Boosting CO2 photoreduction to acetic acid via the van der waals heterostructures of monolayer Nb2O5 modified TiO2 nanotubes

IF 8.1 1区 工程技术 Q1 ENGINEERING, CHEMICAL Separation and Purification Technology Pub Date : 2024-11-29 DOI:10.1016/j.seppur.2024.130835
Ruibin Lv , Kai Liu , Hui Hu , Maohong Fan , Kunpeng Li , Mi Zhang , Hao Huang
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Abstract

Photoreduction of CO2 to hydrocarbons encounters two significant challenges: low product yields and poor selectivity. Furthermore, the difficulty of C-C coupling reactions hinders the formation of higher-value two-carbon products. This paper presents a strategy to address these challenges by fabricating a van der Waals heterostructure photocatalyst through the surface modification of TiO2 nanotubes (TNTs) with monolayer Nb2O5, denoted as 3 %Nb2O5/TNTs. Compared with TNTs, the acetic acid yield of heterostructures reached 28.4 μmol gcat-1h−1, and the selectivity rose from 48 % to 69 %. The van der Waals heterostructures reduced the photogenerated electron-hole recombination, extending the lifetime of charge carriers. The reduction of resistance and the presence of built-in fields accelerated the migration of charge carriers, thereby showing an enhanced photocatalytic performance. Surface modification of monolayer Nb2O5 promoted the activation adsorption of CO2 to CO2·-, facilitating the following C-C coupling reaction. Furthermore, its surface acidity sites modulated the hydrogenation reactions following C-C coupling, thereby increasing both the yield and selectivity of acetic acid.

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通过单层Nb2O5修饰TiO2纳米管的范德华异质结构促进CO2光还原成乙酸
二氧化碳光还原成碳氢化合物面临两个重大挑战:产物收率低和选择性差。此外,C-C偶联反应的难度阻碍了高值二碳产物的形成。本文提出了一种解决这些问题的策略,即通过用单层Nb2O5修饰TiO2纳米管(tnt)表面来制备范德瓦尔斯异质结构光催化剂,表示为3 %Nb2O5/ tnt。与tnt相比,异质结构的乙酸产率达到28.4 μmol gcat-1h−1,选择性从48 %提高到69 %。范德华异质结构减少了光生电子-空穴复合,延长了载流子的寿命。电阻的减小和内嵌场的存在加速了载流子的迁移,从而显示出增强的光催化性能。单层Nb2O5的表面修饰促进了CO2对CO2·-的活化吸附,有利于后续的C-C偶联反应。此外,其表面酸性位点调节了C-C偶联后的加氢反应,从而提高了乙酸的产率和选择性。
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来源期刊
Separation and Purification Technology
Separation and Purification Technology 工程技术-工程:化工
CiteScore
14.00
自引率
12.80%
发文量
2347
审稿时长
43 days
期刊介绍: Separation and Purification Technology is a premier journal committed to sharing innovative methods for separation and purification in chemical and environmental engineering, encompassing both homogeneous solutions and heterogeneous mixtures. Our scope includes the separation and/or purification of liquids, vapors, and gases, as well as carbon capture and separation techniques. However, it's important to note that methods solely intended for analytical purposes are not within the scope of the journal. Additionally, disciplines such as soil science, polymer science, and metallurgy fall outside the purview of Separation and Purification Technology. Join us in advancing the field of separation and purification methods for sustainable solutions in chemical and environmental engineering.
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