Characterization of tar partial oxidative reforming by dielectric barrier discharge using mixed toluene and benzene as model compounds

doi:10.16085/j.issn.1000-6613.2024-0799

Abstract

Abstract:

Biomass tar, one of the main by-products generated in the biomass gasification process, seriously hindered the efficient utilization of the gasification gas. In this study, partial oxidation of biomass tar was carried out in a dielectric barrier discharge (DBD) plasma reactor with mixed toluene and benzene as model compounds. In order to understand the reaction characteristics and thus potential of the approach, the effects of O₂ addition, discharge power and composition of the mixture on performances were investigated. The results indicated that the mixture of toluene and benzene could be converted efficiently through partial oxidation induced by DBD plasma. At 300℃, the highest toluene conversion of 100.0% and benzene conversion of 98.2% with an energy efficiency of 34.2g/kWh were achieved without catalysts usage, together with a sum of CO and CO₂ selectivity of 74.8%. Higher O₂ addition amount and discharge power obtained better performances by promoting mixture destruction and gas product production. The variation in composition of the mixture showed little effect on toluene destruction and gas products production, while the decrease of benzene concentration in the mixture reduced the conversion of benzene. Phenyl and benzyl radicals, important intermediates in the conversion of toluene and benzene, combined with fragments to form liquid products and were oxidized by active species to generate gas products.

Key words: tar, partial oxidation, dielectric barrier discharge, nonthermal plasma

摘要：

以典型焦油组分甲苯与苯的混合物为模型化合物，于介质阻挡放电反应器上开展等离子体部分氧化焦油研究。考察O₂添加量、放电功率、焦油混合物组成对甲苯与苯转化特性的影响。结果表明，介质阻挡放电部分氧化可高效转化甲苯与苯的混合物，300℃下可取得最高100.0%的甲苯转化率和98.2%的苯转化率，相应的总能量效率达34.2g/kWh，产物中CO与CO₂选择性之和可达74.8%。提高O₂添加量与放电功率可提高甲苯与苯混合物的转化率，并促进气相产物生成。焦油混合物中甲苯与苯比例的变化对气相产物生成和甲苯脱除影响不大，但苯脱除率随其中苯比例的降低而下降。苯基和苄基自由基是甲苯和苯转化过程中的重要中间产物，可与分子碎片反应生成液相产物，与含氧活性物质反应生成气相产物。

关键词: 焦油, 部分氧化, 介质阻挡放电, 低温等离子体

CLC Number:

YANG Lanmei, XU Bin, LIU Huacai, YANG Wenshen, YIN Xiuli, WU Chuangzhi. Characterization of tar partial oxidative reforming by dielectric barrier discharge using mixed toluene and benzene as model compounds[J]. Chemical Industry and Engineering Progress, 2025, 44(7): 3869-3878.

杨岚梅, 徐彬, 刘华财, 杨文申, 阴秀丽, 吴创之. 介质阻挡放电部分氧化典型焦油组分混合物的转化特性[J]. 化工进展, 2025, 44(7): 3869-3878.

Figures/Tables 10

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项目	M1	M2	M3	M4	M5
反应物	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈
比例	1∶0	0.75∶0.25	0.5∶0.5	0.25∶0.75	0∶1

项目	M1	M2	M3	M4	M5
反应物	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈	C₆H₆∶C₇H₈
比例	1∶0	0.75∶0.25	0.5∶0.5	0.25∶0.75	0∶1

等离子体	焦油	焦油浓度/g·m^-3	载气	温度/℃	转化率/%	能量效率/g·kW^-1·h^-1	参考文献
DBD	C₇H₈	33.0	H₂	400	99.2	2.0	[37]
GAD	C₇H₈	14.0	N₂	—	83.2	16.6	[20]
DBD	C₇H₈	27.3	气化燃气+O₂/N₂+O₂	300	100.0	25.7	[22]
GAD	C₁₀H₈	1.7	N₂+H₂O	—	85.0	5.7	[19]
DBD+Ni/Al₂O₃	C₇H₈	17.7	N₂+H₂O	< 200	52.0	2.6	[10]
RGAD+Ni/Al₂O₃	C₇H₈	20.0	N₂+H₂O	—	93.5	20.4	[38]
DBD+Ni-HAP	C₆H₆	130.0	N₂+H₂O	400	92.1	8.5	[39]
DBD+Ni1Al3	C₇H₈	180.0	N₂+H₂O	300	96.0	25.0	[40]
DBD	C₆H₆/C₇H₈	23.0	N₂+O₂	300	98.2/100.0	34.2	本文

等离子体	焦油	焦油浓度/g·m^-3	载气	温度/℃	转化率/%	能量效率/g·kW^-1·h^-1	参考文献
DBD	C₇H₈	33.0	H₂	400	99.2	2.0	[37]
GAD	C₇H₈	14.0	N₂	—	83.2	16.6	[20]
DBD	C₇H₈	27.3	气化燃气+O₂/N₂+O₂	300	100.0	25.7	[22]
GAD	C₁₀H₈	1.7	N₂+H₂O	—	85.0	5.7	[19]
DBD+Ni/Al₂O₃	C₇H₈	17.7	N₂+H₂O	< 200	52.0	2.6	[10]
RGAD+Ni/Al₂O₃	C₇H₈	20.0	N₂+H₂O	—	93.5	20.4	[38]
DBD+Ni-HAP	C₆H₆	130.0	N₂+H₂O	400	92.1	8.5	[39]
DBD+Ni1Al3	C₇H₈	180.0	N₂+H₂O	300	96.0	25.0	[40]
DBD	C₆H₆/C₇H₈	23.0	N₂+O₂	300	98.2/100.0	34.2	本文

保留时间/min	化合物	相对峰面积百分比/%
保留时间/min	化合物	M1	M3	M5
2.82	苯	63.1	39.2	10.1
4.35	甲苯	1.2	20.9	42.1
6.03	乙苯	—	—	0.8
7.88	苯甲醛	0.4	5.1	10.6
7.92	苯乙醚	0.5	0.6	0.5
8.09	苯酚	28.2	22.7	17.8
8.26	苯甲腈	3.5	3.9	4.0
9.06	3-甲基苯酚	—	0.8	1.8
9.28	2-羟基苯甲醛	0.2	0.4	0.6
9.31	2-甲基苯酚	0.2	1.9	3.4
9.67	4-甲基苯酚	—	2.5	4.4
9.910	2-甲氧基苯酚	0.1	0.1	0.1
10.01	3-甲基苄腈	—	—	0.5
10.24	2-甲基苯腈	—	—	0.4
11.08	苯甲酸	—	—	0.5
14.30	联苯	0.2	0.2	0.2
—	其他	2.4	1.7	2.2