多弧等离子体去除甲苯的研究

doi:10.16258/j.cnki.1674-5906.2022.05.014

生态环境学报 ›› 2022, Vol. 31 ›› Issue (5): 990-998.DOI: 10.16258/j.cnki.1674-5906.2022.05.014

多弧等离子体去除甲苯的研究

张弛¹^,²(), 郑瓛¹^,², 倪国华¹^,^*(), 赵彦君¹^,²

1.中国科学院等离子体物理研究所,安徽合肥 230031
2.中国科学技术大学,安徽合肥 230026

收稿日期:2021-12-21 出版日期:2022-05-18 发布日期:2022-07-12
通讯作者: * 倪国华（1972年生）,男,研究员,博士。E-mail: ghni@ipp.ac.cn
* 倪国华（1972年生）,男,研究员,博士。E-mail: ghni@ipp.ac.cn
作者简介:张弛（1997年生）,男,硕士研究生,主要从事等离子体大气治理研究。E-mail: 3192053619@qq.com
基金资助:
国家自然科学基金项目(11875295);安徽超越环保科技股份有限公司技术中心固废处置与资源综合利用开放基金项目（2022年度）(2022-KYJJ-1)

Study on the Removal of Toluene by Multi-arc Plasma

ZHANG Chi¹^,²(), ZHENG Huan¹^,², NI Guohua¹^,^*(), ZHAO Yanjun¹^,²

1. Institute of Plasma Physics, Chinese Academy of Sciences, Hefei 230031, P. R. China
2. University of Science and Technology of China, Hefei 230026, P. R. China

Received:2021-12-21 Online:2022-05-18 Published:2022-07-12

摘要/Abstract

摘要：

随着中国对环境治理的深入进行,中国对挥发性有机化合物（Volatile Organic Compound,VOCs）治理的要求越来越高。在各种VOCs治理技术中,等离子体技术具有工艺流程简单,可处理污染物种类范围广,适用性强等优点,尤其适合处理大风量、低浓度的VOCs。非热电弧等离子体由于具有兼具冷、热等离子体的优势,拓宽了等离子体废气处理技术的应用范围,因而备受关注。然而,由于非热电弧固有的自磁压缩和热箍缩效应等属性,导致等离子体尺寸较小,制约了其在实际中的应用。该文通过自主研制的多弧等离子体处理VOCs废气反应器,选择代表性污染物甲苯作为被处理对象,考察了反应器中等离子体的特性,各种参数对甲苯废气处理效果的影响。结果表明,电弧电压随放电电流的增大而减小,随着工作气体流量的增大而增大。多弧等离子体放电区尺寸明显增大,约为相同输入功率单个电弧的1.4倍,并且由于多个电弧的相互作用,稳定性明显提高。甲苯去除率随着初始浓度和气体流量的增大而减小,在气体流量8 m³∙h^-1,平均放电功率410 W,初始质量浓度2000 mg∙m^-3的条件下时,能量效率达到最大值25.8 g∙kW^-1∙h^-1。通过在放电区域下方30 mm处使用堇青石负载纳米Pt催化剂,发现等离子体复合催化剂的使用可有助于促进甲苯的完全分解,显著提高甲苯向CO₂的转化,CO₂选择率均比不使用催化剂时高20%以上,在气体流量8 m³∙h^-1,平均放电功率490 W,初始质量浓度2000 mg∙m^-3的条件下,CO₂选择性达到最大值62%。甲苯降解的气相中间产物主要是苯和苯甲醛。

关键词: 等离子体, 多弧放电, 甲苯, 复合催化, 负载型催化剂, 堇青石

Abstract:

With the environmental improvement in China, the management of Volatile Organic Compounds (VOCs) are of more significance. Among various VOCs elimination technologies, plasma technology has the advantages including simple process, wide range of pollutants treatment, and strong applicability, suitable for the treatment of VOCs with large air volume and low concentration. Non-thermal arc plasma has the advantages of both cold and thermal plasma, which broadens the application of plasma waste gas treatment technology. However, due to the self-magnetic compression and thermal pinch effect of non-thermal arc, the size of plasma is small, and thus restricts its application in practice. In this paper, a self-developed multi-arc plasma reactor was developed to treat VOCs. Toluene was selected as the representative pollutant in the work. The characteristics of plasma in the reactor and the influence of various parameters on the treatment effect of toluene waste gas were investigated. The results showed that the arc voltage decreased with the increase of discharge current and increased with the increase of working gas flow rate. The size of the multi-arc plasma discharge zone increased obviously, about 1.4 times that of a single arc under the same condition of input power. Furthermore, the stability of the multi-arc plasma had significant improvement due to the interaction among arcs. The removal rate of toluene decreased with the increases of initial concentration and gas flow rate. Under the conditions of gas flow rate of 8 m³∙h^-1, discharge power of 410 W and initial concentration of 2000 mg∙m^-3, the energy efficiency was up to 25.8 g∙kW^-1∙h^-1. Catalyst enhanced the complete decomposition of toluene and significantly improved the conversion of toluene to CO₂ in the plasma reaction, which was cordierite supported nano-Pt placed 30mm below the discharge zone. The selectivity was over 20% higher than that without catalyst. Under the conditions of gas flow rate of 8 m³∙h^-1, discharge power of 490 W and toluene initial concentration of 2000 mg∙m^-3, the CO₂ selectivity reached a maximum of 62%. In addition, the main gas phase intermediates of toluene degradation were benzene and benzaldehyde.

Key words: plasma, multi-arc discharge, toluene, composite catalysis, supported catalyst, cordierite

中图分类号:

张弛, 郑瓛, 倪国华, 赵彦君. 多弧等离子体去除甲苯的研究[J]. 生态环境学报, 2022, 31(5): 990-998.

ZHANG Chi, ZHENG Huan, NI Guohua, ZHAO Yanjun. Study on the Removal of Toluene by Multi-arc Plasma[J]. Ecology and Environment, 2022, 31(5): 990-998.

图/表 13

图1 实验系统示意图

Figure 1 Schematic diagram of experimental system

图2 不同气体流量下电弧等离子体放电的V-I特性

Figure 2 V-I characteristics of arc plasma discharge at different gas flow rates

图3 放电产生的亮度区域的图像分析步骤（a）原始放电图像;（b）引入圆形观测区域;（c）将灰度图像转换为二进制图像

Figure 3 Image analysis steps of luminance area generated by discharge (a) original discharge image; (b) introduction of circular observation area; (c) conversion of grayscale image to binary image

图4 多弧放电与单弧放电的亮度面积比

Figure 4 Luminance area ratio of multi-arc discharge and single-arc discharge

图5 甲苯初始浓度对多弧与单弧能量效率的影响

Figure 5 Effect of initial concentrations of toluene on energy efficiency of multi-arc and single-arc

图6 甲苯初始浓度对甲苯去除率的影响

Figure 6 Effect of initial concentrations of toluene on removal rate

图7 甲苯初始浓度对能量效率的影响

Figure 7 Effect of initial concentration of toluene on energy efficiency

图8 气体流量对（a）甲苯去除率和（b）能量效率的影响

Figure 8 Effect of gas flow on (a) toluene removal rate and (b) energy efficiency

图9 气体副产物GC-MS分析图

Figure 9 GC-MS analysis diagram of gas by-products

图10 苯与苯甲醛的产生和降解途径

Figure 10 Benzene and benzaldehyde production pathway

图11 催化剂负载量对（a）去除率和（b）能量效率的影响

Figure 11 Effect of catalyst loading on (a) removal rate and (b) energy efficiency

图12 催化剂对CO2选择性的影响

Figure 12 Effect of catalyst on CO2 selectivity

表1 比较不同等离子体放电类型对甲苯的降解性能

Table 1 Comparison of the degradation performance of toluene by different plasma discharge types

放电类型 Discharge types	放电功率 Discharge power/ W	甲苯浓度 Toluene concentration/ (mg∙m^-3)	气体流量 Gasflow/ (L∙min^-3)	去除率 Removal rate/ %	CO₂选择性 CO₂ selectivity/ %	能量效率 Energy efficiency/ (g∙kW^-1∙h^-1)	参考文献 Reference
DBD协同催化 DBD cocatalysis	24.0	6170	0.25	96	91	3.7	Wang et al., 2017
DBD协同催化 DBD cocatalysis	0.5	440	0.50	99	25	26.1	Tang et al., 2013
DBD协同催化 DBD cocatalysis	56.5	700	10.00	71		5.3	Liang et al., 2015
DBD协同催化 DBD cocatalysis	1.8	206	0.10	98		0.7	Guo et al., 2007
电晕放电协同催化 Corona discharge cocatalysis	2.2	870	0.50	95	70	11.3	Yao et al., 2020
电晕放电协同催化 Corona discharge cocatalysis	5.2	410	0.20	62	52	0.6	Yao et al., 2020
电晕放电协同催化 Corona discharge cocatalysis	10.0	290	0.25	93	20	0.4	Mista et al., 2008
滑动弧放电 Sliding arc discharge	110	1800	30.00	59		17.5	Zheng et al., 2008
多弧等离子体协同催化 Multi-arc plasma cocatalysis	490.4	2000	116.67	84	62	24.1	本研究
多弧等离子体 Multi-arc plasm	490.4	2000	116.67	77	30	22.0	本研究

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多弧等离子体去除甲苯的研究

Study on the Removal of Toluene by Multi-arc Plasma

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