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Elucidating the structure-dependent selectivity towards methane and ethanol of CuZn in the CO2 electroreduction using tailored Cu/ZnO precatalysts

Seyedeh Behnaz Varandili1, Dragos Stoian1, Jan Vavra1, Kevin Rossi1*, James R Pankhurst1, Yannick Guntern1, Nuria Lopez2, Raffaella Buonsanti1*

1 Laboratory of Nanochemistry for Energy (LNCE), Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne, CH-1950 Sion, Switzerland

2 Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology, 43007 Tarragona, Spain

* Corresponding authors emails: kevin.rossi@epfl.ch, Raffaella.buonsanti@epfl.ch
DOI10.24435/materialscloud:3r-gn [version v1]

Publication date: Oct 22, 2021

How to cite this record

Seyedeh Behnaz Varandili, Dragos Stoian, Jan Vavra, Kevin Rossi, James R Pankhurst, Yannick Guntern, Nuria Lopez, Raffaella Buonsanti, Elucidating the structure-dependent selectivity towards methane and ethanol of CuZn in the CO2 electroreduction using tailored Cu/ZnO precatalysts, Materials Cloud Archive 2021.165 (2021), doi: 10.24435/materialscloud:3r-gn.

Description

Understanding the catalyst compositional and structural features that control selectivity is of uttermost importance to target desired products in chemical reactions. In this joint experimental–computational work, we leverage tailored Cu/ZnO precatalysts as a material platform to identify the intrinsic features of methane-producing and ethanol-producing CuZn catalysts in the electrochemical CO2 reduction reaction (CO2RR). Specifically, we find that Cu@ZnO nanocrystals, where a central Cu domain is decorated with ZnO domains, and ZnO@Cu nanocrystals, where a central ZnO domain is decorated with Cu domains, evolve into Cu@CuZn core@shell catalysts that are selective for methane (∼52%) and ethanol (∼39%), respectively. Operando X-ray absorption spectroscopy and various microscopy methods evidence that a higher degree of surface alloying along with a higher concentration of metallic Zn improve the ethanol selectivity. Density functional theory explains that the combination of electronic and tandem effects accounts for such selectivity. These findings mark a step ahead towards understanding structure–property relationships in bimetallic catalysts for the CO2RR and their rational tuning to increase selectivity towards target products, especially alcohols.

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Files

File name Size Description
pbe.inp
MD5md5:0a05a6f37bbcd79a07e48839d50c2e53
1.9 KiB cp2k.inp input file for the calculations
10001.xyz
MD5md5:0ef032b777348f5631b6e5acc3369756
5.5 KiB example position file
pbe-log.cp2k
MD5md5:923ee9ba50687411c9861707932abf26
650.1 KiB log file of the calculation
pbe-bader.inp
MD5md5:0ea2d6aaa9de4ad049ba184519cd0bb7
2.0 KiB cp2k.inp input file for the calculation with charge cube file output
README.txt
MD5md5:50c9af2d04f1af080db329b6525eed15
248 Bytes README

License

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Keywords

CO2RR DFT CO2 Cu CuZn ERC H2020 EPFL SNSF

Version history:

2021.165 (version v1) [This version] Oct 22, 2021 DOI10.24435/materialscloud:3r-gn