填充床介质阻挡放电脱除气化燃气中苯的研究

徐彬; 谢建军; 袁洪友; 阴秀丽; 吴创之

填充床介质阻挡放电脱除气化燃气中苯的研究

徐彬^{1, 2},
谢建军^1, ,,
袁洪友¹,
阴秀丽¹,
吴创之^{1, 2}

1.
中国科学院广州能源研究所, 中国科学院可再生能源重点实验室, 广东省新能源和可再生能源研究开发与应用重点实验室, 广东广州 510640
2.
中国科学院大学, 北京 100049

基金项目:

国家自然科学基金 51576200

广东省自然科学基金重大培育项目 2017B030308002

广东省科技计划项目 2017A010104009

详细信息

中图分类号: TK6
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- 被引次数: 0
出版历程
- 收稿日期: 2018-09-27
- 修回日期: 2019-03-01
- 网络出版日期: 2021-01-23
- 刊出日期: 2019-04-10

Experimental study on benzene removal of fuel gas in a packed-bed dielectric barrier discharge reactor

XU Bin^{1, 2},
XIE Jian-jun^{1
, ,},
YUAN Hong-you¹,
YIN Xiu-li¹,
WU Chuang-zhi^{1, 2}

1.
CAS Key Laboratory of Renewable Energy, Guangdong Provincial Key Laboratory of New and Renewable Energy Research and Development, Guangzhou Institute of Energy Conversion, Chinese Academy of Sciences, Guangzhou 510640, China
2.
University of Chinese Academy of Sciences, Beijing 100049, China

Funds:

the National Natural Science Foundation of China 51576200

the Natural Science Foundation of Guangdong Province of China 2017B030308002

the Science and Technology Project of Guangdong Province of China 2017A010104009

More Information

Corresponding author: XIE Jian-jun, E-mail: xiejj@ms.giec.ac.cn

摘要

摘要: 以生物质气化焦油典型组分——苯作为模型物，采用填充床介质阻挡放电（DBD）对气化燃气氛围中的苯进行脱除。考察了燃气组成、填充物种类、反应温度及催化剂还原方式对苯脱除的影响。结果表明，反应温度200 ℃时，空气气化燃气与水蒸气气化燃气氛围内的苯脱除率比较接近，但燃气中存在少量O₂会导致脱除率明显下降。并且，提高放电能量密度，使用高介电常数、高比表面积及孔容积的填充物能提高苯脱除率。采用传统还原和等离子体还原两种方式分别制得Ni/γ-Al₂O₃（C）、Ni/γ-Al₂O₃（P）催化剂，以Ni/γ-Al₂O₃（C）为DBD填充物，反应温度在230-330 ℃时，苯脱除率随温度升高而下降，330 ℃时达到最低脱除率11.6%；温度高于330 ℃，苯脱除率随温度急剧上升且在430 ℃达到最大值85.4%。等离子体还原可制得大比表面积及高分散性的Ni/γ-Al₂O₃（P），其苯脱除率随温度变化的趋势与Ni/γ-Al₂O₃（C）一致，但在430 ℃时达到更高的脱除率90.0%。苯脱除过程中燃气的甲烷化可提高出口燃气中CH₄浓度，但燃气的热值略有下降。
- 生物质气化 /
- 气化燃气 /
- 焦油 /
- 苯 /
- 低温等离子体 /
- 催化作用
Abstract: A packed-bed dielectric barrier discharge (DBD) reactor was developed to investigate the removal of biomass tar in fuel gas atmosphere, and benzene was used as the tar surrogate. The effects of fuel gas composition, packing materials, reaction temperature and reduction methods of catalysts on the removal efficiency of benzene were investigated. The results indicate that the benzene removal efficiency of air-gasification fuel gas is close to that of steam-gasification fuel gas at low temperatures, but the presence of O₂ in the fuel gas leads to a large drop in the removal efficiency. In addition, the enhancement of the plasma discharge power and the use of packing materials with higher permittivity, specific surface area and pore volume can improve the benzene removal efficiency. For the plasma-catalytic process, the combination of DBD plasma and Ni/γ-Al₂O₃ (C) shows a significant benzene removal potential. The benzene removal efficiency decreases with temperature from 230-330℃, reaching a minimum value of 11.6%, and then notably increases to 85.4% at 430℃. Furthermore, the combination of plasma and Ni/γ-Al₂O₃ (P), which is reduced by plasma under H₂ atmosphere, has a similar tendency of benzene removal behavior within the temperature range of 230-430℃, reaching a maximum removal efficiency of 90.0% at 430℃ due to higher specific surface area and nickel dispersion of Ni/γ-Al₂O₃ (P). Moreover, the increased CH₄ concentration induced by the methanation of the fuel gas and the slightly decreased heating value of the fuel gas are obtained in the plasma-catalytic process.
- biomass gasification /
- fuel gas /
- tar /
- benzene /
- non-thermal plasma /
- catalysis

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图 1 DBD焦油脱除实验装置示意图

Figure 1 Schematic diagram of the experimental setup

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图 2 5% NiO/γ-Al₂O₃催化剂的H₂-TPR谱图

Figure 2 H₂-TPR profiles of 5% NiO/γ-Al₂O₃

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图 3 不同燃气氛围对等离子体脱除苯的影响

Figure 3 Effect of carrier gas on the benzene removal efficiency as a function of specific energy input

reaction conditions: reaction temperature=200 ℃, packing material: γ-Al₂O₃ pellets

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图 4 不同填充物对等离子体脱除苯的影响

Figure 4 Effect of packing material on the benzene removal efficiency as a function of specific energy input

reaction conditions: reaction temperature=200 ℃, carrier gas: air-gasification fuel gas 1

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图 5 反应温度对等离子体脱除苯的影响

Figure 5 Effect of reaction temperature on the benzene removal efficiency

reaction conditions: specific energy input=~350 J/L, packing material: γ-Al₂O₃ pellets and Ni/γ-Al₂O₃(C), carrier gas: air-gasification fuel gas 1

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图 6 不同还原催化剂对等离子体脱除苯的影响

Figure 6 Effect of catalytic reduction method on the benzene removal efficiency

reaction conditions: specific energy input=~350 J/L, packing material: Ni/γ-Al₂O₃(P), carrier gas: air-gasification fuel gas 1

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图 7 不同还原方式催化剂的TEM照片

Figure 7 TEM images of Ni/γ-Al₂O₃ catalysts

(a): Ni/γ-Al₂O₃(P); (b): Ni/γ-Al₂O₃(C)

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图 8 不同反应温度下反应器出口处燃气各组分的浓度

Figure 8 Concentrations of H₂, CO, CO₂ and CH₄ at the outlet as a function of reaction temperature in plasma-catalytic process (a) and catalytic alone process (b)

reaction conditions: specific energy input=~350 J/L, packing material: Ni/γ-Al₂O₃(C), carrier gas: air-gasification fuel gas 1

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表 1 不同填充物的比表面积和孔结构

Table 1 Specific surface area and pore structure of packing materials

Packing material	Specific surface area A/(m²·g^-1)	Pore volume v/(cm³·g^-1)	Average diameter d/nm
Glass pellets	< 1	-	-
γ-Al₂O₃	94	0.343	7.3
Ni/γ-Al₂O₃(P)	84	0.311	7.4
Ni/γ-Al₂O₃(C)	79	0.312	7.8

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表 2 不同类型的燃气组成

Table 2 Gas components of different gasification fuel gases

Gas mixture	Component φ/%
Gas mixture	H₂	CO	CO₂	CH₄	N₂	O₂
Air-gasification fuel gas 1	15	18	12	1.5	53.5	-
Air-gasification fuel gas 2	10	22	15	3	50	-
Steam-gasification fuel gas	40	25	25	8	2	-
Oxygen-containing fuel gas	10	22	15	3	48	2

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表 3 不同等离子体反应器内焦油脱除性能对比

Table 3 Performance comparison of tar removal by different plasma reactors

Process	Target	Carrier gas	Q ^a/ (L·min^-1)	t/℃	Tar content/ (g·m^-3)	η/%	E/ (g·(kW·h)^-1)	SEI/ (kJ·L^-1)	Ref.
Microwave plasma	C₆H₆	N₂+H₂O	20.0	n.a.^b	15.0	90.0	8.8	6.0	[31]
AC gliding arc discharge	C₆H₆	N₂+H₂O	16.7	n.a.	3.7	82.6	20.9	0.61	[32]
AC gliding arc discharge	C₇H₈	N₂+H₂O	3.8	n.a.	23.5	35.8	46.3	0.68	[33]
Rotating gliding arc discharge	C₇H₈	N₂	10.0	n.a.	14.0	83.0	16.6	2.5	[10]
DBD with Ni/Al₂O₃	C₇H₈	N₂+H₂O	0.15	< 200	17.7	52.0	2.6	14.0	[12]
DBD with Ni/Al₂O₃	C₇H₈	N₂+H₂O	0.15	300	180.0	96.0	25.0	25.7	[13]
DBD with Ni/Al₂O₃	C₆H₆	Fuel gas	1.0	430	1.9	85.4	16.7	0.35	this work
^a: Q represents the total flow rate; ^b: n.a. = not available

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表 4 不同温度下等离子体结合催化剂反应器出口处的燃气低位热值

Table 4 LHV of fuel gas at the outlet as a function of reaction temperature in plasma-catalytic process

Reaction temperature	Q_LHV /(MJ·m^-3)	Growth rate /%
Air-gasification fuel gas 1	4.43	-
230 ℃	4.35	-1.7
280 ℃	4.36	-1.4
330 ℃	4.19	-5.3
380 ℃	4.18	-5.6
430 ℃	4.24	-4.4

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