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室温下K改性OMS-2催化剂上甲苯的等离子体催化后分解:K负载量的影响及反应机理

The post plasma-catalytic decomposition of toluene over K-modified OMS-2 catalysts at ambient temperature: Effect of K loading amount and reaction mechanism.

作者信息

Jiang Nan, Li Xuechuan, Kong Xiaoqi, Zhao Yonghe, Li Jie, Shang Kefeng, Lu Na, Wu Yan

机构信息

Key Laboratory of Industrial Ecology and Environmental Engineering, MOE, Dalian University of Technology, Dalian 116024, China; Institute of Electrostatics and Special Power, School of Electrical Engineering, Dalian University of Technology, Dalian 116024, China.

Key Laboratory of Industrial Ecology and Environmental Engineering, MOE, Dalian University of Technology, Dalian 116024, China; School of Environmental Science & Technology, Dalian University of Technology, Dalian 116024, China.

出版信息

J Colloid Interface Sci. 2021 Sep 15;598:519-529. doi: 10.1016/j.jcis.2021.04.028. Epub 2021 May 2.

DOI:10.1016/j.jcis.2021.04.028
PMID:33951548
Abstract

The present work is devoted to study the post plasma-catalytic (PPC) degradation of toluene using packed-bed discharge (PBD) plasma over K-modified manganese oxide octahedral molecular sieve (OMS-2) catalysts at ambient temperature. Compared to plasma alone, PPC can significantly improve the toluene degradation and mineralization performance simultaneously, and the generation of discharge byproducts and organic intermediates is suppressed. The catalytic capacity of OMS-2 for toluene degradation is greatly promoted by tuning potassium ions (K) content in OMS-2 tunnel, which might be owing to the formation of more surface active oxygen species derived from weak Mn-O bonds, plenty of oxygen vacancies, as well as more superior low-temperature reducibility. Highest toluene degradation efficiency (89.4%) and CO selectivity (88.9%) can be achieved in plasma-catalysis system over K-modified OMS-2 sample with K/Mn molar ratio of 2 at the SIE of 658 J/L. A long-term stability test has also been successfully carried out to evaluate the stability of K-modified OMS-2 with the assistance of plasma. Possible reaction mechanism for plasma-catalytic degradation of toluene on K-modified OMS-2 catalyst has been proposed based on the plasma diagnosis, catalysts characterization, and organic intermediates identification. This work aims to gaina deeperunderstandingof plasma-catalytic degradation mechanism and provides an environmentally friendly and energy-efficient method for practical volatile organic compounds (VOCs) abatement in PPC process.

摘要

本工作致力于研究在室温下,利用填充床放电(PBD)等离子体在K改性八面体氧化锰分子筛(OMS-2)催化剂上对甲苯进行等离子体催化(PPC)降解。与单独的等离子体相比,PPC可以同时显著提高甲苯的降解和矿化性能,并抑制放电副产物和有机中间体的生成。通过调节OMS-2通道中的钾离子(K)含量,OMS-2对甲苯降解的催化能力得到极大提升,这可能归因于由弱Mn-O键形成的更多表面活性氧物种、大量氧空位以及更优异的低温还原性。在能量输入为658 J/L时,在K/Mn摩尔比为2的K改性OMS-2样品上的等离子体催化系统中可实现最高甲苯降解效率(89.4%)和CO选择性(88.9%)。还成功进行了长期稳定性测试,以评估在等离子体辅助下K改性OMS-2的稳定性。基于等离子体诊断、催化剂表征和有机中间体鉴定,提出了K改性OMS-2催化剂上甲苯等离子体催化降解的可能反应机理。本工作旨在更深入地了解等离子体催化降解机理,并为PPC过程中实际挥发性有机化合物(VOCs)的减排提供一种环境友好且节能的方法。

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