Regulating the Donor and Acceptor Interaction Mode in Metal–Organic Frameworks for H<sub>2</sub>O<sub>2</sub> Photosynthesis
Mingxue Shao, Rao Bao, Huadong Guo, Yao Cen, Song Wang, Yutong Song, Xianmin Guo
Abstract
Development of novel photocatalysts for hydrogen peroxide (H 2 O 2 ) 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 H 2 O 2, with a remarkable production rate of 5141 μmol h –1 g –1, superior to that of short-range UiO-67-NB (813 μmol h –1 g –1 ) and long-range UiO-67-PE/BB (3361 μmol h –1 g –1 ), 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 H 2 O 2 photosynthesis.