期刊
ACS CATALYSIS
卷 11, 期 21, 页码 13330-13336出版社
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c03717
关键词
CO2 electroreduction; theory-driven; copper cubes; silver; tandem; ethanol
资金
- Gaznat S.A.
- H2020 Marie Curie Individual Fellowship grant SURFCAT [837378]
- Swiss National Science Foundation
- Spanish MICIUN's Grant [RTI2018-095460-B-I00]
- Ramon y Cajal Grant [RYC-2015-18996]
- Maria de Maeztu Grant [MDM-2017-0767]
- Generalitat de Catalunya [2017SGR13]
- Red Espanola de Supercomputacion (RES) [QS-2019-3-0018, QS-2019-20023, QCM-2019-1-0034]
- NWO Physical Sciences
- Marie Curie Actions (MSCA) [837378] Funding Source: Marie Curie Actions (MSCA)
By utilizing theoretical considerations and experimental validation, this study designed an electrocatalyst with higher selectivity towards ethanol in CO2 reduction reaction. Through investigating the catalytic behavior of Cu nano-cubes of different sizes, it was predicted that smaller Cu-cub possess higher selectivity for ethanol due to their larger edge-to-faces ratio.
In the CO2 reduction reaction, the design of electrocatalysts that selectively promote alcohols over hydrocarbons (e.g., ethanol over ethylene) hinges on the understanding of the pathways and specific sites that form alcohols. Herein, theoretical considerations guide state-of-the-art synthesis of well-defined catalysts to show that higher selectivity toward ethanol is achieved on Cu(110) edge sites compared to Cu(100) terraces. Specifically, we study the catalytic behavior of Cu nano-cubes (Cu-cub) of different sizes in the framework of tandem catalysis with CO-producing Ag nano-spheres. We predict and experimentally find that the smaller Cu-cub possess higher selectivity for ethanol in view of their larger edge-to-faces ratio and of the fact that ethylene is produced at terraces while ethanol is selectively produced at step edges. These results call for synthetic developments toward Cu nanostructures exposing only edge sites, such as hollow cubic nanocages, to further increase ethanol selectivity. More generally, this study encourages the application of well-defined nano catalysts as a bridge between theory and experiments in electrocatalysis.
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