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231226s2022 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202204638
|2 doi
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|a pubmed25n1142.xml
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|a (DE-627)NLM342692623
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|a (NLM)35748197
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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|a Song, Jingting
|e verfasserin
|4 aut
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|a Promoting Dinuclear-Type Catalysis in Cu1 -C3 N4 Single-Atom Catalysts
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|c 2022
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|a Text
|b txt
|2 rdacontent
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|a ƒaComputermedien
|b c
|2 rdamedia
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|a ƒa Online-Ressource
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|2 rdacarrier
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|a Date Revised 18.08.2022
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2022 Wiley-VCH GmbH.
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|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
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|a Journal Article
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|a 1,3-dipolar cycloaddition
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|a dinuclear-type catalysis
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|a next-nearest distance
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|a ultrahigh-loading single-atom catalysts
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|a Chen, Zhongxin
|e verfasserin
|4 aut
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1 |
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|a Cai, Xiangbin
|e verfasserin
|4 aut
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1 |
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|a Zhou, Xin
|e verfasserin
|4 aut
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1 |
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|a Zhan, Gaolei
|e verfasserin
|4 aut
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1 |
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|a Li, Runlai
|e verfasserin
|4 aut
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1 |
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|a Wei, Pingping
|e verfasserin
|4 aut
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|a Yan, Ning
|e verfasserin
|4 aut
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|a Xi, Shibo
|e verfasserin
|4 aut
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|a Loh, Kian Ping
|e verfasserin
|4 aut
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|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
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|g volume:34
|g year:2022
|g number:33
|g day:11
|g month:08
|g pages:e2204638
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|u http://dx.doi.org/10.1002/adma.202204638
|3 Volltext
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