One-Dimensional Single-Crystal Mesoporous TiO2 Supported CuW6O24 Clusters as Photocatalytic Cascade Nanoreactor for Boosting Reduction of CO2 to CH4

IF 27.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jiaming Zhang, Duoxin Shi, Junyu Yang, Linlin Duan, Pengfei Zhang, Mingbin Gao, Jinlu He, Yulan Gu, Kun Lan, Jiangwei Zhang, Jian Liu, Dongyuan Zhao, Yuzhu Ma
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引用次数: 0

Abstract

Constructing nanoreactors with multiple active sites in well-defined crystalline mesoporous frameworks is an effective strategy for tailoring photocatalysts to address the challenging of CO2 reduction. Herein, one-dimensional (1-D) mesoporous single-crystal TiO2 nanorod (MS-TiO2-NRs, ≈110 nm in length, high surface area of 117 m2 g−1, and uniform mesopores of ≈7.0 nm) based nanoreactors are prepared via a droplet interface directed-assembly strategy under mild condition. By regulating the interfacial energy, the 1-D mesoporous single-crystal TiO2 can be further tuned to polycrystalline fan- and flower-like morphologies with different oxygen vacancies (Ov). The integration of single-crystal nature and mesopores with exposed oxygen vacancies make the rod-like TiO2 nanoreactors exhibit a high-photocatalytic CO2 reduction selectivity to CO (95.1%). Furthermore, photocatalytic cascade nanoreactors by in situ incorporation of CuW6O24 (W–Cu) clusters onto MS-TiO2-NRs via Ov are designed and synthesized, which improved the CO2 adsorption capacity and achieved two-step CO2–CO–CH4 photoreduction. The second step CO-to-CH4 reaction induced by W–Cu sites ensures a high generation rate of CH4 (420.4 µmol g−1 h−1), along with an enhanced CH4 selectivity (≈94.3% electron selectivity). This research provides a platform for the design of mesoporous single-crystal materials, which potentially extends to a range of functional ceramics and semiconductors for various applications.

Abstract Image

以 CuW6O24 簇为支撑的一维单晶介孔二氧化钛作为光催化级联纳米反应器,促进 CO2 还原成 CH4。
在定义明确的晶体介孔框架中构建具有多个活性位点的纳米反应器,是定制光催化剂以解决二氧化碳还原难题的有效策略。本文通过液滴界面定向组装策略,在温和条件下制备了基于一维(1-D)介孔单晶TiO2纳米棒(MS-TiO2-NRs,长度≈110 nm,高比表面积117 m2 g-1,均匀介孔≈7.0 nm)的纳米反应器。通过调节界面能,可以进一步将一维介孔单晶 TiO2 调整为具有不同氧空位(Ov)的多晶扇形和花状形态。单晶性质和介孔与暴露氧空位的结合,使棒状二氧化钛纳米反应器表现出较高的光催化二氧化碳还原选择性(95.1%)。此外,设计并合成了通过 Ov 在 MS-TiO2-NRs 上原位掺入 CuW6O24 (W-Cu)团簇的光催化级联纳米反应器,提高了 CO2 的吸附能力,实现了 CO2-CO-CH4 两步光还原。W-Cu位点诱导的第二步CO-CH4反应确保了CH4的高生成率(420.4 µmol g-1 h-1),同时提高了CH4的选择性(电子选择性≈94.3%)。这项研究为介孔单晶材料的设计提供了一个平台,它有可能扩展到各种应用领域的功能陶瓷和半导体。
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
Advanced Materials
Advanced Materials 工程技术-材料科学:综合
CiteScore
43.00
自引率
4.10%
发文量
2182
审稿时长
2 months
期刊介绍: Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.
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