光源和辐射变量对十钨酸盐催化乙苯氧化的影响

IF 4.8 2区化学 Q2 CHEMISTRY, PHYSICAL

Applied Catalysis A: General Pub Date : 2025-09-19 DOI:10.1016/j.apcata.2025.120560

Ziqi Zhou, Dan Zhao, Jing Liao, Yachun Liu, Chao Zhang, Zaihui Fu

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引用次数: 0

摘要

光催化氧化作为一种有潜力的绿色合成方案，已被应用于烃类生产含氧化合物，但由于光源和辐射变量对光能利用效率的影响研究不足，其大规模应用仍受到限制。本文以氧（O2）在MeCN-H2O-PhSO3H中选择性氧化乙苯（EB）生成苯乙酮（ACP）为模型反应，采用外部照明的方式，系统研究了不同LED灯带及其辐射变量对两种十钨酸盐（TMADT和TBADT）的光催化效率（周转率，TON）及相应的量子效率（QE）的影响。并与钨溴灯的内外照明方式进行了比较。结果表明，5050型LED灯带与TBADT的光谱匹配最好，而3528型LED灯带的光强更强，光氧化效果最高，分别为5.96 % QE和73.3 TON。此外，采用短距离大面积照明、薄而均匀的光反应溶液、流动供氧等方法也可在一定程度上提高TON或QE值。在TBADT的催化下，优选的3528 LED-1条带能有效触发O2氧化EB，在12 h的辐照下，EB转化率约为93.2 %，ACP选择性为86.6% %。本工作为提高光催化效率提供了有益的探索。

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Effect of light sources and radiation variables on decatungstate-catalyzed ethylbenzene oxidation by molecular oxygen

Photo-catalytic oxidation, as a potential green synthesis protocol, has been applied to produce oxygenates from hydrocarbons, however, its large-scale application is still limited to due to insufficient research on the efficiency of light energy utilization affected by light sources and radiation variables. In this work, with the selective oxidation of ethylbenzene (EB) to acetophenone (ACP) by oxygens (O₂) in MeCN-H₂O-PhSO₃H as the model reaction, the effects of various LED strips and their radiation variables on the photo-catalytic efficiency (turnover number, TON) of two decatungstate salts (TMADT and TBADT) and the corresponding quantum efficiency (QE) were investigated systematically by an external lighting way, which was compared to the internal and external lighting ways of tungsten-bromine lamps. The results showed that a 5050-type LED strip had the best spectral matching with TBADT, while another 3528-type LED strip had a stronger light intensity, providing the highest 5.96 % QE and 73.3 TON for the photo-oxidation, respectively. In addition, short-distance and large-area illumination, thin and homogeneous photo-reaction solution, and flowing supply O₂ were also adopted to improve the TON or QE value to some extent. Under the catalysis of TBADT, the preferred 3528 LED-1 strip could effectively trigger the oxidation of EB by O₂, providing ca. 93.2 % EB conversion and 86.6 % ACP selectivity under 12 h of irradiation. This work provides a beneficial exploration for improving photo-catalytic efficiency.

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来源期刊

Applied Catalysis A: General 化学-环境科学

CiteScore

9.00

自引率

5.50%

发文量

415

审稿时长

24 days

期刊介绍： Applied Catalysis A: General publishes original papers on all aspects of catalysis of basic and practical interest to chemical scientists in both industrial and academic fields, with an emphasis onnew understanding of catalysts and catalytic reactions, new catalytic materials, new techniques, and new processes, especially those that have potential practical implications. Papers that report results of a thorough study or optimization of systems or processes that are well understood, widely studied, or minor variations of known ones are discouraged. Authors should include statements in a separate section "Justification for Publication" of how the manuscript fits the scope of the journal in the cover letter to the editors. Submissions without such justification will be rejected without review.