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化学进展 2021, Vol. 33 Issue (12): 2215-2244 DOI: 10.7536/PC201128 前一篇   后一篇

• 综述 •

中国制氢技术的发展现状

曹军文, 张文强, 李一枫, 赵晨欢, 郑云, 于波*()   

  1. 清华大学核能与新能源技术研究院 北京 100084
  • 收稿日期:2020-11-23 修回日期:2021-03-22 出版日期:2021-12-20 发布日期:2021-07-29
  • 通讯作者: 于波
  • 基金资助:
    国家自然科学基金项目(No.91645126和21273128(91645126); 国家自然科学基金项目(No.91645126和21273128(21273128); 清华大学自主科研计划(2018Z05JZY010); 清华-MIT-剑桥低碳能源大学联盟种子基金项目(201LC004)
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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:2020-11-23 Revised:2021-03-22 Online:2021-12-20 Published:2021-07-29
  • 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)

氢能是一种高效清洁的二次能源,在实现“碳中和”目标中起重要作用。随着制氢规模不断扩大、制氢成本不断降低,氢能将有望与电能共同成为二次能源主体,通过氢电互补推动我国能源结构转型、降低碳排放、保障我国能源安全。目前,我国已成为世界第一大产氢国,主要有三类工业制氢路线:化石燃料重整制氢、工业副产氢和清洁能源电解水制氢。依托清洁能源发展起来的其他制氢新技术,如太阳能光解水制氢、生物质制氢、核能制氢等也受到广泛研究和关注。此外,制氢系统组成复杂,建模和优化难度高,人工智能在制氢系统的预测、评估和优化方面表现出独特的优势,受到国际学者的关注。本文结合最新研究进展,对上述制氢路线的发展情况进行了综述,并通过技术成熟度、经济性和环保性比较,结合国情对我国未来氢气供应结构做出展望。同时,本文综述了人工智能在制氢系统中的最新应用进展,以期为我国制氢工艺发展提供新思路。

关键词： 制氢, 化石能源重整, 工业副产氢, 电解水, 其他制氢新技术, 人工智能

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
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图1 国内外氢能产业链对比
Fig.1 Comparison of hydrogen energy industry chain at home and abroad
表1 煤气化的主要反应
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
图2 煤气化制氢流程图[15]
Fig.2 The process of coal gasification to produce hydrogen[15]
表2 四种常见气化炉的基本信息
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		 -
表3 几种典型天然气制氢反应器的主要特点对比[37]
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
表4 不同条件下通过实验或理论计算得到的催化剂活性顺序
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]
图3 我国焦炭企业和氯碱工业历年副产氢量及其总量[61]
Fig.3 The number of the by-product hydrogen from coke enterprises and chlor-alkali industry in China[61]
表5 不同副产氢源的组成成分[62⇓⇓~65]
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
图4 气体膜分离过程及机理:(a)扩散过程;(b)微孔扩散机理;(c)溶解-扩散机理
Fig.4 Gas film separation process and mechanism: (a) diffusion process; (b) microporous diffusion mechanism; (c) solution-diffusion mechanism
表6 不同工业氢气分离方式的不同指标对比[63,87]
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
图5 AEC电解原理[104]
Fig.5 AEC electrolysis principle[104]. Copyright 2012, IEEE
图6 电解温度与电解电压的关系[99]
Fig.6 The relationship between electrolytic temperature and electrolytic voltage[99]. Copyright 2009, Elsevier
表7 不同电解效率的计算形式及含义[99]
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 $E_{Loss}=\eta+iR_{cell}$
表8 电流密度为100 mA/m2的不同氢电极材料电解参数
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]
图7 不同氢电极和氧电极材料超电势随电流密度变化的关系曲线。(a), (b)氢电极;(c), (d)氧电极;(a), (c)T=30 ℃;SS316L:不锈钢(Cr17Ni12Mo2)圆盘电极;Ra-Ni:兰尼镍(Raney Ni,具有高内表面积的多孔镍);电解质溶液:KOH,6 mol/L[106]
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]
图8 PEMEC的电解原理[104]
Fig.8 Electrolysis principle of PEMEC[104]. Copyright 2012, IEEE
图9 SOEC的组成和基本原理[104]
Fig.9 Composition and basic principles of SOEC[104]. Copyright 2012, IEEE
图10 SOEC中各部分能量随温度的变化关系[134]
Fig.10 The relationship of energy in SOEC with temperature[134]. Copyright 2009, Journal of Tsinghua University (Science and Technology)
图11 不同电解质材料的电导率[135]
Fig.11 Conductivity of different electrolyte materials[135]. Copyright 2008, Royal Society of Chemistry
图12 SOEC的钙钛矿型氧电极材料晶体结构[139]
Fig.12 The crystal structure of perovskite type oxygen electrode material for SOEC[139]. Copyright 2019, Royal Society of Chemistry
图13 钙钛矿的OER比活度随B位阴离子表面的eg轨道填充变化关系[140]
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
图14 近15年SOEC和SOEC堆的技术进展:(a)不同电解池初始性能比较;(b)SOEC单体衰减性能的提升;(c)SOEC堆测试时长进展;(d)SOEC堆衰减性能的提升[4]
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
图15 清华大学核研院自主研发设计的SOEC电堆
Fig.15 SOEC stack developed and designed by INET, Tsinghua University
图16 太阳能光解水制氢[171]
Fig.16 Solar photolysis of water to produce hydrogen[171]. Copyright 2019, Elsevier
图17 部分半导体的能带带隙[172]
Fig.17 The band gap of several semiconductors[172]. Copyright 2020, Elsevier
图18 Z型半导体催化剂[178]
Fig.18 Z-type semiconductor catalyst[178]
表9 主要制氢工艺的基本信息比较
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]
图19 风力制氢系统的基本结构[200]
Fig.19 Basic structure of wind power hydrogen production system[200]。Copyright 2019, SAGE
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摘要

中国制氢技术的发展现状