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

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 () and Guanjie He ()
Additional contact information
Longxiang Liu: University College London
Liqun Kang: Max-Planck-Institute for Chemical Energy Conversion
Jianrui Feng: University College London
David G. Hopkinson: Harwell Science and Innovation Campus
Christopher S. Allen: Harwell Science and Innovation Campus
Yeshu Tan: University College London
Hao Gu: University College London
Iuliia Mikulska: Harwell Science and Innovation Campus
Veronica Celorrio: Harwell Science and Innovation Campus
Diego Gianolio: Harwell Science and Innovation Campus
Tianlei Wang: University College London
Liquan Zhang: University College London
Kaiqi Li: University College London
Jichao Zhang: University College London
Jiexin Zhu: University College London
Georg Held: Harwell Science and Innovation Campus
Pilar Ferrer: Harwell Science and Innovation Campus
David Grinter: Harwell Science and Innovation Campus
June Callison: Rutherford Appleton Laboratory
Martin Wilding: Rutherford Appleton Laboratory
Sining Chen: University College London
Ivan Parkin: University College London
Guanjie He: University College London

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-48209-0

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