Constructing sulfur and oxygen super-coordinated main-group electrocatalysts for selective and cumulative H2O2 production

被引：63

作者：

Zhou, Xiao ^{[1
]}

Min, Yuan ^{[1
]}

Zhao, Changming ^{[2
]}

Chen, Cai ^{[2
]}

Ke, Ming-Kun ^{[1
]}

Xu, Shi-Lin ^{[1
]}

Chen, Jie-Jie ^{[1
]}

Wu, Yuen ^{[2
]}

Yu, Han-Qing ^{[1
]}

机构：

[1] Univ Sci & Technol China, Dept Environm Sci & Engn, CAS Key Lab Urban Pollutant Convers, Hefei 230026, Peoples R China

[2] Univ Sci & Technol China, Sch Chem & Mat Sci, Hefei 230026, Peoples R China

来源：

NATURE COMMUNICATIONS | 2024年 / 15卷 / 01期

基金：

中国国家自然科学基金;

关键词：

TOTAL-ENERGY CALCULATIONS; HYDROGEN-PEROXIDE; ELECTROCHEMICAL SYNTHESIS; CATALYTIC-ACTIVITY; FORMIC-ACID; REDUCTION; WATER; ELECTROSYNTHESIS; ELECTROLYSIS; EFFICIENCY;

D O I：

10.1038/s41467-023-44585-1

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Direct electrosynthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction presents a burgeoning alternative to the conventional energy-intensive anthraquinone process for on-site applications. Nevertheless, its adoption is currently hindered by inferior H2O2 selectivity and diminished H2O2 yield induced by consecutive H2O2 reduction or Fenton reactions. Herein, guided by theoretical calculations, we endeavor to overcome this challenge by activating a main-group Pb single-atom catalyst via a local micro-environment engineering strategy employing a sulfur and oxygen super-coordinated structure. The main-group catalyst, synthesized using a carbon dot-assisted pyrolysis technique, displays an industrial current density reaching 400mA cm(-2) and elevated accumulated H2O2 concentrations (1358mM) with remarkable Faradaic efficiencies. Both experimental results and theoretical simulations elucidate that S andOsuper-coordination directs a fraction of electrons from the main-group Pb sites to the coordinated oxygen atoms, consequently optimizing the *OOHbinding energy and augmenting the 2e(-) oxygen reduction activity. This work unveils novel avenues for mitigating the production-depletion challenge in H2O2 electrosynthesis through the rational design of main-group catalysts.

引用

页数：13

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