电合成
催化作用
法拉第效率
硫黄
化学
氧气
氧化还原
过氧化氢
产量(工程)
碳纤维
纳米技术
电化学
化学工程
材料科学
无机化学
物理化学
有机化学
电极
冶金
复合材料
复合数
工程类
作者
Xiao Zhou,Min Yuan,Changming Zhao,Cai Chen,Ming‐Kun Ke,Shan Xu,Jie-Jie Chen,Yuen Wu,Han‐Qing Yu
标识
DOI:10.1038/s41467-023-44585-1
摘要
Abstract Direct electrosynthesis of hydrogen peroxide (H 2 O 2 ) 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 H 2 O 2 selectivity and diminished H 2 O 2 yield induced by consecutive H 2 O 2 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 400 mA cm −2 and elevated accumulated H 2 O 2 concentrations (1358 mM) with remarkable Faradaic efficiencies. Both experimental results and theoretical simulations elucidate that S and O super-coordination directs a fraction of electrons from the main-group Pb sites to the coordinated oxygen atoms, consequently optimizing the *OOH binding energy and augmenting the 2e − oxygen reduction activity. This work unveils novel avenues for mitigating the production-depletion challenge in H 2 O 2 electrosynthesis through the rational design of main-group catalysts.
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