Issue 15, 2024

Isolated cobalt–nitrogen sites on high-curvature carbon achieving industrial-level current density and pH-universal CO2 electroreduction

Abstract

Achieving industrial-level current density and pH-universal CO2 reduction using single atom catalysts is a significant but challenging task. In this work, we demonstrate that isolated cobalt–nitrogen sites supported on high-curvature carbon could achieve industrial-level current density and pH-universal CO2 electroreduction to CO. In an H-type cell, the catalyst achieves a remarkable maximum CO faradaic efficiency of 98.2%, while maintaining CO faradaic efficiency above 90% over a wide potential window from −0.4 to −1.4 V vs. RHE. In a gas-diffusion flow cell, the CO faradaic efficiency could reach 98.9%, 96.5% and 98.6% in alkaline, acidic and neutral electrolytes, respectively. Impressively, the CO current density could reach 437, 337 and 367 mA cm−2, exceeding industrial-level current density requirements. In situ characterization studies coupled with theoretical calculations reveal that compared with the planar cobalt–nitrogen structure, the curved cobalt–nitrogen structure could effectively activate CO2, facilitate *COOH formation and inhibit the hydrogen evolution reaction, thus affording high activity, selectivity and pH-universal feasibility.

Graphical abstract: Isolated cobalt–nitrogen sites on high-curvature carbon achieving industrial-level current density and pH-universal CO2 electroreduction

Supplementary files

Article information

Article type
Paper
Submitted
16 Nov 2023
Accepted
04 Mar 2024
First published
05 Mar 2024

J. Mater. Chem. A, 2024,12, 9147-9154

Isolated cobalt–nitrogen sites on high-curvature carbon achieving industrial-level current density and pH-universal CO2 electroreduction

J. Wang, X. Chen, Z. Yang, J. Xiao, C. Qin, Z. Yan, Z. Wang, J. Yang and J. Wang, J. Mater. Chem. A, 2024, 12, 9147 DOI: 10.1039/D3TA07074C

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