School of Low-Carbon Energy and Power Engineering, China University of Mining and Technology, Xuzhou 221116, PR China; Jiangsu Smart Energy Technology and Equipment Engineering Research Center, Xuzhou 221116, PR China.
School of Low-Carbon Energy and Power Engineering, China University of Mining and Technology, Xuzhou 221116, PR China; Jiangsu Smart Energy Technology and Equipment Engineering Research Center, Xuzhou 221116, PR China.
J Hazard Mater. 2023 Apr 15;448:130894. doi: 10.1016/j.jhazmat.2023.130894. Epub 2023 Feb 2.
Non-thermal plasma (NTP) is emerging as an attractive method for decomposing volatile organic compounds (VOCs). In this paper, to study toluene degradation mechanism in air/HO dielectric barrier discharge (DBD) plasma, optical emission spectrometry (OES) was employed to in-situ monitor active species in plasma, with the permanent degradation products being detected by on-line mass spectrometry under various operations. A detailed kinetic model of NTP with incorporation of non-constant electron filed and thermal effects has also been established. A toluene degradation efficiency > 82% could be achieved at P = 115 W, C = 1000 ppm. The relative spectrum intensity of excited OH, O, H and N (AΣ) increased with increase of discharge power and was decreased at higher gas flowrates. Toluene degradation was mainly induced by oxidation of OH and O at afterglow stage, while part of toluene was decomposed by attack of electrons and reactive particles N (AΣ) in discharge stage. A toluene degradation pathway has been proposed as: toluene→benzyl→benzaldehyde→benzene→phenoxy→cyclopentadiene→polycarbenes/alkynol→CO/HO. Benzoquinone, benzaldehyde, cyclopentadiene and cyclopentadienyl are supposed to be important intermediates for the ring-opening of toluene. Clarification of toluene degradation behaviors at discharge and afterglowing stage could provide new insights for plasma-catalytic process in future.
非热等离子体(NTP)作为一种有吸引力的方法,正在被用于分解挥发性有机化合物(VOCs)。在本文中,为了研究空气中甲苯在介质阻挡放电(DBD)等离子体中的降解机制,采用了光学发射光谱(OES)原位监测等离子体中的活性物质,同时在不同操作条件下,通过在线质谱仪检测到永久性降解产物。还建立了一个详细的包含非恒定电子场和热效应的 NTP 动力学模型。在 P = 115 W、C = 1000 ppm 的条件下,甲苯的降解效率>82%。随着放电功率的增加,激发态 OH、O、H 和 N(AΣ)的相对光谱强度增加,而在较高的气体流速下则降低。甲苯的降解主要是由 OH 和 O 在余晖阶段的氧化作用引起的,而部分甲苯则是由电子和活性粒子 N(AΣ)在放电阶段的攻击引起的。提出了甲苯的降解途径为:甲苯→苄基→苯甲醛→苯→苯氧基→环戊二烯→多碳/炔醇→CO/HO。苯醌、苯甲醛、环戊二烯和环戊二烯基被认为是甲苯开环的重要中间体。阐明了放电和余晖阶段甲苯的降解行为,可为今后的等离子体-催化过程提供新的见解。