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使用TiO通过光催化从乙酸水溶液中生产碳氢化合物并同时光沉积铜。

Photocatalytic hydrocarbon production from aqueous acetic acid using TiO with simultaneous photodeposition of Cu.

作者信息

Uzzaman Monir, Furukawa Mai, Tateishi Ikki, Katsumata Hideyuki, Afrin Mst Farhana, Kaneco Satoshi

机构信息

Department of Applied Chemistry, Graduate School of Engineering, Mie University Tsu Mie 514-8507 Japan

Mie Global Environment Center for Education & Research, Mie University Tsu Mie 514-8507 Japan.

出版信息

RSC Adv. 2025 Feb 17;15(7):5316-5326. doi: 10.1039/d4ra08731c. eCollection 2025 Feb 13.

Abstract

Photocatalytic techniques are considered clean, sustainable and cost-effective in energy conversion and environmental restoration. The large band gap, light harvesting limitation and rapid electron-hole pair recombination can suppress the photocatalytic efficiency in photocatalytic applications. Metal deposition has become one of the most important technical means to improve photocatalytic efficiency. This study has dealt with photocatalytic hydrocarbon and hydrogen production from the acetic acid solution with simultaneous Cu deposition on TiO photocatalyst surface. Due to having favorable redox potential and work function values, the photodeposition and Schottky junction formation of Cu occurred smoothly on the TiO surface, which further contributed to accelerating the interfacial charge transfer and photocatalytic activity. The reaction conditions (Cu loading, reaction pH and initial concentration of acetic acid) were optimized to enhance photocatalytic methane production. Under the optimum condition, the Cu/TiO photocatalytic hydrocarbon production was maximum (4136 μmol g), approximately 9 times better than those obtained with pure TiO (450 μmol g). The surface morphological and optical properties of photodeposited Cu/TiO samples were characterized before and after the photocatalytic reaction with utmost precision and thoroughness using a TEM, XPS, DRS, PL, N adsorption-desorption isotherm and BET surface area analysis. The DRS and PL study confirm that Cu-deposition on TiO reduced the energy bandgap and improved the light-harvesting area, photogenerated electron-hole pair separation and migration efficiency, respectively. Cycle experiments disclose that the simultaneous Cu-deposited photocatalyst has excellent stability and reusability. A reaction mechanism was proposed for the photocatalytic hydrocarbon formation from the acetic acid by Cu/TiO photocatalytic reaction.

摘要

光催化技术在能量转换和环境修复方面被认为是清洁、可持续且具有成本效益的。大的带隙、光捕获限制以及快速的电子 - 空穴对复合会抑制光催化应用中的光催化效率。金属沉积已成为提高光催化效率的最重要技术手段之一。本研究涉及在TiO光催化剂表面同时沉积Cu的情况下,由乙酸溶液进行光催化制烃和制氢。由于具有良好的氧化还原电位和功函数值,Cu在TiO表面顺利发生光沉积并形成肖特基结,这进一步有助于加速界面电荷转移和光催化活性。优化了反应条件(Cu负载量、反应pH值和乙酸初始浓度)以提高光催化甲烷产量。在最佳条件下,Cu/TiO光催化制烃量最大(4136 μmol g),约为纯TiO(450 μmol g)的9倍。使用透射电子显微镜(TEM)、X射线光电子能谱(XPS)、漫反射光谱(DRS)、光致发光(PL)、N吸附 - 脱附等温线和BET比表面积分析,以极高的精度和彻底性对光沉积的Cu/TiO样品在光催化反应前后的表面形态和光学性质进行了表征。DRS和PL研究证实,在TiO上沉积Cu分别降低了能带隙、提高了光捕获面积、光生电子 - 空穴对的分离和迁移效率。循环实验表明,同时沉积Cu的光催化剂具有优异的稳定性和可重复使用性。提出了Cu/TiO光催化反应由乙酸光催化形成烃的反应机理。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6dde/11831735/ea157dae00a8/d4ra08731c-f1.jpg

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