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Article Abstract

Development of novel photocatalysts for hydrogen peroxide (HO) production from water and oxygen is gathering great attention, but still suffers from inefficient photogenerated charge mobility. Reticular chemistry in metal-organic frameworks (MOFs) provides a promising platform to enhance the charge-transfer kinetics by assembling a donor-acceptor (D-A) system. Here, we designed and synthesized a series of D-A type MOFs (UiO-67-NB, UiO-67-PE/BB, and UiO-67-PE/NB) via regulating the interaction mode of donor and acceptor. As the first example of short and long-range combined D-A MOF, UiO-67-PE/NB exerted enhanced photogenerated electron transfer as well as suppressed their backward recombination, which facilitated the indirect two-step 2e ORR for visible-light driven photosynthesis of HO, with a remarkable production rate of 5141 μmol h g, superior to that of short-range UiO-67-NB (813 μmol h g) and long-range UiO-67-PE/BB (3361 μmol h g), and also exceeding most of MOF-based photocatalysts. This work puts forward new insights into systematic engineering of D-A MOFs at the molecular level for highly efficient HO photosynthesis.

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http://dx.doi.org/10.1021/acs.inorgchem.5c03360DOI Listing

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