Bias-Adaptable CO2-to-CO Conversion via Tuning the Binding of Competing Intermediates
Article
Liang, Y, Zhao, J, Zhang, H et al. (2021). Bias-Adaptable CO2-to-CO Conversion via Tuning the Binding of Competing Intermediates
. NANO LETTERS, 21(20), 8924-8932. 10.1021/acs.nanolett.1c02719
Liang, Y, Zhao, J, Zhang, H et al. (2021). Bias-Adaptable CO2-to-CO Conversion via Tuning the Binding of Competing Intermediates
. NANO LETTERS, 21(20), 8924-8932. 10.1021/acs.nanolett.1c02719
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.
