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231226s2023 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202300695
|2 doi
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|a pubmed25n1180.xml
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|a (DE-627)NLM354346652
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|a (NLM)36929182
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|a DE-627
|b ger
|c DE-627
|e rakwb
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|a eng
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| 100 |
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|a Wang, Qiyou
|e verfasserin
|4 aut
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|a Asymmetric Coordination Induces Electron Localization at Ca Sites for Robust CO2 Electroreduction to CO
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|c 2023
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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 Completed 25.05.2023
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|a Date Revised 25.05.2023
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2023 The Authors. Advanced Materials published by Wiley-VCH GmbH.
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|a Main group single atom catalysts (SACs) are promising for CO2 electroreduction to CO by virtue of their ability in preventing the hydrogen evolution reaction and CO poisoning. Unfortunately, their delocalized orbitals reduce the CO2 activation to *COOH. Herein, an O doping strategy to localize electrons on p-orbitals through asymmetric coordination of Ca SAC sites (Ca-N3 O) is developed, thus enhancing the CO2 activation. Theoretical calculations indicate that asymmetric coordination of Ca-N3 O improves electron-localization around Ca sites and thus promotes *COOH formation. X-ray absorption fine spectroscopy shows the obtained Ca-N3 O features: one O and three N coordinated atoms with one Ca as a reactive site. In situ attenuated total reflection infrared spectroscopy proves that Ca-N3 O promotes *COOH formation. As a result, the Ca-N3 O catalyst exhibits a state-of-the-art turnover frequency of ≈15 000 per hour in an H-cell and a large current density of -400 mA cm-2 with a CO Faradaic efficiency (FE) ≥ 90% in a flow cell. Moreover, Ca-N3 O sites retain a FE above 90% even with a 30% diluted CO2 concentration
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|a Journal Article
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|a CO2 electroreduction
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|a asymmetric coordination
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|a calcium
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|a electron localization
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|a p-orbital
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| 700 |
1 |
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|a Dai, Minyang
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Li, Hongmei
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Lu, Ying-Rui
|e verfasserin
|4 aut
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1 |
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|a Chan, Ting-Shan
|e verfasserin
|4 aut
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1 |
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|a Ma, Chao
|e verfasserin
|4 aut
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1 |
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|a Liu, Kang
|e verfasserin
|4 aut
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|a Fu, Junwei
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Liao, Wanru
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Chen, Shanyong
|e verfasserin
|4 aut
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1 |
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|a Pensa, Evangelina
|e verfasserin
|4 aut
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1 |
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|a Wang, Ye
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Zhang, Shiguo
|e verfasserin
|4 aut
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1 |
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|a Sun, Yifei
|e verfasserin
|4 aut
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|a Cortés, Emiliano
|e verfasserin
|4 aut
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| 700 |
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|a Liu, Min
|e verfasserin
|4 aut
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| 773 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 35(2023), 21 vom: 16. Mai, Seite e2300695
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnas
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| 773 |
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|g volume:35
|g year:2023
|g number:21
|g day:16
|g month:05
|g pages:e2300695
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|u http://dx.doi.org/10.1002/adma.202300695
|3 Volltext
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