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Identification of the Highly Active Co–N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide

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Chen, Shanyong, Luo, Tao, Li, Xiaoqing, Chen, Kejun, Fu, Junwei, Liu, Kang, Cai, Chao, Wang, Qiyou, Li, Hongmei, Chen, Yu, Ma, Chao, Zhu, Li, Lu, Ying-Rui, Chan, Ting-Shan, Zhu, Mingshan, Cortés, Emiliano, Liu, Min·2022·Journal of the American Chemical Society

DOI 10.1021/jacs.2c01194

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Abstract

High Resolution Image Download MS PowerPoint Slide Electrosynthesis of hydrogen peroxide (H 2 O 2 ) through oxygen reduction reaction (ORR) is an environment-friendly and sustainable route for obtaining a fundamental product in the chemical industry. Co–N 4 single-atom catalysts (SAC) have sparkled attention for being highly active in both 2e – ORR, leading to H 2 O 2 and 4e – ORR, in which H 2 O is the main product. However, there is still a lack of fundamental insights into the structure–function relationship between CoN 4 and the ORR mechanism over this family of catalysts. Here, by combining theoretical simulation and experiments, we unveil that pyrrole-type CoN 4 (Co–N SAC Dp ) is mainly responsible for the 2e – ORR, while pyridine-type CoN 4 catalyzes the 4e – ORR. Indeed, Co–N SAC Dp exhibits a remarkable H 2 O 2 selectivity of 94% and a superb H 2 O 2 yield of 2032 mg for 90 h in a flow cell, outperforming most reported catalysts in acid media. Theoretical analysis and experimental investigations confirm that Co–N SAC Dp ─with weakening O 2 /HOO* interaction─boosts the H 2 O 2 production.

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See all 560

Authors: Chen, S., Luo, T., Li, X., Chen, K., Fu, J., Liu, K., Cai, C., Wang, Q., Li, H., Chen, Y., Ma, C., Zhu, L., Lu, Y.-R., Chan, T.-S., Zhu, M., Cortés, E., & Liu, M.
Venue: Journal of the American Chemical Society
Publisher: American Chemical Society (ACS)
Published: 2022-08-03
Volume: 144
Issue: 32
Pages: 14505-14516
ISSN: 0002-7863 (ISSN-L)
1520-5126
DOI: 10.1021/jacs.2c01194
OpenAlex: W4289711467
Cited by: 560
References: 62
FWCI: 19.76
Type: journal article
Language: en
Open access: hybrid

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Identification of the Highly Active Co–N4 Coordination Motif for Selective Oxygen Reduction to Hydrogen Peroxide

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