碳基催化剂用于两电子氧还原合成过氧化氢的研究进展  

Recent progress on carbon-based electrocatalysts for hydrogen peroxide production via two-electron oxygen reduction reaction

作　　者：许琴 王保国[1] XU Qin;WANG Baoguo(Department of Chemical Engineering,Tsinghua University,Beijing 100084,China)

机构地区：[1]清华大学化学工程系,北京100084

出　　处：《化工进展》2024年第11期6155-6172,共18页Chemical Industry and Engineering Progress

基　　金：国家自然科学基金(222278239)。

摘　　要：电化学两电子氧还原反应(2e-ORR)制备过氧化氢(H_(2)O_(2))是一种可替代工业蒽醌法的绿色环保且安全高效的技术路线,具有广阔发展前景。然而,受限于缓慢的氧还原反应(ORR)动力学以及竞争的四电子反应过程,开发具有高氧还原反应活性以及两电子选择性的高性能催化剂是目前研究的核心关键。近年来,碳基材料因其储量丰富、成本低廉、结构易于调控等优势,被广泛应用于2e-ORR合成H_(2)O_(2)领域,并取得了显著的研究进展。基于此,本文首先简要介绍了氧还原过程的基本原理以及催化剂的一般评价方法,指出了构建高效催化剂的基本设计指导原则;其次重点综述了近年来碳基催化剂用于2e-ORR制备H_(2)O_(2)的最新研究进展,针对非金属碳基材料和过渡金属碳基材料两大类,细致讨论并总结了异相原子掺杂、缺陷工程、孔结构工程、单原子局部微环境调控等催化剂活性位点优化策略对提升催化性能的作用效果;最后,针对H_(2)O_(2)生产介质、催化剂结构-性能关系以及在工业级电流密度下稳定生产H_(2)O_(2)三方面,展望了两电子氧还原合成H_(2)O_(2)领域未来发展的挑战及方向。The production of hydrogen peroxide(H_(2)O_(2))via electrochemical two-electron(2e-)oxygen reduction reaction(ORR)is a green,safe and efficient technical route,showing broad development prospects as an alternative to the industrial anthraquinone process.However,this route at present is limited by the sluggish ORR kinetics and the competitive four-electron(4e-)reaction,and thus it is critically desired to develop efficient catalysts with high ORR activity and selectivity.Currently,carbon-based materials are the most widely studied catalysts for electrosynthesis of H_(2)O_(2) via 2e-ORR and great progress has been made due to their abundance in earth,low cost and tunable catalytic properties.This review summarizes the recent advances in carbon-based electrocatalysts for 2e-ORR to H_(2)O_(2).Fundamental principles of the ORR and general methods of electrocatalyst evaluation are first introduced and the basic design guidelines for constructing highly-efficient electrocatalyst is also pointed out.Next,with a focus on the non-metal carbon-based materials and transition-metal carbon-based materials,the active site optimization strategies of catalysts including heteroatom doping,defect engineering,pore engineering and single-atom site local environment regulation are in depth discussed.Finally,the challenges and future development trend in the field of H_(2)O_(2)electrosynthesis by 2e-ORR are proposed in terms of H_(2)O_(2) production medium,catalyst structure-performance relationship and steady production under industrial current densities.

关 键 词：两电子氧还原反应 过氧化氢 电化学合成 碳基催化剂 选择性 

分 类 号：O643.3[理学—物理化学]