单原子催化剂在电催化氧还原直接合成过氧化氢中的研究进展

doi:10.16085/j.issn.1000-6613.2022-1480

摘要/Abstract

摘要：

电催化二电子氧还原过程产过氧化氢具有绿色、高效、安全、即时的特点，是一项被认为能够代替传统高污染，能耗密集型蒽醌生产的潜在技术，但仍具有挑战性。单原子催化剂具有原子利用率高、位点均一、催化活性高的优点，在电催化氧还原产过氧化氢中展现了广阔的应用前景。本文重点综述了贵金属单原子催化剂和过渡金属单原子催化剂在氧还原二电子产过氧化氢中的研究进展，着重于通过实验和理论计算结合的方式揭示电催化氧还原二电子催化活性和结构的联系。总结提出了提升单原子催化剂在二电子氧还原反应性能的调控策略，包括金属活性中心调控、配位结构调控、局域微环境调控，旨在为设计高活性、高选择性电催化氧还原二电子产过氧化氢催化剂提供借鉴和设计思路。文章对单原子催化剂在电催化氧还原产过氧化氢应用中的机遇和挑战进行了展望。单原子催化剂在活性位点表征、稳定性、制备方法等方面亟需改善，以促进其在电催化氧还原制过氧化氢中的发展。

关键词: 过氧化氢, 催化剂, 氧还原反应, 电化学

Abstract:

With the merits of green, effective, safe and on site, hydrogen peroxide production via electrocatalytic two-electron oxygen reduction process is considered as an alternative to the traditional high pollution and energy intensive anthraquinone method. Benefitting from the virtues of high atom utilization, homogeneous active sites and high activity, single atom catalysts for two-electron oxygen reduction show great potential in hydrogen peroxide production. This paper focuses on the progress of single atom catalysts including both noble metal and non-precious metal in electrocatalytic oxygen reduction to hydrogen peroxide. Both experimental results and theoretical calculations are emphasized to reveal the relations between electronic structure and catalytic performance. Strategies to enhance the two-electron catalytic performance including altering of central metal atoms, regulation of coordinated atoms and local environment are also summarized. This paper aims to provide ideas and reference for the design of catalysts with high activity and selectivity towards hydrogen peroxide production. Opportunities and challenges of single atom catalysts for electrocatalytic oxygen reduction to hydrogen peroxide are prospected. Characterization of active sites, stability and preparation method for single atom catalysts are urgently needed to be improved to promote their development in hydrogen peroxide production via electrocatalytic oxygen reduction.

Key words: hydrogen peroxide, catalysts, oxygen reduction reaction, electrochemistry

中图分类号:

O643.36

张鹏, 潘原. 单原子催化剂在电催化氧还原直接合成过氧化氢中的研究进展[J]. 化工进展, 2023, 42(6): 2944-2953.

ZHANG Peng, PAN Yuan. Progress of single atom catalysts in electrocatalytic oxygen reduction to hydrogen peroxide[J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2944-2953.

图/表 6

图1 Pt1-CuS x 单原子催化剂合成及电催化氧还原产过氧化氢性能图[20]

图2 Fe单原子催化剂电催化氧还原性能火山图及其ORR催化性能图[30]

图3 Co单原子催化剂制备及其电催化氧还原制过氧化氢催化性能图[35]

图4 不同金属中心单原子M-N-C对ORR二电子过程催化性能的影响[31]

图5 配位结构调控Co单原子催化剂ORR二电子催化性能图[45]

图6 氧官能团修饰Co单原子催化剂ORR二电子电催化活性和选择性图[46]

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