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增强潮湿条件下多组分挥发性有机化合物的光热氧化:不同氧活化途径中锰和钾的协同机制

Boosting the Photothermal Oxidation of Multicomponent VOCs in Humid Conditions: Synergistic Mechanism of Mn and K in Different Oxygen Activation Pathways.

作者信息

Yang Yang, Bi Fukun, Wei Jiafeng, Han Xiao, Gao Bin, Qiao Rong, Xu Jingcheng, Liu Ning, Zhang Xiaodong

机构信息

School of Environment and Architecture, University of Shanghai for Science and Technology, Shanghai 200093, China.

Zhejiang Institute of Quality Sciences, Hangzhou 310018, China.

出版信息

Environ Sci Technol. 2025 Jun 10;59(22):11341-11352. doi: 10.1021/acs.est.5c00953. Epub 2025 May 29.

DOI:10.1021/acs.est.5c00953
PMID:40439229
Abstract

The complexity of actual industrial emissions has brought significant challenges for volatile organic compounds (VOCs) purification. Herein, Mn and K atoms were incorporated into CoO/TiO through theoretical study, and its excellent properties were verified in experiments. The different pathways of oxygen activation by Mn and K were revealed by characterization experiments and theoretical calculations. Mn species effectually reduced the dissociation energy barrier of HO adsorbed on the surface, and the surface hydroxyl group promoted the dissociation of O and the formation of O under light and humid conditions. The introduction of K promoted the formation of more oxygen vacancies, which served as adsorption sites for gaseous O. Meanwhile, the electron transfer accelerated by K contributed to the activation of HO and the rapid production of OH under light. The synergistic effect of Mn and K successfully achieved simultaneous improvements in the activity, stability, and water resistance of CoO/TiO. Furthermore, the catalyst was applied to the degradation of multicomponent VOCs, and the reaction path was analyzed through the test of intermediates, along with an investigation of the interaction among different types of VOCs. This study provided a new idea for the theoretical optimization of polymetallic catalysts and the analysis of degradation paths for multicomponent VOCs.

摘要

实际工业排放的复杂性给挥发性有机化合物(VOCs)净化带来了重大挑战。在此,通过理论研究将锰(Mn)和钾(K)原子引入到CoO/TiO中,并在实验中验证了其优异性能。通过表征实验和理论计算揭示了Mn和K激活氧的不同途径。Mn物种有效降低了吸附在表面的HO的解离能垒,并且表面羟基在光照和潮湿条件下促进了O的解离和O的形成。K的引入促进了更多氧空位的形成,这些氧空位作为气态O的吸附位点。同时,K加速的电子转移有助于HO的激活以及光照下OH的快速产生。Mn和K的协同作用成功实现了CoO/TiO的活性、稳定性和耐水性的同时提高。此外,将该催化剂应用于多组分VOCs的降解,并通过中间体测试分析了反应路径,同时研究了不同类型VOCs之间的相互作用。本研究为多金属催化剂的理论优化和多组分VOCs降解路径分析提供了新思路。

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