Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO2 Reduction at Modified Cu Surfaces
| Autor: | Aya K. Buckley, F. Dean Toste, Francesca M. Toma, David M. Larson, Michelle Lee, Roman V. Kazantsev, William A. Goddard, Tao Cheng |
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| Rok vydání: | 2019 |
| Předmět: |
Formic acid
Cationic polymerization General Chemistry 010402 general chemistry Electrocatalyst 01 natural sciences Biochemistry Catalysis 0104 chemical sciences Metal Molecular dynamics chemistry.chemical_compound Colloid and Surface Chemistry chemistry Chemical engineering visual_art visual_art.visual_art_medium ReaxFF Selectivity |
| Zdroj: | Journal of the American Chemical Society. 141:7355-7364 |
| ISSN: | 1520-5126 0002-7863 |
| DOI: | 10.1021/jacs.8b13655 |
| Popis: | The limited selectivity of existing CO_2 reduction catalysts and rising levels of CO_2 in the atmosphere necessitate the identification of specific structure–reactivity relationships to inform catalyst development. Herein, we develop a predictive framework to tune the selectivity of CO_2 reduction on Cu by examining a series of polymeric and molecular modifiers. We find that protic species enhance selectivity for H_2, hydrophilic species enhance formic acid formation, and cationic hydrophobic species enhance CO selectivity. ReaxFF reactive molecular dynamics simulations indicate that the hydrophilic/hydrophobic modifiers influence the formation of surface hydrides, which yield formic acid or H_2. These observations offer insights into how these modifiers influence catalytic behavior at the non-precious Cu surface and may aid in the future implementation of organic structures in CO_2 reduction devices. |
| Databáze: | OpenAIRE |
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