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https://hdl.handle.net/2440/131257
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dc.contributor.author | Tang, C. | - |
dc.contributor.author | Chen, L. | - |
dc.contributor.author | Li, H. | - |
dc.contributor.author | Li, L. | - |
dc.contributor.author | Jiao, Y. | - |
dc.contributor.author | Zheng, Y. | - |
dc.contributor.author | Xu, H. | - |
dc.contributor.author | Davey, K. | - |
dc.contributor.author | Qiao, S. | - |
dc.date.issued | 2021 | - |
dc.identifier.citation | Journal of the American Chemical Society, 2021; 43(20):4819-4827 | - |
dc.identifier.issn | 0002-7863 | - |
dc.identifier.issn | 1520-5126 | - |
dc.identifier.uri | http://hdl.handle.net/2440/131257 | - |
dc.description.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. | - |
dc.description.statementofresponsibility | Cheng Tang, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth Davey, and Shi-Zhang Qiao | - |
dc.language.iso | en | - |
dc.publisher | American Chemical Society (ACS) | - |
dc.rights | © 2021 American Chemical Society | - |
dc.source.uri | http://dx.doi.org/10.1021/jacs.1c03135 | - |
dc.title | Tailoring acidic oxygen reduction selectivity on single-atom catalysts via modification of first and second coordination spheres | - |
dc.type | Journal article | - |
dc.identifier.doi | 10.1021/jacs.1c03135 | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/FL170100154 | - |
dc.relation.grant | http://purl.org/au-research/grants/arc/DE190100636 | - |
pubs.publication-status | Published | - |
dc.identifier.orcid | Tang, C. [0000-0002-5167-1192] | - |
dc.identifier.orcid | Chen, L. [0000-0002-8898-5769] | - |
dc.identifier.orcid | Li, L. [0000-0002-3301-9029] | - |
dc.identifier.orcid | Jiao, Y. [0000-0003-1329-4290] | - |
dc.identifier.orcid | Zheng, Y. [0000-0002-2411-8041] | - |
dc.identifier.orcid | Davey, K. [0000-0002-7623-9320] | - |
dc.identifier.orcid | Qiao, S. [0000-0002-1220-1761] [0000-0002-4568-8422] | - |
Appears in Collections: | Aurora harvest 8 Chemical Engineering publications |
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