Molecular Compartments Created in Metal-Organic Frameworks for Efficient Visible-Light-Driven CO 2 Overall Conversion.

Journal of the American Chemical Society(2022)

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摘要
We report the construction of molecular compartments by the growth of narrow-band semiconductor nanoparticles, tungsten oxide and its hydrate, in the mesopores of a metal-organic framework (MOF), MIL-100-Fe. The location of these nanoparticles in pores and their spatial arrangement across the MOF crystal are unveiled by powder X-ray diffraction and small-angle neutron scattering, respectively. Such a composition with pore-level precision leads to efficient overall conversion of gas-phase CO and HO to CO, CH, and HO under visible light. When WO·HO nanoparticles are positioned in 2.5 nm mesopores with 24 wt %, the resulting composite, namely, 24%-WO·HO-in-MIL-100-Fe, exhibits a CO reduction rate of 0.49 mmol·g·h beyond 420 nm and an apparent quantum efficiency of 1.5% at 420 nm. These performances stand as new benchmarks for visible-light-driven CO overall conversion. In addition to the size and location of semiconductor nanoparticles, the coordinated water species in the crystal are found critical for high catalytic activity, an aspect usually overlooked.
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