%X Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e- ORR) provides a promising alternative to replace the energy-intensive anthraquinone process. M-N-C electrocatalysts, which consist of atomically dispersed transition metals and nitrogen-doped carbon, have demonstrated considerable EHPP efficiency. However, their full potential, particularly regarding the correlation between structural configurations and performances in neutral media, remains underexplored. Herein, a series of ultralow metal-loading M-N-C electrocatalysts are synthesized and investigated for the EHPP process in the neutral electrolyte. CoNCB material with the asymmetric Co-C/N/O configuration exhibits the highest EHPP activity and selectivity among various as-prepared M-N-C electrocatalyst, with an outstanding mass activity (6.1 × 105 A gCo-1 at 0.5 V vs. RHE), and a high practical H2O2 production rate (4.72 mol gcatalyst-1 h-1 cm-2). Compared with the popularly recognized square-planar symmetric Co-N4 configuration, the superiority of asymmetric Co-C/N/O configurations is elucidated by X-ray absorption fine structure spectroscopy analysis and computational studies.
%K Electrocatalysis, Synthesis and processing
%V 15
%A Longxiang Liu
%A Liqun Kang
%A Jianrui Feng
%A David G Hopkinson
%A Christopher S Allen
%A Yeshu Tan
%A Hao Gu
%A Iuliia Mikulska
%A Veronica Celorrio
%A Diego Gianolio
%A Tianlei Wang
%A Liquan Zhang
%A Kaiqi Li
%A Jichao Zhang
%A Jiexin Zhu
%A Georg Held
%A Pilar Ferrer
%A David Grinter
%A June Callison
%A Martin Wilding
%A Sining Chen
%A Ivan Parkin
%A Guanjie He
%J Nature Communications
%C England
%N 1
%I Springer Science and Business Media LLC
%L discovery10192479
%D 2024
%O This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
%T Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media