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240916s2024 xx |||||o 00| ||eng c |
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|a 10.1002/adma.202410125
|2 doi
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|a pubmed24n1587.xml
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|a (DE-627)NLM377630314
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|a (NLM)39267437
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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 Wang, Ting
|e verfasserin
|4 aut
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|a Ni-Electrocatalytic CO2 Reduction Toward Ethanol
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|c 2024
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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
|b cr
|2 rdacarrier
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|a Date Revised 01.11.2024
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|a published: Print-Electronic
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|a Citation Status PubMed-not-MEDLINE
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|a © 2024 Wiley‐VCH GmbH.
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|a The electroreduction of CO2 offers a sustainable route to generate synthetic fuels. Cu-based catalysts have been developed to produce value-added C2+ alcohols; however, the limited understanding of complex C-C coupling and reaction pathway hinders the development of efficient CO2-to-C2+ alcohols catalysts. Herein, a Cu-free, highly mesoporous NiO catalyst, derived from the microphase separation of a block copolymer, is reported, which achieves selective CO2 reduction toward ethanol with a Faradaic efficiency of 75.2% at -0.6 V versus RHE. The dense mesopores create a favorable local reaction environment with CO2-rich and H2O-deficient interfaces, suppressing hydrogen evolution and maximizing catalytic activity of NiO for CO2 reduction. Importantly, the C1-feeding experiments, in situ spectroscopy, and theoretical calculations consistently show that the direct coupling of *CO2 and *COOH is responsible for C-C bond formation on NiO, and subsequent reduction of *CO2-COOH to ethanol is energetically facile through the *COCOH and *OC2H5 pathway. The unconventional C-C coupling mechanism on NiO, in contrast to the *CO dimerization on Cu, is triggered by strong CO2 adsorption on the polarized Ni2+-O2- sites. The work not only demonstrates a highly selective Cu-free Ni-based alternative for CO2-to-C2+ alcohols transformation but also provides a new perspective on C-C coupling toward C2+ synthesis
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|a Journal Article
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|a CO2 reduction
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|a C−C coupling
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|a Ni‐based catalyst
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|a catalytic mechanism
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|a ethanol
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|a Duan, Xinyi
|e verfasserin
|4 aut
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1 |
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|a Bai, Rui
|e verfasserin
|4 aut
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1 |
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|a Li, Haoyang
|e verfasserin
|4 aut
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|a Qin, Chen
|e verfasserin
|4 aut
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1 |
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|a Zhang, Jian
|e verfasserin
|4 aut
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1 |
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|a Duan, Zhiyao
|e verfasserin
|4 aut
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1 |
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|a Chen, Kai-Jie
|e verfasserin
|4 aut
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1 |
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|a Pan, Fuping
|e verfasserin
|4 aut
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773 |
0 |
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|i Enthalten in
|t Advanced materials (Deerfield Beach, Fla.)
|d 1998
|g 36(2024), 44 vom: 01. Nov., Seite e2410125
|w (DE-627)NLM098206397
|x 1521-4095
|7 nnns
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|g volume:36
|g year:2024
|g number:44
|g day:01
|g month:11
|g pages:e2410125
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|u http://dx.doi.org/10.1002/adma.202410125
|3 Volltext
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