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Inorg Chem ; 62(19): 7235-7249, 2023 May 15.
Artigo em Inglês | MEDLINE | ID: mdl-37126665

RESUMO

The construction of photoactive units in the proximity of a stable framework support is one of the promising strategies for uplifting photocatalysis. In this work, the ultrasmall Pd NPs implanted onto core-shell (CS) metal organic frameworks (MOFs), i.e., CS@Pd nanoarchitectures with tailored electronic and structural properties are reported. The all-in-one heterogeneous catalyst CS@Pd3 improves the surface functionalities and exhibits an outstanding hydrogen evolution reaction (HER) activity rate of 12.7 mmol g-1 h-1, which is 10-folds higher than the pristine frameworks with an apparent quantum efficiency (AQE) of 9.02%. The bifunctional CS@Pd shows intriguing results when subjected to photocatalytic CO2 reduction with an impressive rate of 71 µmol g-1 h-1 of MeOH under visible-light irradiation at ambient conditions. Spectroscopic data reveal efficient charge migrations and an extended lifetime of 2.4 ns, favoring efficient photocatalysis. The microscopic study affirms the formation of well-ordered CS morphology with precise decoration of Pd NPs over the CS networks. The significance of active Pd and Co sites is addressed by congruent charge-transfer kinetics and computational density functional theory calculations of CS@Pd, which validate the experimental findings with their synergistic involvement in improved photocatalytic activity. This present work provides a facile and competent avenue for the systematic construction of MOF-based CS heterostructures with active Pd NPs.

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