Enhanced oxidative desulfurization activity over NH2-MIL-125(HAc) through facet modulation by acetic acid and surface modification by amino group
APPLIED SURFACE SCIENCE(2024)
摘要
Designation and optimization of facets of photocatalysts is an effective strategy to address the issue of facet-dependent photocatalytic reactions. However, studies regarding the facet effect of metal-organic frameworks (MOFs) on the photocatalytic process are in infancy. In this study, NH2-MIL-125(Ti) with different ratios of {001} and {111} facets was exactly controlled and synthesized, and it was found that the activity in photoreduction of CO2 is enhanced with gradually increasing exposed proportion of {111} facets. The {111} facets exhibit photocatalytic activity with the maximal CO and CH4 yields of 8.25 and 1.01 mu mol g(-1) h(-1), which are 9 and 5 times higher than those of {001} facets, respectively. Also, the {111} facets give the highest quantum yields of 0.14 and 0.07% for CO and CH4 production, respectively. Steady-state and time-resolved fluorescence spectra reveal the importance of inhibiting the recombination of photoinduced electrons and holes for the sample with {111} facets. Besides, Ti-III formed during the reaction process exhibits strong reducibility for CO2. Starting from NH2-MIL-125(Ti), the photocatalytic performance can be enhanced by regulating exposed {111} facets. This work not only provides a strategy for further enhancing photocatalytic performance by tuning the exposed active facets of MOFs, but also provides a deep understanding of the factors for improving the photocatalytic reduction of CO2.
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关键词
Oxidative desulfurization,Facet modulation,Surface modification,Metal -organic frameworks
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