2 ppm 29 ppm 700 ppm 195 ppm - 1.34 10~20 ppm 0.1~0.6
Fig.4 Gas film separation process and mechanism: (a) diffusion process; (b) microporous diffusion mechanism; (c) solution-diffusion mechanism
Table 6 Comparison of different indicators of different hydrogen separation methods[63,87]
Cryogenic separation Organic membrane separation PSA
Scale (Standard conditions) (m3·h-1) 5000 ~ 100 000 100 ~ 64 900 10 000 ~ 500 000
Operating pressure(MPa) 1.0 ~ 8.0 10.0 ~ 15.0 0.5 ~ 6.0
Feed pressure(MPa) 1.0 0.2 ~ 0.5 1.0
Minimum hydrogen content of raw gas(%) 30 30 50
Preprocessing requirement Removing H2O、CO2、H2S Removing H2S No requirement
Purified hydrogen volume fraction(%) 90 ~ 95 80 ~ 99 > 99.99
Hydrogen recovery(%) 98 95 85
Relative investment expense(thousand) 20 ~ 30 10 10 ~ 30
Elasticity of operation(%) 30 ~ 50 30 ~ 100 30 ~ 100
Expansion difficulties Very difficult Very simple Simple
Fig.5 AEC electrolysis principle[104]. Copyright 2012, IEEE
Fig.6 The relationship between electrolytic temperature and electrolytic voltage[99]. Copyright 2009, Elsevier
Table 7 Calculation forms and meanings of different expressions of electrolytic efficiency[99]
Calculate formula Explain Supplement
Electrolytic efficiency $η_{V}=\frac{E_{O_2}-E_{H_2}}{E} \times 100\%$ The ratio of effective voltage of electrolysis to total voltage The electrolytic efficiency described by balancing electromotive force and electrolytic voltage is a common way to measure the electrolytic efficiency of hydrogen production system
Faraday efficiency $\eta_{\Delta G}=\frac{\Delta G}{\Delta G+Losses}=\frac{E_{\Delta G}}{E}$ The ratio of the theoretical energy of electrolytic water to the actual input energy $\eta_{25 ℃}=\frac{1.23V}{E}$
Thermal efficiency $\eta_{\Delta H}=\frac{\Delta H}{\Delta G+Losses}=\frac{E_{\Delta H}}{E}$ The proportion of the actual electrolytic energy that is input to maintain heat balance $\eta_{25 ℃}=\frac{1.48V}{E}$,1.48 is the electrolytic voltage when thermoneutral, and the thermal efficiency is 100% when E is equal to 1.48. The thermal efficiency can be higher than 100% when external heating is provided
Hydrogen production efficiency $\eta_{H_2}=\frac{283.8(kJ)}{Uit}$ The ratio of the energy generated by 1g of hydrogen to the total energy input The calorific value of hydrogen is 283.8kJ/g, U is the electrolytic voltage, i is the current, and t is the time required to produce 1g hydrogen
Net efficiency $\eta_{Loss}=1=\frac{E_{Loss}}{E_{input}}$ 1 minus the energy lost as a percentage of the total energy $E_{Loss}=\eta+iR_{cell}$
Table 8 Electrolytic parameters of different hydrogen electrode materials with current density of 100 mA/m2
T(℃) Concentration of KOH Overpotential(mV) Preparation methods ref
NiCu Room temperature 6 M -370 Electrodeposition Sang et al.[107]
Dense NiCu 35 6 M -500 Arc fusion Yu et al.[108]
Sintered Porous Ni-Cu 35 6 M -400 Powder metallurgy Yu et al.[108]
Metallurgical NiCu 25 6 M (NaOH) -300 Powder metallurgy Wang et al.[109]
Smooth NiCo 25 6 M -380 Electrodeposition Fan et al.[110]
NiCo 25 6 M -430 Electrodeposition Hong et al.[111]
Ra-Ni from Al 22 6 M -115 Pressing sintering Brennecke et al.[112]
Fig.7 Relationship curve of superpotential with current density of different hydrogen electrode & oxygen electrode materials. (a), (b): Hydrogen electrode; (c), (d): oxygen electrode; (a), (c): T=30 ℃; SS316l:Stainless steel (Cr17Ni12Mo2) disk electrode; Ra-Ni:Raney Ni (Raney Ni, porous nickel with high internal surface area); Electrolyte solution:KOH, 6 mol/L[106]
Fig.8 Electrolysis principle of PEMEC[104]. Copyright 2012, IEEE
Fig.9 Composition and basic principles of SOEC[104]. Copyright 2012, IEEE
Fig.10 The relationship of energy in SOEC with temperature[134]. Copyright 2009, Journal of Tsinghua University (Science and Technology)
Fig.11 Conductivity of different electrolyte materials[135]. Copyright 2008, Royal Society of Chemistry
Fig.12 The crystal structure of perovskite type oxygen electrode material for SOEC[139]. Copyright 2019, Royal Society of Chemistry
Fig.13 The OER’s specific activity of perovskite varies with the filling of eg orbital on the surface of B anion[140]. Copyright 2011, AAAS
Fig.14 Technical progress of SOEC and SOEC stack in recent 15 years: (a) Comparison of several typical hydroelectrolysis technologies; (b) SOEC monomer attenuation performance improvement; (c) SOEC stack duration tests progress; (d) the corresponding degradation of SOEC stack[4]. Copyright 2020, AAAS
Fig.15 SOEC stack developed and designed by INET, Tsinghua University
Fig.16 Solar photolysis of water to produce hydrogen[171]. Copyright 2019, Elsevier
Fig.17 The band gap of several semiconductors[172]. Copyright 2020, Elsevier
Fig.18 Z-type semiconductor catalyst[178]
Table 9 Basic information of major hydrogen production process
Hydrogen production process Raw material Technology maturity Energy conversion efficiency (%) Cost
(/Yuan·kg-1)		 CO2 emission (kg CO2/kg H2)
Fossil fuel
reforming		 Coal gasification Coal Mature ~47[62] 6~10[10] 11~25[10]
Coal gasification +CCS Coal Completing pilot scale test - 12~16[10] 2~7[10]
Coal supercritical water gasification Coal, water Completing pilot scale test ~60a[31] ~8[36] ~0[10]
SMR methane Mature - 9~18[10] 8~16[10]
Industrial by-product of hydrogen Industrial exhaust Mature - 10~16[10] -
Electrolysis of
water		 Grid electricity/AEC Water Mature ~25[133] 30~40[10] ~45[10]
Renewable energy sources electrolyze water AEC Water Mature ~25[133] 18~23[10] 1~3[10]
PEMEC Water Relatively mature, Early industrialization ~35[133] ≤62[191] 1~3[10]
SOEC Water demonstration works 52 ~ 59[133] - 1~3[10]
Abandoned electric from Renewable energy sources electrolyzes water Water Demonstration stage - ~10[10] 1~3[10]
Other new
technologies for hydrogen production		 Solar energy photolysis water Water Laboratory stage <10[182] - ~0[10]
Biomass fermentation Biomass Demonstration stage 10~40[188]b - ~0[10]
Biomass gasification Biomass Mature 35~50[197] ~16[191] 0.4~5.6[198]
Thermochemical cycle Water Laboratory stage ~38[198] ~18[191] 0.3~0.86[198]
Fig.19 Basic structure of wind power hydrogen production system[200]。Copyright 2019, SAGE
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