Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis

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Sun, Ji Wei
Wu, Xuefeng
Liu, Peng Fei
Chen, Jiacheng
Liu, Yuanwei
Lou, Zhen Xin
Zhao, Jia Yue
Yuan, Hai Yang
Chen, Aiping
Wang, Xue Lu
Zhu, Minghui
Dai, Sheng
Yang, Hua Gui
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2023
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http://creativecommons.org/licenses/by/4.0/
Abstract

Practical electrochemical CO2-to-CO conversion requires a non-precious catalyst to react at high selectivity and high rate. Atomically dispersed, coordinatively unsaturated metal-nitrogen sites have shown great performance in CO2 electroreduction; however, their controllable and large-scale fabrication still remains a challenge. Herein, we report a general method to fabricate coordinatively unsaturated metal-nitrogen sites doped within carbon nanotubes, among which cobalt single-atom catalysts can mediate efficient CO2-to-CO formation in a membrane flow configuration, achieving a current density of 200 mA cm−2 with CO selectivity of 95.4% and high full-cell energy efficiency of 54.1%, outperforming most of CO2-to-CO conversion electrolyzers. By expanding the cell area to 100 cm2, this catalyst sustains a high-current electrolysis at 10 A with 86.8% CO selectivity and the single-pass conversion can reach 40.4% at a high CO2 flow rate of 150 sccm. This fabrication method can be scaled up with negligible decay in CO2-to-CO activity. In situ spectroscopy and theoretical results reveal the crucial role of coordinatively unsaturated metal-nitrogen sites, which facilitate CO2 adsorption and key *COOH intermediate formation.

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Nature Communications
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14
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© The Author(s) 2023. 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 license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license 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 license, visit http://creativecommons.org/licenses/by/4.0/.
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Electrochemistry
Science & Technology
Multidisciplinary Sciences
Science & Technology - Other Topics
INITIO MOLECULAR-DYNAMICS
TOTAL-ENERGY CALCULATIONS
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Sun, JW; Wu, X; Liu, PF; Chen, J; Liu, Y; Lou, ZX; Zhao, JY; Yuan, HY; Chen, A; Wang, XL; Zhu, M; Dai, S; Yang, HG, Scalable synthesis of coordinatively unsaturated metal-nitrogen sites for large-scale CO2 electrolysis, Nature Communications, 2023, 14, pp. 1599
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