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231226s2024 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202309648
|2 doi
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|a pubmed24n1284.xml
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|a eng
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1 |
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|a Cao, Xueying
|e verfasserin
|4 aut
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|a Strong p-d Orbital Hybridization on Bismuth Nanosheets for High Performing CO2 Electroreduction
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|c 2024
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|a Text
|b txt
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|a ƒaComputermedien
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|a ƒa Online-Ressource
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|a Date Revised 08.02.2024
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2023 Wiley-VCH GmbH.
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|a Single-atom alloys (SAAs) show great potential for a variety of electrocatalytic reactions. However, the atomic orbital hybridization effect of SAAs on the electrochemical reactions is unclear yet. Herein, the in situ confinement of vanadium/molybdenum/tungsten atoms on bismuth nanosheet is shown to create SAAs with rich grain boundaries, respectively. With the detailed analysis of microstructure and composition, the strong p-d orbital hybridization between bismuth and vanadium enables the exceptional electrocatalytic performance for carbon dioxide (CO2 ) reduction with the Faradaic efficiency nearly 100% for C1 products in a wide potential range from -0.6 to -1.4 V, and a long-term electrolysis stability for 90 h. In-depth in situ investigations with theoretical computations reveal that the electron delocalization toward vanadium atoms via the p-d orbital hybridization evokes the bismuth active centers for efficient CO2 activation via the σ-donation of O-to-Bi, thus reduces protonation energy barriers for formate production. With such fundamental understanding, SAA electrocatalyst is employed to fabricated the solar-driven electrolytic cell of CO2 reduction and 5-hydroxymethylfurfural oxidation, achieving an outstanding 2,5-furandicarboxylic acid yield of 90.5%. This study demonstrates a feasible strategy to rationally design advanced SAA electrocatalysts via the basic principles of p-d orbital hybridization
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|a Journal Article
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|a atomic doping
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|a carbon dioxide reduction
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|a electrocatalysis
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| 650 |
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4 |
|a orbital hybridization
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1 |
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|a Tian, Yadong
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Ma, Jizhen
|e verfasserin
|4 aut
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| 700 |
1 |
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|a Guo, Weijian
|e verfasserin
|4 aut
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| 700 |
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|a Cai, Wenwen
|e verfasserin
|4 aut
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| 700 |
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|a Zhang, Jintao
|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 36(2024), 6 vom: 01. Feb., Seite e2309648
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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| 773 |
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|g volume:36
|g year:2024
|g number:6
|g day:01
|g month:02
|g pages:e2309648
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|u http://dx.doi.org/10.1002/adma.202309648
|3 Volltext
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