Electrochemically scrambled nanocrystals are catalytically active for CO2-to-multicarbons.
Proc Natl Acad Sci U S A
; 117(17): 9194-9201, 2020 04 28.
Article
in En
| MEDLINE
| ID: mdl-32295882
ABSTRACT
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.
Full text:
1
Collection:
01-internacional
Database:
MEDLINE
Language:
En
Journal:
Proc Natl Acad Sci U S A
Year:
2020
Document type:
Article