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C 点掺杂提高非热等离子体-催化剂体系中 TiO/5A 对甲苯降解的催化性能。

C-dot doping for enhanced catalytic performance of TiO/5A for toluene degradation in non-thermal plasma-catalyst system.

机构信息

School of Environmental and Chemical Engineering, Shanghai University, Shanghai, 200444, China.

Institute of Environment Safety and Pollution Control, Jinan University, Guangzhou, 510632, China.

出版信息

Environ Sci Pollut Res Int. 2022 Jan;29(2):2480-2492. doi: 10.1007/s11356-021-15840-z. Epub 2021 Aug 9.

Abstract

Non-thermal plasma (NTP) is gaining attention as a powerful tool to induce various reactions. The combination of NTP with catalysts has been successfully used to degrade volatile organic compounds (VOCs) for pollution control. In this study, a series of TiO-C/5A catalysts, synthesized by carbon dots (C-dots) that decorate TiO by sol-gel and wetness impregnation methods, were incorporated with a dielectric barrier discharge (DBD) reactor in a single-stage structure to degrade toluene at atmospheric pressure and room temperature. A proton-transfer reaction mass spectrometer and a CO analyzer were used to monitor the concentration variations of organic by-products and CO online. The effects of input power, mass ratio of C-dots/TiO (TiO/5A (0 wt%), TiO-C1/5A (2.5 wt%), TiO-C2/5A (5 wt%), TiO-C3/5A (10 wt%)), gas flow rate, initial concentration of toluene on the toluene degradation efficiency, and CO selectivity were studied. The plasma-catalyst hybrid system could effectively improve the energy efficiency and reaction selectivity, attaining a maximum toluene degradation efficiency of 99.6% and CO selectivity of 83.0% compared to 79.5% and 37.5%, respectively, using the conventional plasma alone. Moreover, the generation of organic by-products also declined dramatically, averaging only half as much in plasma alone. The results also indicated that the appropriate amount of C-dot doping could greatly improve the catalyst efficiency in the hybrid plasma system. This is because the interaction between C-dots and TiO favors the formation of photoelectron holes and reduces the energy band gap and the recombination rate of photogenerated electron holes, which facilitates the generation of more active species on the catalyst surface, thereby leading to a more effective degradation reaction. These observations will provide guidance for the interaction studies between NTP and catalysts, not only for the exploration of new chemical mechanisms of aromatic compounds, but also for the screening of favorable materials for the desired reactions.

摘要

非热等离子体(NTP)作为一种诱导各种反应的强大工具引起了人们的关注。NTP 与催化剂的结合已成功用于降解挥发性有机化合物(VOCs)以控制污染。在这项研究中,通过溶胶-凝胶和湿法浸渍法将碳点(C-dots)修饰 TiO,合成了一系列 TiO-C/5A 催化剂,然后将其与介质阻挡放电(DBD)反应器结合在一个单级结构中,以在大气压和室温下降解甲苯。使用质子转移反应质谱仪和 CO 分析仪在线监测有机副产物和 CO 的浓度变化。研究了输入功率、C-dots/TiO 的质量比(TiO/5A(0wt%)、TiO-C1/5A(2.5wt%)、TiO-C2/5A(5wt%)、TiO-C3/5A(10wt%))、气体流量、甲苯初始浓度对甲苯降解效率和 CO 选择性的影响。等离子体-催化剂混合系统可以有效地提高能量效率和反应选择性,与单独使用传统等离子体相比,甲苯的降解效率达到 99.6%,CO 的选择性达到 83.0%,而分别达到 79.5%和 37.5%。此外,有机副产物的生成也大幅下降,单独使用等离子体时仅为其一半。结果还表明,适量的 C-dot 掺杂可以大大提高混合等离子体系统中催化剂的效率。这是因为 C-dots 和 TiO 之间的相互作用有利于形成光生电子空穴,并降低能带隙和光生电子空穴的复合率,从而在催化剂表面产生更多的活性物质,从而导致更有效的降解反应。这些观察结果将为 NTP 与催化剂之间的相互作用研究提供指导,不仅为探索芳香族化合物的新化学机制提供指导,也为筛选所需反应的有利材料提供指导。

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