催化学报

催化学报 ›› 2024, Vol. 58: 1-6.DOI: 10.1016/S1872-2067(23)64625-X

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电化学合成耦合可再生能源制氢: 机遇与挑战

魏子栋a,*(), 黄寻a, 段昊泓b, 邵明飞c, 李仁贵d, 张金利e, 李灿d,*(), 段雪c,*()   

  1. a重庆大学化学化工学院, 重庆400044
    b清华大学化学系, 北京100084
    c北京化工大学化学学院, 北京100029
    d中国科学院大连化学物理研究所, 辽宁大连116023
    e天津大学化工学院, 天津300072
  • 收稿日期:2024-01-08 接受日期:2024-02-18 出版日期:2024-03-18 发布日期:2024-03-28
  • 通讯作者: *电子信箱: zdwei@cqu.edu.cn (魏子栋),canli@dicp.ac.cn (李灿);duanx@mail.buct.edu.cn (段雪).
  • 基金资助:
    国家自然科学基金(22342016);国家自然科学基金(22090030);国家自然科学基金(22325805);国家自然科学基金(22178033)

Electrochemical synthesis in company with hydrogen production via renewable energy: Opportunities and challenges

Zidong Weia,*(), Xun Huanga, Haohong Duanb, Mingfei Shaoc, Rengui Lid, Jinli Zhange, Can Lid,*(), Xue Duanc,*()   

  1. aSchool of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China
    bDepartment of Chemistry, Tsinghua University, Beijing 100084, China
    cSchool of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China
    dDalian Institute of Chemical Physics, Chinese Academy of Science, Dalian 116023, Liaoning, China
    eSchool of Chemical Engineering, Tianjin University, Tianjin 300072, China
  • Received:2024-01-08 Accepted:2024-02-18 Online:2024-03-18 Published:2024-03-28
  • Contact: *E-mail: zdwei@cqu.edu.cn (Z. Wei),canli@dicp.ac.cn (C. Li),duanx@mail.buct.edu.cn (X. Duan).
  • About author:Zidong Wei (College of Chemistry and Chemical Engineering, Chongqing University) was invited as an Associate Editor of the 6th Editorial Board of Chin. J. Catal. Prof. Zidong Wei received his BSc. Degree in material science and technology in 1984 at Shaanxi University of Science and Technology, his MSc. Degree in analytical chemistry in 1987 at Shaanxi Normal University and his Ph.D. in applied chemistry in 1994 at Tianjin University. He carried out his overseas research as a JACA fellow at Catalysis Research Center in Hokkaido University (Japan) from May, 2001 to November, 2001, and as a TCT fellow at Fuel Cells Center in Nanyang Technology University (Singapore) from October, 2002 to January, 2003. Since June, 1997, he has been working in Chongqing University. He was appointed as the dean of the college of Chemistry and Chemical Engineering, Chongqing University from 2010 to 2021. He was also appointed as a Chungkung Professor by the Ministry of Education of China in 2009. He is now the Professor and the Director of the National Local Joint Engineering Laboratory of Chemical Process Intensification, Chongqing University. His research interests mainly focuses on chemical energy conversation, electrocatalysis, electrosynthesis, advanced chemical power and water electrolysis with experimental investigation and theoretical simulation. He has published more than 300 peer reviewed papers and obtained more than 40 invention patents in China. His work has been cited over 23,000 times. He is the author of two books, Electrochemical Catalysis, and Electrocatalysis of Oxygen Reduction Reaction.
    Can Li (Dalian Institute of Chemical Physics, Chinese Academy of Science) received his Ph.D. degree from Dalian Institute of Chemical Physics, Chinese Academy of Sciences in 1988 through a cooperative program with Tokyo Institute of Technology, Japan. He later joined the same institute and was promoted to full professor in 1993. He conducted postdoctoral research at Northwestern University in the USA. He was elected as a member of the Chinese Academy of Sciences in 2003, a member of the Academy of Science for Developing Countries in 2005, a foreign member of Academia European in 2008, and a Fellow of the Royal Society of Chemistry in 2008. His research interests include in-situ/operando spectroscopic studies on catalysts and catalytic reactions. His research has been focused on photocatalytic, photoelectrocatalytic and electrolytic water splitting, and CO2 reduction utilizing renewable energy for solar fuel production. A 1000-ton scale pilot production of liquid sunshine methanol was successfully demonstrated in China in 2020. He is the Editor-in-Chief of the Chin. J. Catal. and serves on the editorial boards of several international journals. He has published more than 900 peer-reviewed papers with over 40000 citations, more than 200 granted patents and over 150 plenary and keynote lectures at international conferences.
    Xue Duan (School of Chemistry, Beijing University of Chemical Technology) received his B.S. in 1982 from Jilin University and Ph.D. degree in 1988 from Chinese Academy of Sciences. He later joined BUCT staff and founded the Applied Chemistry Research Institute in 1990. In 2007, he was elected as an Academician of the Chinese Academy of Sciences. He has published over 400 research papers in leading SCI international journals in chemical engineering, chemistry, and materials. He has been acknowledged as a Highly Cited Chinese Researcher for several years. Prof. Duan has developed a unique research program focusing on Intercalation Assembly and Resource Utilization. He has introduced innovative concepts like correlating the deformation of octahedral metal sites with intercalated materials' structure, coupling catalytic reactions with heat transfer, ultrastable mineralization, green hydrogen generation, and carbonate mineral hydrorefining. More than 30 industrial production lines have been built based on his technologies to manufacture salt-lake resource related materials, automotive fine chemicals, mesoporous adsorption materials, and soil remediation materials.
  • Supported by:
    National Nature Science Foundation of China(22342016);National Nature Science Foundation of China(22090030);National Nature Science Foundation of China(22325805);National Nature Science Foundation of China(22178033)

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摘要：

利用可再生能源实现物质和能量的转化, 是发展节能减排技术、实现双碳目标的重要手段. 有机电合成是一种温和、清洁、高效的物质合成方法, 可以有效解决传统化工过程的高能耗和高污染问题. 将电解水制氢与有机电合成耦合, 利用水分解产生的活性氧/氢直接氧化/还原有机物, 不仅有助于降低能耗, 还可以生产高附加值有机化工产品, 是提高电能利用效率、降低生产成本的有效方案. 然而, 尽管这种方法具有诸多优势, 其工业化应用仍面临一系列难题.

本文回顾了电化学合成的发展历史, 探讨了氢能时代为电化学合成带来的发展机遇. 同时, 分析了将电化学合成与电解水耦合所面临的挑战以及未来发展方向. 首先, 应当慎重选择与电解水制氢耦合的阳极反应体系, 其氧化产物不但要具有比反应物更高的经济价值, 而且要有较大的市场需求量, 以匹配制氢规模. 其次, 虽然在热力学上有机物氧化比析氧更容易发生, 但在动力学及传质方面, 有机物氧化可能存在劣势, 因此必须开发适用于工业制氢电流密度(500‒2000 mA cm‒2)的有机物氧化电极材料. 第三, 阳极有机产物选择性不仅影响反应物的利用率, 而且决定后续分离纯化成本, 需要通过调控活性氢/氧及有机物表面的竞争吸附等手段, 提高阳极目标产物选择性及法拉第效率. 第四, 隔膜是分离两极反应物料、防止副反应发生的重要部件. 然而, 现有的阴、氧离子交换膜的耐有机物腐蚀性能差, 需要开发适用于电解耦合体系的、具有高离子传导能力且性能稳定的新型隔膜材料. 最后, 当有机物氧化与电解水耦合后, 产物的分离复杂程度增加, 需要将精馏、萃取、膜分离等手段与电化学反应相结合, 以提升电解过程效率.

综上, 本文讨论了电化学合成耦合可再生能源制氢的若干技术难题, 为未来电合成与氢能技术共同发展提供新思路.

关键词: 电化学合成, 电解水制氢, 反应匹配, 产物选择性, 隔膜稳定性, 过程强化

Abstract:

Organic electromechanical synthesis is an eco-friendly and efficient method for material synthesis, effectively addressing the high energy consumption and pollution problems in the traditional chemical industry. By combining hydrogen production from water electrolysis with organic electromechanical synthesis, the reactive oxygen/hydrogen from water hydrolysis can be utilized to oxidize/reduce organic compounds, reducing energy consumption and producing valuable organic products. However, this strategy still faces challenges when implemented in the industry. This paper addresses major technical challenges in the field, providing new insights for future advancements. Firstly, when selecting anode reactions for hydrogen production, it is important to consider the value and market demand of the oxidation product to match the production scale. Secondly, the development of efficient electrocatalysts and electrodes is required to enhance the oxidation kinetics and mass transfer of organics at the current density levels of industrial hydrogen production (500‒2000 mA cm‒2). Thirdly, it is essential to improve the selectivity and Faraday efficiency of the anode target product to lower the cost of subsequent separation and purification. Fourthly, existing anion and oxygen ion exchange membranes lack corrosion resistance to organic matter, and new separator materials with high ion conductivity and stability are crucial for the electrolytic coupling system. Finally, when combining organic oxidation and water electrolysis, the complexity of product separation increases, and it is recommended to integrate distillation, extraction, membrane separation, and electrochemical reactions to improve process efficiency.

Key words: Electrochemical synthesis, Hydrogen evolution, Reaction match, Product selectivity, Membrane stability, Process intensification