Selective CO2 Electrochemical Reduction Enabled by a Tricomponent Copolymer Modifier on a Copper Surface
| Autor: | Turki N. Baroud, Robert H. Grubbs, William A. Goddard, Tao Cheng, Jeong Hoon Ko, Aidan Q. Fenwick, Alonso Rosas-Hernández, Jianchun Wang, Quan Gan |
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| Rok vydání: | 2021 |
| Předmět: | |
| Zdroj: | Journal of the American Chemical Society. 143:2857-2865 |
| ISSN: | 1520-5126 0002-7863 |
| Popis: | Electrochemical CO2 reduction over Cu could provide value-added multicarbon hydrocarbons and alcohols. Despite recent breakthroughs, it remains a significant challenge to design a catalytic system with high product selectivity. Here we demonstrate that a high selectivity of ethylene (55%) and C2+ products (77%) could be achieved by a highly modular tricomponent copolymer modified Cu electrode, rivaling the best performance using other modified polycrystalline Cu foil catalysts. Such a copolymer can be conveniently prepared by a ring-opening metathesis polymerization, thereby offering a new degree of freedom for tuning the selectivity. Control experiments indicate all three components are essential for the selectivity enhancement. A surface characterization showed that the incorporation of a phenylpyridinium component increased the film robustness against delamination. It was also shown that its superior performance is not due to a morphology change of the Cu underneath. Molecular dynamics (MD) simulations indicate that a combination of increased local CO2 concentration, increased porosity for gas diffusion, and the local electric field effect together contribute to the increased ethylene and C2+ product selectivity. |
| Databáze: | OpenAIRE |
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