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.

The relationship between the structural configurations of M-N-C electrocatalysts and their performances in neutral environments has been insufficiently investigated. Here the authors demonstrate that an ultralow metal-loaded Co-N-C electrocatalyst, featuring the asymmetric Co-C/N/O configuration, exhibit exceptional efficiency in electrochemically producing hydrogen peroxide under neutral conditions.

Details

Title
Atomically dispersed asymmetric cobalt electrocatalyst for efficient hydrogen peroxide production in neutral media
Author
Liu, Longxiang 1 ; Kang, Liqun 2   VIAFID ORCID Logo  ; Feng, Jianrui 1 ; Hopkinson, David G. 3   VIAFID ORCID Logo  ; Allen, Christopher S. 4 ; Tan, Yeshu 1 ; Gu, Hao 5 ; Mikulska, Iuliia 6   VIAFID ORCID Logo  ; Celorrio, Veronica 6   VIAFID ORCID Logo  ; Gianolio, Diego 6   VIAFID ORCID Logo  ; Wang, Tianlei 1 ; Zhang, Liquan 1 ; Li, Kaiqi 1 ; Zhang, Jichao 1 ; Zhu, Jiexin 1 ; Held, Georg 6   VIAFID ORCID Logo  ; Ferrer, Pilar 6   VIAFID ORCID Logo  ; Grinter, David 6   VIAFID ORCID Logo  ; Callison, June 7   VIAFID ORCID Logo  ; Wilding, Martin 7   VIAFID ORCID Logo  ; Chen, Sining 1 ; Parkin, Ivan 1   VIAFID ORCID Logo  ; He, Guanjie 1   VIAFID ORCID Logo 

 University College London, Christopher Ingold Laboratory, Department of Chemistry, London, UK (GRID:grid.83440.3b) (ISNI:0000 0001 2190 1201) 
 Max-Planck-Institute for Chemical Energy Conversion, Department of Inorganic Spectroscopy, Mülheim an der Ruhr, Germany (GRID:grid.419576.8) (ISNI:0000 0004 0491 861X) 
 Harwell Science and Innovation Campus, Electron Physical Science Imaging Centre, Diamond Light Source, Didcot, UK (GRID:grid.18785.33) (ISNI:0000 0004 1764 0696) 
 Harwell Science and Innovation Campus, Electron Physical Science Imaging Centre, Diamond Light Source, Didcot, UK (GRID:grid.18785.33) (ISNI:0000 0004 1764 0696); University of Oxford, Department of Materials, Oxford, UK (GRID:grid.4991.5) (ISNI:0000 0004 1936 8948) 
 University College London, Department of Chemical Engineering, London, UK (GRID:grid.83440.3b) (ISNI:0000 0001 2190 1201) 
 Harwell Science and Innovation Campus, Diamond Light Source, Didcot, UK (GRID:grid.18785.33) (ISNI:0000 0004 1764 0696) 
 Rutherford Appleton Laboratory, UK Catalysis Hub, Research Complex at Harwell, Didcot, UK (GRID:grid.76978.37) (ISNI:0000 0001 2296 6998) 
Pages
4079
Publication year
2024
Publication date
2024
Publisher
Nature Publishing Group
e-ISSN
20411723
Source type
Scholarly Journal
Language of publication
English
ProQuest document ID
3054660876
Copyright
© The Author(s) 2024. This work is published under http://creativecommons.org/licenses/by/4.0/ (the “License”). Notwithstanding the ProQuest Terms and Conditions, you may use this content in accordance with the terms of the License.