Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media

Electrochemical hydrogen peroxide (H2O2) production (EHPP) via a two-electron oxygen reduction reaction (2e ORR) offers a promising alternative to the energy-intensive anthraquinone process. M-N-C electrocatalysts, featuring atomically dispersed transition metals and nitrogen-doped carbon, show significant EHPP efficiency. However, their full potential, especially the correlation between structural configurations and performance in neutral media, remains largely unexplored. This study synthesizes and investigates a series of ultralow metal-loading M-N-C electrocatalysts for EHPP in neutral electrolytes. CoNCB, exhibiting an asymmetric Co-C/N/O configuration, shows the highest EHPP activity and selectivity, with exceptional mass activity (6.1 × 10⁵ A gCo⁻¹ at 0.5 V vs. RHE) and H2O2 production rate (4.72 molcatalyst⁻¹ h⁻¹ cm⁻²). X-ray absorption fine structure spectroscopy and computational studies reveal the superiority of asymmetric Co-C/N/O over the common square-planar symmetric Co-N₄ configuration.

Longxiang Liu, Liqun Kang, Jianrui Feng, David G. Hopkinson, Christopher S. Allen, Yeshu Tan, Hao Gu, Iuliia Mikulska, Veronica Celorrio, Diego Gianolio, Tianlei Wang, Liquan Zhang, Kaiqi Li, Jichao Zhang, Jiexin Zhu, Georg Held, Pilar Ferrer, David Grinter, June Callison, Martin Wilding, Sining Chen, Ivan Parkin, Guanjie He