催化学报 ›› 2023, Vol. 55: 44-115.DOI: 10.1016/S1872-2067(23)64544-9

• 综述 • 上一篇    下一篇

联产混合电解水策略实现节能电化学制氢的最新进展

Diab khalafallaha,b,*(), 张运祥a, 王昊c, Jong-Min Leed,*(), 张勤芳a,e,*()   

  1. a盐城工学院材料科学与工程学院, 江苏盐城 224051, 中国
    b阿斯旺大学能源工程学院机械设计与材料系, 埃及
    c南京大学超导电子学研究所, 江苏南京 210023, 中国
    d新加坡南洋理工大学化学与生物医学工程学院, 新加坡
    e盐城工学院江苏省生态环境材料重点实验室, 江苏盐城 224051, 中国
  • 收稿日期:2023-08-04 接受日期:2023-10-13 出版日期:2023-12-18 发布日期:2023-12-07
  • 通讯作者: *电子信箱: diab_khalaf@energy.aswu.edu.eg (D. khalafallah), jmlee@ntu.edu.sg (J.-M. Lee), qfangzhang@gmail.com (张勤芳).
  • 基金资助:
    国家自然科学基金(12274361);江苏省自然科学基金(BK20211361);江苏省高校自然科学研究项目(20KJA430004)

Energy-saving electrochemical hydrogen production via co-generative strategies in hybrid water electrolysis: Recent advances and perspectives

Diab khalafallaha,b,*(), Yunxiang Zhanga, Hao Wangc, Jong-Min Leed,*(), Qinfang Zhanga,e,*()   

  1. aSchool of Materials Science and Engineering, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China
    bMechanical Design and Materials Department, Faculty of Energy Engineering, Aswan University, P.O. Box 81521, Aswan, Egypt
    cResearch Institute of Superconductor Electronics, Nanjing University, Nanjing 210023, Jiangsu, China
    dSchool of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore 637459, Singapore
    eJiangsu Provincial Key Laboratory of Eco-Environmental Materials, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China
  • Received:2023-08-04 Accepted:2023-10-13 Online:2023-12-18 Published:2023-12-07
  • Contact: *E-mail: diab_khalaf@energy.aswu.edu.eg (D. khalafallah), jmlee@ntu.edu.sg (J.-M. Lee), qfangzhang@gmail.com (Q. Zhang).
  • About author:Diab Khalafallah received his M.Sc. degree in 2012 and PhD degree in 2017. He is currently an Associate professor at the Faculty of Energy Engineering, Aswan University (Egypt). Khalafallah joined the Yancheng Institute of Technology (Jiangsu, China) as a researcher in the School of Materials Science and Engineering. His research activities are focused on developing functional materials for energy conversion and storage systems including hybrid water electrolysis, hydrogen evolution reaction, supercapacitors, and water splitting.
    Jong-Min Lee received his Ph.D. degree at the Department of Chemical Engineering, Columbia University. He worked in the Chemical Science Division, Lawrence Berkeley National Laboratory and at the Department of Chemical Engineering, University of California at Berkeley as a postdoctoral fellow. Currently, he is an associate professor in the School of Chemical and Biomedical Engineering at Nanyang Technological University. His research interests are electrochemistry, green chemistry, and nanotechnology.
    Dr. Qinfang Zhang is currently a full professor at the Yancheng Institute of Technology (Jiangsu, China). He received his PhD degree from the Nanjing University in 2005. His current research focus on the preparation and application of atomic clusters and oxyhalides. From 2005, he has published more than 100 research papers in peer-reviewed journals, such as: Phys. Rev. Lett., Nature Comm., Adv. Mater., Phys. Rev. B, Appl. Surf. Sci., Appl. Phys. Lett. His publications have been cited 3687 times, and his H-Index is 31. He has been leading 14 scientific research projects including the National Defense Science and Technology Innovation Special Zone Project, the National Natural Science Foundation of China, and the Provincial Outstanding Youth Fund and so on.
  • Supported by:
    National Natural Science Foundation of China(12274361);Natural Science Foundation of Jiangsu Province(BK20211361);College Natural Science Research Project of Jiangsu Province(20KJA430004)

摘要:

随着全球能源需求增长和环境污染加剧, 发展可持续能源减少对化石燃料(如石油、天然气和煤炭等)的消耗成为实现人类社会可持续发展的关键. 氢能因其能量密度高、燃烧无污染、应用形式多样被认为是最理想的替代能源. 电解水制氢包括阴极析氢反应(HER)和阳极析氧反应(OER), 具有绿色环保、生产灵活和纯度高等特点, 是理想的绿色生产技术之一. 然而, 阳极电解水产氧反应动力学缓慢, 导致阴极的产氢效率低. 此外, 在电解水过程中, 会产生高氧化性的过氧化氢(H2O2), 降低电解水膜的寿命, 阻碍电解水技术的实际应用. 因此, 亟待开发新型高效、稳定且具有高附加值的电解水催化剂. 目前, 电化学整体水分解(OWS)制氢技术存在安全风险、投资回报低、阳极OER动力学慢和电能消耗大等问题, 将阳极氧化反应与混合电解水(HWE)装置中的HER相结合, 借助热力学较好的电氧化反应取代缓慢的传统OER反应协同产氢, 可以有效克服传统电解水的产率不足, 解决污染排放和生物质回收问题.

本文综述了协同电催化用于联产氢气和低能耗、高法拉第效率高价值产品的催化剂结构设计, 揭示不同协同电催化系统的催化途径和意义, 以实现更高效、零碳排放的目标. 首先, 介绍了HWE系统的发展现状, 重点关注各种富氢物质的协同电解, 例如酒精、生物质衍生物、葡萄糖和在阳极形成的高附加值化学品. 与传统阳极OER工艺相比, 有机/生物质底物小分子的OER表现出较低的热力学需求, 降低产氢能耗. 随后, 详细介绍了基于阴极HER和阳极OER协同电解反应、协同催化HWE高效电极/电催化剂的合理设计, 以实现高催化活性、高选择性和良好的电化学稳定性. 重点讨论了新型电极/电催化剂设计、活性改进以及结构-催化活性关系提升的合成策略. 再后, 讨论了基于有机/生物质小分子协同HWE系统电催化的代表性研究进展和突破, 强调了其在促进可持续低压制氢方面的重要作用, 并回顾了近年来HWE的研究突破, 同时, 对一些可行性分析和机理探索进行比较, 为制氢提供了新的研究方向. 最后, 提出了协同电催化制氢面临的挑战并展望未来的研究方向.

综上, 大多数电催化剂存在催化活性低、稳定性差等问题, 要实现可持续、经济高效和清洁的产氢技术, 仍有很多方面需要进一步的深入研究. 本文综述了高效多功能HWE系统发展现状和催化剂结构设计, 为电解水制氢和高附加值产品的节能联产提供一定的参考.

关键词: 阳极氧化反应, 小有机分子, 混合电解水, 节能制氢, 附加值产品, 过渡金属, 协调效应, 活性位, 催化活性, 稳定性

Abstract:

Traditional overall water splitting has been regarded as a potential pathway for H2 production, but the intrinsic slow kinetics of the anodic oxygen evolution reaction severely hampers the efficiency of H2 production. Given the challenges in traditional water electrolysis, coupling the kinetically favorable anodic electrooxidation reactions of easily oxidizable substances with the hydrogen evolution reaction in a hybrid water electrolysis (HWE) configuration not only solves the pollutant emission and biomass recycling problems but also maximizes the return on energy profiteering. Various advanced compounds have been engineered through compositional regulation, structural optimization, surface nano-building, and electronic structure modification, yet some issues like tedious preparation and unsatisfactory durability still exist. Considering the gap between research and practical deployment, this review amply addresses the state-of-the-art achievements of synergistic electrocatalysis systems for the co-production of high-purity H2 and valuable products with a low energy consumption and high Faradaic efficiency. An overview of HWE system is presented first accompanied by a discussion on the design and engineering of high reactive/selective/stable electrodes/electrocatalysts for anodic oxidation of organic/biomass substrates. Importantly, the in-depth understanding of possible reaction mechanisms from both experimental and theoretical perspectives is elucidated to promote the efficiency of synergistic electrocatalysis. Subsequently, the recent research breakthroughs in the field of HWE technology are emphatically reviewed, providing a new room for low-voltage H2 generation from waste products and renewable feedstock. Some mechanism explorations, feasibility analyses, and correlation comparisons are highlighted. Finally, we propose the prospects on existing challenges with some opportunities for future research directions to push forward the progress in synergistic electrocatalysis configurations.

Key words: Anodic electrooxidation reaction, Small organic molecule, Hybrid water electrolysis, Energy-saving H2 production, Value-added product, Transition metal, Synergistic effect, Active site, Catalytic activity, Stability