期刊
DALTON TRANSACTIONS
卷 50, 期 48, 页码 17953-17959出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1dt03424c
关键词
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资金
- National Natural Science Foundation of China [21908113, 22035003, 22005153, 91856124]
- Frontiers Science Center for New Organic Matter [63181206]
Facet-engineering has been proven as an effective method to improve the photocatalytic activity of metal-organic framework (MOF)-based photocatalysts by promoting charge transfer. In this study, different crystal facets of NH2-UiO-66 were synthesized and tetra-decahedral NH2-UiO-66 with co-exposed (100) and (111) crystal facets showed superior photocatalytic performance. This study demonstrates the feasibility and potential of facet-engineering for enhancing the photocatalytic applications of MOFs.
Sluggish charge transfer is the major problem which restricts the development of metal-organic framework (MOF)-based photocatalysts. Recently, facet-engineering has been proven to be an effective method for solving this issue. However, due to difficulties in regulating the exposed facets of MOFs, there are few reports about the facet-engineering of MOF-based photocatalysts. Here, we firstly report facet-engineering for promoting the photocatalytic activity of NH2-UiO-66 crystals. In this study, by regulating the influence of kinetics and thermodynamics, cubic, tetra-decahedral, and octahedral forms of NH2-UiO-66 are synthesized. The photocatalytic hydrogen evolution rate of tetra-decahedral NH2-UiO-66 with co-exposed (100) and (111) crystal facets reaches 64.06 mu mol g(-1) h(-1), which is approximately 2 and 1.5 times greater than that of the cubic and octahedral forms of NH2-UiO-66, respectively. The density functional theory (DFT) calculation and ultrafast spectroscopy results indicate that a slight staggering exists in the band structure of (100) and (111) facets, causing the facets junction to appear. The facet junction promotes the charge separation efficiency and prolongs the lifetime of the charge carriers, thereby giving tetra-decahedral NH2-UiO-66 optimal photocatalytic performance. This study demonstrates the feasibility and potential of facet-engineering for photocatalytic applications of MOFs.
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