| 樊昊,周颖,代朋,姜文,万财文,李园园.化学通报,2025,88(2):200-211. |
| 金属Mn掺杂对Li2TiO3光催化性能的影响：非辐射耦合作用 |
| Effect of Metal Mn Doping on the Photocatalytic Performance of Li2TiO3: Non-Radiative Coupling Effects |
| 投稿时间：2024-09-12 修订日期：2024-11-04 |
| DOI： |
| 中文关键词: Li2TiO3 Li2MnO3 固溶体 光催化降解 密度泛函理论(DFT) 非辐射耦合 |
| 英文关键词:Li2TiO3 Li2MnO3 Solid Solution, photocatalytic degradation, Density Functional Theory(DFT), Non-Radiative Coupling |
| 基金项目:国家自然科学基金(22209017)、重庆市教委科学技术研究项目(KJQN202301613)、重庆市自然科学基金项目(CSTB2022NSCQ-MSX0981)、重庆第二师范学院校级重点项目(KY202307B)和重庆市大学生创新创业项目(S202214388010)资助 |
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| 中文摘要: |
| 我国部分海域存在氯酚类污染物，其中2,4-二氯苯酚(2,4-DCP)被纳入我国优先污染物名单，需要针对2,4-DCP进行研究为水质改善提供基础数据。本文通过固相法制备过渡金属Mn掺杂氧化物Li2TiO3，并研究其光催化降解2, 4-DCP的性能。使用粉末X射线衍射(PXRD)、傅里叶红外变换(FTIR)光谱、紫外可见漫反射光谱(UV-Vis DRS)、扫描电镜(SEM)、高倍透射电镜(HRTEM)以及X射线光电子能谱(XPS)对制备的光催化剂晶体结构、微观形貌、光学性能、化学组成进行表征。以高压汞灯为光源，探究了掺杂样品光催化降解2,4-DCP性能。光催化降解实验发现母体Li2TiO3在光源照射30 min后可降解76%的2,4-DCP。当掺杂Mn后，样品Li2Ti1-xMnxO3(x=0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0)材料的光催化效果都会得到大幅度的抑制。实验发现尽管Mn掺杂提升了材料的光吸收能力，但是Mn掺杂后光催化中光生载流子寿命大幅度减小。理论计算表明，Mn掺杂增强了光催化剂中的非辐射耦合系数从而抑制了光催化效率。本文的研究为理性掺杂优化光催化效率提供了重要的基础认，同时为景区氯酚类化合物的治理提供新方法和新思路。 |
| 英文摘要: |
| Chlorophenol pollutants exist in some sea areas of China, among which 2,4-dichlorophenol (2,4-DCP) has been included in the list of priority pollutants in China. Research on 2,4-DCP is needed to provide basic data for water quality improvement. This study prepared Mn-doped Li2TiO3 transition metal oxide via a solid-state method and investigated its photocatalytic degradation performance for 2,4-DCP. The synthesized photocatalysts are characterized by powder X-ray diffraction (PXRD), Fourier-transform infrared spectroscopy (FTIR), ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis DRS), scanning electron microscopy (SEM), high-resolution transmission electron microscopy (HRTEM), and X-ray photoelectron spectroscopy (XPS) to assess their crystal structure, morphology, optical properties, and chemical composition. Using a high-pressure mercury lamp as a light source, the photocatalytic degradation performance of the doped samples is explored. The degradation experiments show that the parent Li2TiO3 can degrade 76% of 2,4-DCP after 30 minutes of light exposure. However, the photocatalytic efficiency of the Li2Ti1-xMnxO3(x=0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0)(x = 0.1, 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8, 0.9, 1.0) is significantly suppressed. Despite the fact that Mn doping enhances the light absorption capacity of the material, it greatly reduces the lifetime of photogenerated carriers. Theoretical calculations indicate that Mn doping increases the non-radiative coupling coefficient in the photocatalyst, thereby suppressing photocatalytic efficiency. This study provides an important basic understanding for rational doping optimization of photocatalytic efficiency, and also provides new methods and ideas for the treatment of chlorophenols in scenic spots. |
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