Promoting Dinuclear-Type Catalysis in Cu1 -C3 N4 Single-Atom Catalysts

© 2022 Wiley-VCH GmbH.

Détails bibliographiques
Publié dans:Advanced materials (Deerfield Beach, Fla.). - 1998. - 34(2022), 33 vom: 11. Aug., Seite e2204638
Auteur principal: Song, Jingting (Auteur)
Autres auteurs: Chen, Zhongxin, Cai, Xiangbin, Zhou, Xin, Zhan, Gaolei, Li, Runlai, Wei, Pingping, Yan, Ning, Xi, Shibo, Loh, Kian Ping
Format: Article en ligne
Langue:English
Publié: 2022
Accès à la collection:Advanced materials (Deerfield Beach, Fla.)
Sujets:Journal Article 1,3-dipolar cycloaddition dinuclear-type catalysis next-nearest distance ultrahigh-loading single-atom catalysts
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520 |a Reducing particle size in supported metal catalysts to single-atom level isolates the active metal sites and maximizes the atomic utilization efficiency. However, the large inter-atom distance, particularly in low-loading single-atom catalyst (SAC), is not favorable for a complex reaction where two (or more) reactants have to be activated. A key question is how to control the inter-atom distances to promote dinuclear-type coactivation at the adjacent metal sites. Here, it is reported that reducing the average inter-atom distance of copper SACs supported on carbon nitride (C3 N4 ) to 0.74 ± 0.13 nm allows these catalysts to exhibit a dinuclear-type catalytic mechanism in the nitrile-azide cycloaddition. Operando X-ray absorption fine structure study reveals a dynamic ligand exchange process between nitrile and azide, followed by their coactivation on dinuclear Cu SAC sites to form the tetrazole product. This work highlights that reducing the nearest-neighbor distance of SAC allows the mechanistic pathway to diversify from single-site to multisite catalysis 
650 4 |a Journal Article 
650 4 |a 1,3-dipolar cycloaddition 
650 4 |a dinuclear-type catalysis 
650 4 |a next-nearest distance 
650 4 |a ultrahigh-loading single-atom catalysts 
700 1 |a Chen, Zhongxin  |e verfasserin  |4 aut 
700 1 |a Cai, Xiangbin  |e verfasserin  |4 aut 
700 1 |a Zhou, Xin  |e verfasserin  |4 aut 
700 1 |a Zhan, Gaolei  |e verfasserin  |4 aut 
700 1 |a Li, Runlai  |e verfasserin  |4 aut 
700 1 |a Wei, Pingping  |e verfasserin  |4 aut 
700 1 |a Yan, Ning  |e verfasserin  |4 aut 
700 1 |a Xi, Shibo  |e verfasserin  |4 aut 
700 1 |a Loh, Kian Ping  |e verfasserin  |4 aut 
773 0 8 |i Enthalten in  |t Advanced materials (Deerfield Beach, Fla.)  |d 1998  |g 34(2022), 33 vom: 11. Aug., Seite e2204638  |w (DE-627)NLM098206397  |x 1521-4095  |7 nnas 
773 1 8 |g volume:34  |g year:2022  |g number:33  |g day:11  |g month:08  |g pages:e2204638 
856 4 0 |u http://dx.doi.org/10.1002/adma.202204638  |3 Volltext 
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