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Enhanced Photocatalytic CO2 Reduction Activity over NH2-MIL-125(Ti) by Facet Regulation
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-12-29 , DOI: 10.1021/acscatal.0c04426
Xiao-Mei Cheng 1, 2 , Xiao-Yao Dao 1 , Shi-Qing Wang 1 , Jing Zhao 2 , Wei-Yin Sun 1
Affiliation  

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 μmol 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, TiIII 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.

中文翻译:

通过方面调节提高了NH 2 -MIL-125(Ti)上的光催化CO 2还原活性

指定和优化光催化剂的构面是解决依赖于构面的光催化反应问题的有效策略。但是,有关金属有机骨架(MOF)对光催化过程的刻面影响的研究仍处于起步阶段。本研究精确控制和合成了{001}和{111}晶面比例不同的NH 2 -MIL-125(Ti),发现随着暴露比例的逐渐增加,CO 2的光还原活性增强。 {111}个方面。{111}刻面显示出光催化活性,最大CO和CH 4产率为8.25和1.01μmolg –1 h –1,分别比{001}小平面高9倍和5倍。同样,{111}刻面在产生CO和CH 4时分别具有最高的量子产率,分别为0.14和0.07%。稳态和时间分辨荧光光谱揭示了抑制具有{111}刻面的样品的光致电子和空穴复合的重要性。此外,在反应过程中形成的Ti III显示出对CO 2的强还原性。从NH 2开始-MIL-125(Ti),可以通过调节暴露的{111}面来增强光催化性能。这项工作不仅提供了通过调整MOF暴露的活性面来进一步提高光催化性能的策略,而且还提供了对改善CO 2的光催化还原性的因素的深刻理解。
更新日期:2021-01-15
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