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通过ZnSe敏化的封装MIL-125(Ti)空心纳米盘的分级TiO纳米片的多通道电荷转移用于高效CO光还原

Multi-channel charge transfer of hierarchical TiO nanosheets encapsulated MIL-125(Ti) hollow nanodisks sensitized by ZnSe for efficient CO photoreduction.

作者信息

Jiao Yuzhen, Chen Yajie, Han Wei, Liang Shumei, Li Wei, Tian Guohui

机构信息

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080, PR China.

Key Laboratory of Functional Inorganic Material Chemistry, Ministry of Education of the People's Republic of China, Heilongjiang University, Harbin 150080, PR China.

出版信息

J Colloid Interface Sci. 2022 Dec;627:492-502. doi: 10.1016/j.jcis.2022.07.038. Epub 2022 Jul 9.

DOI:10.1016/j.jcis.2022.07.038
PMID:35870402
Abstract

Metal-organic frameworks-based hybrids with desirable components, structures, and properties have been proven to be promising functional materials for photocatalysis and energy conversion applications. Herein, we proposed and prepared ZnSe sensitized hierarchical TiO nanosheets encapsulated MIL-125(Ti) hollow nanodisks with sandwich-like structure (MIL-125(Ti)@TiO\ZnSe HNDs) through a successive solvothermal and selenylation reaction route using the as-prepared MIL-125(Ti) nanodisks as precursor. In the ternary MIL-125(Ti)@TiO\ZnSe HNDs hybrid, TiO nanosheets were transformed from MIL-125(Ti) and in situ grown on both sides of the MIL-125(Ti) shell, forming sandwich-like hollow nanodisks, and the ratio of MIL-125(Ti)/TiO can be tuned by changing the solvothermal time. The ternary hybrids possess the advantages of enhanced incident light utilization and abundant accessible active sites originating from bimodal pore-size distribution and hollow sandwich-like heterostructure, which can effectively promote CO photoreduction reaction. Especially, the formed multi-channel charge transfer routes in the ternary heterojunctions contribute to the charge transfer/separation and extend the lifespan of charge-separated state, thus boosting CO photoreduction performance. The CO (513.1 μmol gh) and CH (45.1 μmol gh) evolution rates over the optimized ternary hybrid were greatly enhanced compared with the single-component and binary hybrid photocatalysts.

摘要

具有理想成分、结构和性能的金属有机框架基杂化物已被证明是用于光催化和能量转换应用的有前景的功能材料。在此,我们以制备的MIL-125(Ti)纳米盘为前驱体,通过连续的溶剂热和硒化反应路线,提出并制备了具有三明治状结构的ZnSe敏化分级TiO纳米片包裹的MIL-125(Ti)中空纳米盘(MIL-125(Ti)@TiO\ZnSe HNDs)。在三元MIL-125(Ti)@TiO\ZnSe HNDs杂化物中,TiO纳米片由MIL-125(Ti)转变而来,并在MIL-125(Ti)壳的两侧原位生长形成三明治状中空纳米盘,且MIL-125(Ti)/TiO的比例可通过改变溶剂热时间来调节。三元杂化物具有增强的入射光利用率以及源自双峰孔径分布和中空三明治状异质结构的丰富可及活性位点的优势,这可以有效地促进CO光还原反应。特别是,三元异质结中形成的多通道电荷转移路线有助于电荷转移/分离并延长电荷分离态的寿命,从而提高CO光还原性能。与单组分和二元杂化光催化剂相比,优化后的三元杂化物上的CO(513.1 μmol g h)和CH(45.1 μmol g h)析出速率大大提高。

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