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dc.contributor.authorLei, Qiong
dc.contributor.authorZhu, Hui
dc.contributor.authorSong, Kepeng
dc.contributor.authorWei, Nini
dc.contributor.authorLiu, Lingmei
dc.contributor.authorZhang, Daliang
dc.contributor.authorYin, Jun
dc.contributor.authorDong, Xinglong
dc.contributor.authorYao, Kexin
dc.contributor.authorWang, Ning
dc.contributor.authorLi, Xinghua
dc.contributor.authorDavaasuren, Bambar
dc.contributor.authorWang, Jianjian
dc.contributor.authorHan, Yu
dc.date.accessioned2020-02-16T11:53:32Z
dc.date.available2020-02-16T11:53:32Z
dc.date.issued2020-02-10
dc.identifier.citationLei, Q., Zhu, H., Song, K., Wei, N., Liu, L., Zhang, D., … Han, Y. (2020). Investigating the Origin of Enhanced C2+ Selectivity in Oxide-/Hydroxide-derived Copper Electrodes during CO2 Electroreduction. Journal of the American Chemical Society. doi:10.1021/jacs.9b11790
dc.identifier.doi10.1021/jacs.9b11790
dc.identifier.urihttp://hdl.handle.net/10754/661538
dc.description.abstractOxide-/hydroxide-derived copper electrodes exhibit excellent selectivity toward C2+ products during electrocatalytic CO2 reduction reaction (CO2RR). However, the origin of such enhanced selectivity remains controversial. Here, we prepared two Cu-based electrodes with mixed oxidation states, namely HQ-Cu (containing Cu, Cu2O, CuO) and AN-Cu (containing Cu, Cu(OH)2). We extracted ultra-thin specimen from the electrodes using a focused ion beam to investigate the distribu-tion and evolution of various Cu species by electron microscopy and electron energy loss spectroscopy. We found that at the steady stage of CO2RR, the electrodes have all been reduced to Cu0, regardless of the initial states, suggesting that the high C2+ selectivities are not associated with specific oxidation states of Cu. We verified this conclusion by control experi-ments, in which HQ-Cu and AN-Cu were pretreated to fully reduce oxides/hydroxides to Cu0, and the pretreated elec-trodes showed even higher C2+ selectivity, compared with their un-pretreated counterparts. We observed that the ox-ide/hydroxide crystals in HQ-Cu and AN-Cu were fragmented into nano-sized irregular Cu grains under the applied nega-tive potentials. Such a fragmentation process, which is the consequence of an oxidation-reduction cycle and does not oc-cur in electropolished Cu, not only built an intricate network of grain boundaries, but also exposed a variety of high-index facets. These two features greatly facilitated the C-C coupling, thus accounting for the enhanced C2+ selectivity. Our work demonstrates that the use of advanced characterization techniques enables investigating the structural and chemical states of electrodes in unprecedented detail, to gain new insights into a widely studied system.
dc.description.sponsorshipThe financial support for this work was provided by Baseline Funds (BAS/1/1372-01-01) to Y.H. from King Abdullah University of Science and Technology. This research used resources of the Core Labs of King Abdullah University of Science and Technology.
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttps://pubs.acs.org/doi/10.1021/jacs.9b11790
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of the American Chemical Society, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://pubs.acs.org/doi/10.1021/jacs.9b11790.
dc.titleInvestigating the Origin of Enhanced C2+ Selectivity in Oxide-/Hydroxide-derived Copper Electrodes during CO2 Electroreduction
dc.typeArticle
dc.contributor.departmentAdvanced Membranes and Porous Materials Research Center
dc.contributor.departmentChemical Science Program
dc.contributor.departmentElectron Microscopy
dc.contributor.departmentNanostructured Functional Materials (NFM) laboratory
dc.contributor.departmentPhysical Characterization
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalJournal of the American Chemical Society
dc.rights.embargodate2021-02-11
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionMulti-scale Porous Materials Center, Institute of Advanced Interdisciplinary Studies, & School of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, P. R. China.
kaust.personLei, Qiong
kaust.personZhu, Hui
kaust.personSong, Kepeng
kaust.personWei, Nini
kaust.personLiu, Lingmei
kaust.personYin, Jun
kaust.personDong, Xinglong
kaust.personDong, Xinglong
kaust.personWang, Ning
kaust.personLi, Xinghua
kaust.personDavaasuren, Bambar
kaust.personHan, Yu
kaust.personHan, Yu
dc.date.accepted2020-02-10
refterms.dateFOA2020-02-16T13:05:03Z
dc.date.published-online2020-02-10
dc.date.published-print2020-03-04


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