Modulation of interface structure on titanium-based metal-organic frameworks heterojunctions for boosting photocatalytic carbon dioxide reduction.

IF 9.4 1区 化学 Q1 CHEMISTRY, PHYSICAL
Journal of Colloid and Interface Science Pub Date : 2025-05-01 Epub Date: 2025-01-16 DOI:10.1016/j.jcis.2025.01.125
Xiaoyu Ma, Yan Zhang, Awu Zhou, Yutong Jia, Zhenghe Xie, Lifeng Ding, Jian-Rong Li
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引用次数: 0

Abstract

Rational regulation of interface structure in photocatalysts is a promising strategy to improve the photocatalytic performance of carbon dioxide (CO2) reduction. However, it remains a challenge to modulate the interface structure of multi-component heterojunctions. Herein, a strategy integrating heterojunction with facet engineering is developed to modulate the interface structure of metal-organic frameworks (MOF)-based heterojunctions. A series of core-shell UiO-66 (Zr-MOF)-loaded MIL-125 (Ti-MOF) heterojunctions with exposed specific facets were prepared to enhance the separation efficiency of photogenerated electrons-holes in CO2 photoreduction. Impressively, MIL-125to@UiO-66 with exposed {1 1 1} facet exhibits an excellent CO production rate (56.4 μmol g-1 h-1) and selectivity (99 %) under visible light irradiation without any photosensitizers/sacrificial agents, being 1.4 and 11.3 times higher than individual MIL-125to and UiO-66, respectively. The type-II heterojunction significantly enhances the separation of photogenerated electrons-holes in physical space. The photogenerated electrons migrate from Zr in UiO-66 to Ti in MIL-125to, promoting a spatial synergy between CO2 reduction on MIL-125to and H2O oxidation on UiO-66. Compared with MIL-125rd@UiO-66 with exposed {1 1 0} facet and MIL-125ds@UiO-66 with exposed {0 0 1} facet, MIL-125to@UiO-66 with exposed {1 1 1} facet improves the exposure of surface-active Ti sites, thereby enhancing the adsorption/activation of CO2 to generate the *COOH intermediate. This work provides an effective strategy for designing MOF-based heterojunction photocatalysts to improve photocatalytic performance.

钛基金属-有机骨架异质结界面结构的调制促进光催化二氧化碳还原。
合理调节光催化剂的界面结构是提高光催化还原二氧化碳性能的有效途径。然而,如何调制多组分异质结的界面结构仍然是一个挑战。在此基础上,提出了一种将异质结与面工程相结合的策略来调节金属有机骨架异质结的界面结构。为了提高CO2光还原过程中光电子空穴的分离效率,制备了一系列具有暴露特定表面的核壳负载UiO-66 (Zr-MOF) MIL-125 (Ti-MOF)异质结。令人惊讶的是,在不使用任何光敏剂/牺牲剂的情况下,暴露{11 11}面的MIL-125to@UiO-66在可见光照射下表现出良好的CO产率(56.4 μmol g-1 h-1)和选择性(99%),分别是MIL-125to和UiO-66的1.4倍和11.3倍。ii型异质结显著增强了光生电子空穴在物理空间上的分离。光生电子从UiO-66中的Zr迁移到MIL-125to中的Ti,促进了MIL-125to上的CO2还原和UiO-66上的H2O氧化之间的空间协同作用。与暴露在{11 0}面的MIL-125rd@UiO-66和暴露在{0 0 1}面的MIL-125ds@UiO-66相比,暴露在{11 1}面的MIL-125to@UiO-66改善了表面活性Ti位点的暴露,从而增强了CO2的吸附/活化,生成了*COOH中间体。本研究为设计基于mof的异质结光催化剂以提高光催化性能提供了有效的策略。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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来源期刊
CiteScore
16.10
自引率
7.10%
发文量
2568
审稿时长
2 months
期刊介绍: The Journal of Colloid and Interface Science publishes original research findings on the fundamental principles of colloid and interface science, as well as innovative applications in various fields. The criteria for publication include impact, quality, novelty, and originality. Emphasis: The journal emphasizes fundamental scientific innovation within the following categories: A.Colloidal Materials and Nanomaterials B.Soft Colloidal and Self-Assembly Systems C.Adsorption, Catalysis, and Electrochemistry D.Interfacial Processes, Capillarity, and Wetting E.Biomaterials and Nanomedicine F.Energy Conversion and Storage, and Environmental Technologies
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