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

Xiao Zhou, Yuan Min, Changming Zhao, Cai Chen, Ming-Kun Ke, Shi-Lin Xu, Jie-Jie Chen, Yuen Wu () and Han-Qing Yu ()
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Xiao Zhou: University of Science and Technology of China
Yuan Min: University of Science and Technology of China
Changming Zhao: University of Science and Technology of China
Cai Chen: University of Science and Technology of China
Ming-Kun Ke: University of Science and Technology of China
Shi-Lin Xu: University of Science and Technology of China
Jie-Jie Chen: University of Science and Technology of China
Yuen Wu: University of Science and Technology of China
Han-Qing Yu: University of Science and Technology of China

Nature Communications, 2024, vol. 15, issue 1, 1-13

Abstract: Abstract 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 400 mA cm−2 and elevated accumulated H2O2 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 H2O2 electrosynthesis through the rational design of main-group catalysts.

Date: 2024
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DOI: 10.1038/s41467-023-44585-1

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