Electrochemically scrambled nanocrystals are catalytically active for CO 2 -to-multicarbons
| Autor: | Sunmoon Yu, Tom Lin, Chenlu Xie, Sheena Louisia, Yifan Li, Peidong Yang, Shaul Aloni, Dohyung Kim, Qiao Kong, Sirine C. Fakra |
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| Rok vydání: | 2020 |
| Předmět: | |
| Zdroj: | Proceedings of the National Academy of Sciences. 117:9194-9201 |
| ISSN: | 1091-6490 0027-8424 |
| DOI: | 10.1073/pnas.1918602117 |
| Popis: | Promotion of C-C bonds is one of the key fundamental questions in the field of CO2 electroreduction. Much progress has occurred in developing bulk-derived Cu-based electrodes for CO2-to-multicarbons (CO2-to-C2+), especially in the widely studied class of high-surface-area "oxide-derived" copper. However, fundamental understanding into the structural characteristics responsible for efficient C-C formation is restricted by the intrinsic activity of these catalysts often being comparable to polycrystalline copper foil. By closely probing a Cu nanoparticle (NP) ensemble catalyst active for CO2-to-C2+, we show that bias-induced rapid fusion or "electrochemical scrambling" of Cu NPs creates disordered structures intrinsically active for low overpotential C2+ formation, exhibiting around sevenfold enhancement in C2+ turnover over crystalline Cu. Integrating ex situ, passivated ex situ, and in situ analyses reveals that the scrambled state exhibits several structural signatures: a distinct transition to single-crystal Cu2O cubes upon air exposure, low crystallinity upon passivation, and high mobility under bias. These findings suggest that disordered copper structures facilitate C-C bond formation from CO2 and that electrochemical nanocrystal scrambling is an avenue toward creating such catalysts. |
| Databáze: | OpenAIRE |
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