期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 143, 期 17, 页码 6333-6338出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.1c01764
关键词
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资金
- Swedish Research Council (VR) [2016-04625, 2017-04321]
- Swedish Research Council Formas [2020-00831]
- Knut and Alice Wallenberg Foundation (KAW) [2016.072]
- Natural Science Foundation of Jiangsu Province [BK20180723]
- Open Project of State Key Laboratory of Supramolecular Structure and Materials [sklssm2021011]
- Swedish Foundation for Strategic Research
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
This study presents a series of novel multivariate metalorganic frameworks (MTV-MOFs) denoted as MTV-MIL-100, constructed by ordered metal clusters that enhance electronic structures of crystalline materials and improve mass transport utilizing the high porosity of the MOF structure.
Catalysts for photochemical reactions underlie many foundations in our lives, from natural light harvesting to modern energy storage and conversion, including processes such as water photolysis by TiO2. Recently, metal-organic frameworks (MOFs) have attracted large interest within the chemical research community, as their structural variety and tunability yield advantages in designing photocatalysts to address energy and environmental challenges. Here, we report a series of novel multivariate metalorganic frameworks (MTV-MOFs), denoted as MTV-MIL-100. They are constructed by linking aromatic carboxylates and AB(2)OX(3) bimetallic clusters, which have ordered atomic arrangements. Synthesized through a solvent-assisted approach, these ordered and multivariate metal clusters offer an opportunity to enhance and fine-tune the electronic structures of the crystalline materials. Moreover, mass transport is improved by taking advantage of the high porosity of the MOF structure. Combining these key advantages, MTV-MIL-100(Ti,Co) exhibits a high photoactivity with a turnover frequency of 113.7 mol(H2) g(cat).(-1) min(-1), a quantum efficiency of 4.25%, and a space time yield of 4.96 x 10(-5) in the photocatalytic hydrolysis of ammonia borane. Bridging the fields of perovskites and MOFs, this work provides a novel platform for the design of highly active photocatalysts.
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