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Type: Journal article
Title: Tailoring acidic oxygen reduction selectivity on single-atom catalysts via modification of first and second coordination spheres
Author: Tang, C.
Chen, L.
Li, H.
Li, L.
Jiao, Y.
Zheng, Y.
Xu, H.
Davey, K.
Qiao, S.
Citation: Journal of the American Chemical Society, 2021; 43(20):4819-4827
Publisher: American Chemical Society (ACS)
Issue Date: 2021
ISSN: 0002-7863
Statement of
Cheng Tang, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth Davey, and Shi-Zhang Qiao
Abstract: Product selectivity in multielectron electrocatalytic reactions is crucial to energy conversion efficiency and chemical production. However, a present practical drawback is the limited understanding of actual catalytic active sites. Here, using as a prototype single-atom catalysts (SACs) in acidic oxygen reduction reaction (ORR), we report the structure–property relationship of catalysts and show for the first time that molecular-level local structure, including first and second coordination spheres (CSs), rather than individual active atoms, synergistically determines the electrocatalytic response. ORR selectivity on Co-SACs can be tailored from a four-electron to a two-electron pathway by modifying first (N or/and O coordination) and second (C–O–C groups) CSs. Using combined theoretical predictions and experiments, including X-ray absorption fine structure analyses and in situ infrared spectroscopy, we confirm that the unique selectivity change originates from the structure-dependent shift of active sites from the center Co atom to the O-adjacent C atom. We show this optimizes the electronic structure and *OOH adsorption behavior on active sites to give the present “best” activity and selectivity of >95% for acidic H₂O₂ electrosynthesis.
Rights: © 2021 American Chemical Society
DOI: 10.1021/jacs.1c03135
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Chemical Engineering publications

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