Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 21, Pages 6192-6197Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201802083
Keywords
copper cubes; electroreduction; density functional calculations; nanoelectrochemistry; surface chemistry
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Funding
- Cluster of Excellence RESOLV at RUB - Deutsche Forschungsgemeinschaft [EXC 1069]
- German Federal Ministry of Education and Research (Bundesministerium fur Bildung und Forschung BMBF) [03SF0523C]
- European Research Council [ERC-725915]
- U.S. National Science Foundation (NSF-Chemistry) [1213182]
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1213182] Funding Source: National Science Foundation
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Insitu and operando spectroscopic and microscopic methods were used to gain insight into the correlation between the structure, chemical state, and reactivity of size- and shape-controlled ligand-free Cu nanocubes during CO2 electroreduction (CO2RR). Dynamic changes in the morphology and composition of Cucubes supported on carbon were monitored under potential control through electrochemical atomic force microscopy, X-ray absorption fine-structure spectroscopy and X-ray photoelectron spectroscopy. Under reaction conditions, the roughening of the nanocube surface, disappearance of the (100) facets, formation of pores, loss of Cu and reduction of CuOx species observed were found to lead to a suppression of the selectivity for multi-carbon products (i.e. C2H4 and ethanol) versus CH4. A comparison with Cucubes supported on Cu foils revealed an enhanced morphological stability and persistence of Cu-I species under CO2RR in the former samples. Both factors are held responsible for the higher C-2/C-1 product ratio observed for the Cu cubes/Cu as compared to Cu cubes/C. Our findings highlight the importance of the structure of the active nanocatalyst but also its interaction with the underlying substrate in CO2RR selectivity.
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