两电子氧还原制备过氧化氢:贵金属催化剂的几何与电子结构调控的研究进展  

Progress on Tuning the Geometric and Electronic Structure of Precious Metal Catalysts for Hydrogen Peroxide Production via Two-Electron Oxygen Reduction

作　　者：罗二桂 唐涛 王艺 张俊明 常宇虹 胡天军[1] 贾建峰[1] LUO Er-Gui;TANG Tao;WANG Yi;ZHANG Jun-Ming;CHANG Yu-Hong;HU Tian-Jun;JIA Jian-Feng(Key Laboratory of Magnetic Molecules and Magnetic Information Materials of Ministry of Education&School of Chemistry and Materials Science of Shanxi Normal University,Taiyuan 030032,China)

机构地区：[1]山西师范大学化学与材料科学学院,磁性分子与磁信息材料教育部重点实验室,太原030032

出　　处：《应用化学》2023年第8期1063-1076,共14页Chinese Journal of Applied Chemistry

基　　金：国家自然科学基金(No.22209102);山西省自然科学基金(Nos.20210302124473,202203021212398)资助。

摘　　要：通过两电子氧还原反应(2e-ORR)电化学合成过氧化氢(H_(2)O_(2))的显著优势是高成本效益和环境友好性,且可以实现H_(2)O_(2)的按需现场生产,其关键技术之一是安全、经济和高效2e-ORR催化剂的开发。本文概述了利用2e-ORR制备H_(2)O_(2)贵金属基催化材料近10年的研究进展。从ORR反应机理出发,介绍了贵金属表面反应途径的调节旋钮,即*OOH结合能和O_(2)吸附模式;重点总结并举例说明了贵金属材料的几何结构和电子结构调控的方法学,强调了平衡优化催化活性和选择性的重要性;此外,简要介绍了基础实验室中2e-ORR催化剂性能的评估方法;最后,讨论了贵金属电催化合成H_(2)O_(2)的挑战和前景,特别是催化剂的稳定性和成本的客观评价。旨在为新型2e-ORR催化剂的理性设计提供参考。Electrochemical synthesis of hydrogen peroxide(H_(2)O_(2))via two-electron oxygen reduction reaction(2e-ORR)is featured with cost effectiveness and environmental friendliness,and enables on-site production of H_(2)O_(2)on demand.One of the key technologies is the development of safe,economical and efficient 2e-ORR catalysts.Here,the research progress in precious-metal-based catalytic materials for the synthesis of H_(2)O_(2)via 2e-ORR in recent ten years is reviewed.This review starts with the fundamental mechanism of ORR,pointing out the tuning knobs of reaction pathway on precious-metal surfaces,namely,*OOH binding energy and O_(2)adsorption mode.The regulating methodologies of geometric structure and electronic structure of precious-metal materials are summarized and exemplified,emphasizing the importance of balanced optimization of catalytic activity and selectivity.We have also briefly introduced the lab-scale methods for performance evaluation of 2e-ORR catalysts.Finally,the challenges and prospects of H_(2)O_(2)synthesis catalyzed by precious metals are discussed,especially the catalyst stability and the objective evaluation of cost.This review is expected to provide a reference for rational design of novel 2e-ORR catalysts.

关 键 词：电化学合成过氧化氢 氧还原反应 贵金属催化剂 选择性 

分 类 号：O646[理学—物理化学]