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dc.contributor.authorYao, Xiangdong
dc.contributor.authorLi, Daohao
dc.contributor.authorWang, Binbin
dc.contributor.authorLong, Xiaojing
dc.contributor.authorXu, Wenjia
dc.contributor.authorXia, Yanzhi
dc.contributor.authorYang, Dongjiang
dc.date.accessioned2021-10-18T06:08:28Z
dc.date.available2021-10-18T06:08:28Z
dc.date.issued2021
dc.identifier.issn1433-7851
dc.identifier.doi10.1002/anie.202109057
dc.identifier.urihttp://hdl.handle.net/10072/409189
dc.description.abstractActive center reconstruction is essential for searching high performance oxygen reduction reaction (ORR) electrocatalysts. Usually, the ORR activity stems from the special electronic environment of active sites through charge redistribution. In this work, we introduce "asymmetry" strategy to adjust the charge distribution of active centers by precisely designing conjugated polymer (CP) catalysts with different degrees of asymmetry. We synthesized asymmetric backbone CP ( asy-PB ) by modifying boron-nitrogen coordination bonds (B←N) and asymmetric sidechain CP ( asy-PB-A ) with different alkyl chain lengths. As a result, both CPs with backbone and sidechain asymmetry exhibit superior ORR performance to their symmetric counterparts ( sy-P and sy-PB ). Interestingly, asy-PB with greater asymmetry degree shows higher catalytic activity than asy-PB-A with relatively smaller asymmetry. Density functional theory calculations reveal that the increased dipole moment and non-uniform charge distribution caused by asymmetric structure endows the center carbon atom of bipyridine with efficient catalytic activity. These findings provide a mechanistic understanding of asymmetric ORR active structures and this approach gives a new strategy to design high-performance non-metal electrocatalysts.
dc.description.peerreviewedYes
dc.languageeng
dc.publisherWiley
dc.relation.ispartofjournalAngewandte Chemie International Edition
dc.subject.fieldofresearchAnalytical chemistry
dc.subject.fieldofresearchcode3401
dc.subject.keywordsasymmetric structure · heterocycles · linear conjugated polymer · electrocatalysis · oxygen reduction reaction
dc.titleControlled Asymmetric Charge Distribution of Active Centers in Conjugated Polymers for Oxygen Reduction
dc.typeJournal article
dc.type.descriptionC1 - Articles
dcterms.bibliographicCitationYao, X; Li, D; Wang, B; Long, X; Xu, W; Xia, Y; Yang, D, Controlled Asymmetric Charge Distribution of Active Centers in Conjugated Polymers for Oxygen Reduction, Angewandte Chemie International Edition, 2021
dcterms.dateAccepted2021-09-21
dc.date.updated2021-10-14T00:28:54Z
dc.description.versionAccepted Manuscript (AM)
gro.description.notepublicThis publication has been entered as an advanced online version in Griffith Research Online.
gro.rights.copyright© 2021 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. This is the peer reviewed version of the following article: Controlled Asymmetric Charge Distribution of Active Centers in Conjugated Polymers for Oxygen Reduction, Angewandte Chemie, International Edition, 2021, which has been published in final form at https://doi.org/10.1002/anie.202109057. This article may be used for non-commercial purposes in accordance with Wiley Terms and Conditions for Self-Archiving (http://olabout.wiley.com/WileyCDA/Section/id-828039.html)
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gro.griffith.authorYao, Xiangdong


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