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  The Role of the Copper Oxidation State in the Electrocatalytic Reduction of CO2 into Valuable Hydrocarbons

Velasco Vélez, J., Jones, T., Gao, D., Carbonio, E., Arrigo, R., Hsu, C.-J., et al. (2019). The Role of the Copper Oxidation State in the Electrocatalytic Reduction of CO2 into Valuable Hydrocarbons. ACS Sustainable Chemistry & Engineering, 7(1), 1485-1492. doi:10.1021/acssuschemeng.8b05106.

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 Creators:
Velasco Vélez, Juan1, 2, Author              
Jones, Travis1, Author              
Gao, Dunfeng3, 4, Author              
Carbonio, Emilia1, Author              
Arrigo, Rosa5, 6, Author
Hsu, Cheng-Jhih7, Author
Huang, Yu-Cheng7, 8, Author
Dong, Chung Li7, Author
Chen, Jin-Ming8, Author
Lee, Jyh-Fu8, Author
Strasser, Peter9, Author
Roldan Cuenya, Beatriz3, 4, Author              
Schlögl, Robert1, 2, Author              
Knop-Gericke, Axel1, 2, Author              
Chuang, Cheng-Hao 7, Author
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Heterogeneous Reactions, Max-Planck-Institute for Chemical Energy Conversion , Stiftstr. 34 - 36 45470 Mülheim an der Ruhr, Germany, ou_persistent13              
3Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
4Department of Physics, Ruhr-University Bochum, ou_persistent22              
5Diamond Light source Ltd., Harwell Science & Innovation Campus, Didcot, Oxfordshire OX 11 0DE, UK, ou_persistent22              
6School of Environment and Life Sciencesm, University of Salford, Cockcroft building, M5 4WT, Manchester, UK, ou_persistent22              
7Department of Physics, Tamkang University, No. 151 ,Yingzhuan Rd., Danshui Dist, New Taipei City 25137, Taiwan, ou_persistent22              
8National Synchrotron Radiation Research Center, No. 101, Hsin Ann Rr., East District., Hsinchu 30076, Taiwan, ou_persistent22              
9Department of Chemistry, Technical University Berlin, Straße des 17., Berlin, Germany, ou_persistent22              

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 Abstract: Redox-active copper catalysts with accurately prepared oxidation states (Cu0, Cu+ and Cu2+) and high selectivity to C2 hydrocarbon formation, from electrocatalytic cathodic reduction of CO2, were fabricated and characterized. The electrochemically prepared copper-redox electro-cathodes yield higher activity for the production of hydrocarbons at lower oxidation state. By combining advanced X-ray spectroscopy and in situ micro-reactors it was possible to unambiguously reveal the variation in the complex electronic structure that the catalysts undergo at different stages (i.e. during fabrication and electrocatalytic reactions). It was found that the surface, sub-surface and bulk properties of the electrochemically prepared catalysts are dominated by the formation of copper carbonates on the surface of cupric-like oxides, which prompts catalyst deactivation by restraining effective charge transport. Furthermore, the formation of reduced or partially-reduced copper catalysts yields the key dissociative proton-consuming reactive adsorption of CO2 to produce CO; allowing the subsequent hydrogenation into C2 and C1 products by dimerization and protonation. These results yield valuable information on the variations in the electronic structure that redox-active copper catalysts undergo in the course of the electrochemical reaction, which, under extreme conditions are mediated by thermodynamics but, critically, kinetics dominate near the oxide/metal phase transitions.

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Language(s): eng - English
 Dates: 2018-10-112018-11-292019-01-07
 Publication Status: Published online
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acssuschemeng.8b05106
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: ACS Sustainable Chemistry & Engineering
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 8 Volume / Issue: 7 (1) Sequence Number: - Start / End Page: 1485 - 1492 Identifier: ISSN: 2168-0485
CoNE: https://pure.mpg.de/cone/journals/resource/2168-0485