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dc.contributor.authorZhang, Xiaofei
dc.contributor.authorLiu, Haitao
dc.contributor.authorAn, Pengfei
dc.contributor.authorShi, Yanan
dc.contributor.authorHan, Jianyu
dc.contributor.authorYang, Zhongjie
dc.contributor.authorLong, Chang
dc.contributor.authorGuo, Jun
dc.contributor.authorZhao, Shenlong
dc.contributor.authorZhao, Kun
dc.contributor.authorYin, Huajie
dc.contributor.authorZheng, Lirong
dc.contributor.authorZhang, Binhao
dc.contributor.authorTang, Zhiyong
dc.contributor.authoret al.
dc.date.accessioned2020-07-10T01:01:27Z
dc.date.available2020-07-10T01:01:27Z
dc.date.issued2020
dc.identifier.issn2375-2548
dc.identifier.doi10.1126/sciadv.aaz4824
dc.identifier.urihttp://hdl.handle.net/10072/395302
dc.description.abstractCO2 cycloaddition with epoxides at low temperature and pressure has been broadly recognized as an ambitious but challenging goal, which requires the catalysts to have precisely controlled Lewis acid sites. Here, we demonstrate that both stereochemical environment and oxidation state of single cobalt active sites in cobalt tetraaminophthalocyanine [CoPc(NH2)4] are finely tuned via molecular engineering with 2,5-di-tert-butyl-1,4-benzoquinone (DTBBQ). Notably, DTBBQ incorporation not only enables formation of 5-nm-thick conjugated microporous polymer (CMP) nanosheets due to the steric hindrance effect of tert-butyl groups but also makes isolated cobalt sites with high oxidation state due to the presence of delocalized electron-withdrawing effect of alkene groups in DTBBQ via conjugated skeleton. Notably, when used as heterogeneous catalysts for CO2 cycloaddition with different epoxides, single cobalt active sites on the ultrathin CMP nanosheets exhibit unprecedentedly high activity and excellent stability under mild reaction conditions.
dc.description.peerreviewedYes
dc.languageEnglish
dc.language.isoeng
dc.publisherAmerican Association for the Advancement of Science (AAAS)
dc.relation.ispartofpagefromeaaz4824:1
dc.relation.ispartofpagetoeaaz4824:10
dc.relation.ispartofissue17
dc.relation.ispartofjournalScience Advances
dc.relation.ispartofvolume6
dc.subject.fieldofresearchEnvironmental sciences
dc.subject.fieldofresearchcode41
dc.subject.keywordsScience & Technology
dc.subject.keywordsMultidisciplinary Sciences
dc.subject.keywordsScience & Technology - Other Topics
dc.subject.keywordsHETEROGENEOUS CATALYST
dc.subject.keywordsCYCLIC CARBONATES
dc.titleDelocalized electron effect on single metal sites in ultrathin conjugated microporous polymer nanosheets for boosting CO2 cycloaddition
dc.typeJournal article
dc.type.descriptionC1 - Articles
dcterms.bibliographicCitationZhang, X; Liu, H; An, P; Shi, Y; Han, J; Yang, Z; Long, C; Guo, J; Zhao, S; Zhao, K; Yin, H; Zheng, L; Zhang, B; Liu, X; Zhang, L; Li, G; Tang, Z, Delocalized electron effect on single metal sites in ultrathin conjugated microporous polymer nanosheets for boosting CO2 cycloaddition, Science Advances, 2020, 6 (17), pp. eaaz4824:1-eaaz4824:10
dcterms.dateAccepted2020-01-24
dcterms.licensehttps://creativecommons.org/licenses/by-nc/4.0/
dc.date.updated2020-07-10T00:55:10Z
dc.description.versionVersion of Record (VoR)
gro.rights.copyright© 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S.Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC).
gro.hasfulltextFull Text
gro.griffith.authorTang, Zhiyong
gro.griffith.authorYin, Huajie


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