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Tailoring acidic oxygen reduction selectivity on single-atom catalysts via modification of first and second coordination spheres

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dc.contributor.authorTang, C.
dc.contributor.authorChen, L.
dc.contributor.authorLi, H.
dc.contributor.authorLi, L.
dc.contributor.authorJiao, Y.
dc.contributor.authorZheng, Y.
dc.contributor.authorXu, H.
dc.contributor.authorDavey, K.
dc.contributor.authorQiao, S.
dc.date.issued2021
dc.description.abstractProduct 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.statementofresponsibilityCheng Tang, Ling Chen, Haijing Li, Laiquan Li, Yan Jiao, Yao Zheng, Haolan Xu, Kenneth Davey, and Shi-Zhang Qiao
dc.identifier.citationJournal of the American Chemical Society, 2021; 43(20):4819-4827
dc.identifier.doi10.1021/jacs.1c03135
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.orcidTang, C. [0000-0002-5167-1192]
dc.identifier.orcidChen, L. [0000-0002-8898-5769]
dc.identifier.orcidLi, L. [0000-0002-3301-9029]
dc.identifier.orcidJiao, Y. [0000-0003-1329-4290]
dc.identifier.orcidZheng, Y. [0000-0002-2411-8041]
dc.identifier.orcidXu, H. [0000-0002-9126-1593]
dc.identifier.orcidDavey, K. [0000-0002-7623-9320]
dc.identifier.orcidQiao, S. [0000-0002-1220-1761] [0000-0002-4568-8422]
dc.identifier.urihttp://hdl.handle.net/2440/131257
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.granthttp://purl.org/au-research/grants/arc/FL170100154
dc.relation.granthttp://purl.org/au-research/grants/arc/DE190100636
dc.rights© 2021 American Chemical Society
dc.source.urihttps://doi.org/10.1021/jacs.1c03135
dc.subjectoxygen reduction
dc.subjectenergy conversion
dc.subjectchemical production
dc.titleTailoring acidic oxygen reduction selectivity on single-atom catalysts via modification of first and second coordination spheres
dc.typeJournal article
pubs.publication-statusPublished

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