期刊
NANO LETTERS
卷 21, 期 20, 页码 8924-8932出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.1c02719
关键词
palladium; metal-organic frameworks; ligand modification; CO2 electroreduction; intermediate binding strength
类别
资金
- National Key Research and Development Program of China [2019YFA0405600]
- National Science Fund for Distinguished Young Scholars [21925204]
- NSFC [U1932146, U19A2015]
- Fundamental Research Funds for the Central Universities, Provincial Key Research and Development Program of Anhui [202004a05020074]
- USTC Research Funds of the Double First-Class Initiative [YD2340002002]
- Canada Foundation for Innovation (CFI)
- Natural Sciences and Engineering Research Council (NSERC)
- National Research Council (NRC)
- Canadian Institutes of Health Research (CIHR)
- Government of Saskatchewan
- University of Saskatchewan
- Australian Research Council Discovery Early Career Researcher Award - Australian Government [DE200100477]
- Australian Research Council [DE200100477] Funding Source: Australian Research Council
By modifying the catalyst with functional ligands, the study successfully adjusted the intermediate binding of the catalyst, achieving a highly selective CO2-to-CO conversion over a widened potential window. The catalyst exhibited over 80% CO faradaic efficiency in the range of -0.3 to -1.2 V, reaching a maximum of 98.2% at -0.8 V.
CO2 electroreduction powered by renewable electricity represents a promising method to enclose anthropogenic carbon cycle. Current catalysts display high selectivity toward the desired product only over a narrow potential window due primarily to unoptimized intermediate binding. Here, we report a functional ligand modification strategy in which palladium nanoparticles are encapsulated inside metal-organic frameworks with 2,2'- bipyridine organic linkers to tune intermediate binding and thus to sustain a highly selective CO2-to-CO conversion over widened potential window. The catalyst exhibits CO faradaic efficiency in excess of 80% over a potential window from -0.3 to -1.2 V and reaches the maxima of 98.2% at -0.8 V. Mechanistic studies show that the 2,2'- bipyridine on Pd surface reduces the binding strength of both *H and *CO, a too strong binding of which leads to competing formate production and CO poison, respectively, and thus enhances the selectivity and stability of CO product.
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