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

作者：Xiao Zhou, Yuan Min, Changming Zhao, Cai Chen, Ming‐Kun Ke, Shilin Xu, Jie‐Jie Chen, Yuen Wu, Han‐Qing Yu · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-023-44585-1 · 被引用次数：124 · 研究领域：Electrocatalysts for Energy Conversion、Advanced battery technologies research、Advanced Photocatalysis Techniques

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.