期刊
NANO LETTERS
卷 21, 期 2, 页码 1003-1010出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.0c04051
关键词
face-centered tetragonal gold; metastable phase; interface strain; CO2 electroreduction
类别
资金
- NSFC [U2032149, 21905089, U1932212]
- Hunan Provincial Natural Science Foundation of China [2020JJ2001, 2020JJ3001]
- Fundamental Research Funds for the Central Universities
- Youth Innovation Promotion Association CAS [2019441]
The stable fct Au nanocrystals synthesized through intermetallic core-shell structure exhibit significantly improved catalytic activity in CO2 reduction, attributed to the upshifted d-band center lowering the energy barrier for key intermediate COOH* formation.
Synthesis of the unconventional phase of noble metal nanocrystals may create new opportunities in exploring intriguing physicochemical properties but remains challenging. In the research field of thin film growth, the interface strain offers a general driving force to stabilize the metastable phase of epitaxial film. Herein we extend this concept to the field of noble metal nanocrystals and report the solution synthesis of metastable face-centered tetragonal Au that has not been discovered before. The successful synthesis relies on the formation of intermetallic AuCu3@Au core-shell structure, where the interface strain stabilizes the metastable fct Au overlayer. Compared with the face-centered cubic Au counterpart, the metastable fct Au shows greatly improved catalytic activity toward CO2 reduction to CO. The density functional theory calculations and spectroscopic studies reveal that the metastable fct Au upshifts the d-band center, which lowers the energy barrier of key intermediate COOH* formation and thus facilitates the reaction kinetics.
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