添加剂CH3COONH4对介质阻挡-电晕放电耦合法脱除NO、SO2的影响

doi:10.16085/j.issn.1000-6613.2019-0152

摘要/Abstract

摘要：

采用自行研究设计的介质阻挡-电晕放电等离子体反应装置在模拟烟气中进行NO、SO₂的脱除研究。考察了O₂、CO₂、水蒸气等气体组分对脱除NO、SO₂的影响，并进一步探讨了添加剂CH₃COONH₄对脱除NO、SO₂的影响及作用机理。实验结果表明：O₂、CO₂和水蒸气浓度的增加对NO脱除有抑制作用，而引入CH₃COONH₄后，这些抑制作用会被减弱，使NO的脱除率得到大幅度提升，但这些抑制作用不会完全消除。在引入CH₃COONH₄后，气体组分和输入电流的变化对脱除SO₂的影响不明显，SO₂脱除率可达到94%左右。在N₂/O₂/CO₂/H₂O/NO/SO₂体系中加入0.27%的CH₃COONH₄后，NO初始浓度不变的条件下，SO₂含量较少时，对NO的脱除影响不明显，随着SO₂浓度的增加，NO的脱除率不断下降，增加CH₃COONH₄的添加量可消除SO₂的影响；另一方面，在SO₂初始浓度恒定的条件下，随着NO含量的增加，SO₂的脱除率保持在94%左右。在N₂/O₂/CO₂/H₂O/NO/SO₂体系中加入0.51%的CH₃COONH₄后，输入电流2.5A时，NO的脱除率达到72%。

关键词: 脱硫脱硝, 介质阻挡-电晕放电, CH₃COONH₄, 气体组分, 脱除效率

Abstract:

The removal of NO and SO₂ in simulated flue gas was studied by self-designed dielectric barrier - corona discharge plasma reactor. The effects of gas composition such as O₂ concentration, CO₂concentration and water vapor on the removal of NO and SO₂ were investigated. The effect of additive CH₃COONH₄ on NO and SO₂ removal and its mechanism of action were also discussed. Experimental results showed that the increase of O₂ concentration, CO₂ concentration and H₂O vapor concentration would inhibit the removal of NO. After the introduction of CH₃COONH₄, these inhibitory effects would be weakened and the removal rate of NO would be greatly increased, but its inhibitory effects would not be completely eliminated. After the introduction of CH₃COONH₄ into N₂/O₂/SO₂ system, the influence of gas composition and input current on SO₂ removal was not obvious, and the removal rate of SO₂ could reach about 94%. When 0.27%CH₃COONH₄ was added into N₂/O₂/CO₂/H₂O/NO/SO₂ system, under the initial concentration of NO was constant, When the content of SO₂ was low, the effect on NO removal was not obvious, the removal rate of NO decreased with the increase of SO₂ concentration, the effect of SO₂ could be eliminated by increasing the addition of CH₃COONH₄. On the other hand, under the condition of constant initial concentration of SO₂, with the increase of NO content, the removal rate of SO₂ remained around 94%. When 0.51%CH₃COONH₄ was added into N₂/O₂/CO₂/H₂O/NO/SO₂ system, the removal rate of NO reached 72% when the input current was 2.5A.

Key words: desulfurization and denitrification, dielectric barrier-corona discharge, CH₃COONH₄, gas component, removal efficiency

中图分类号:

X511

阚青,杨岚,刘露,马晓迅. 添加剂CH₃COONH₄对介质阻挡-电晕放电耦合法脱除NO、SO₂的影响[J]. 化工进展, 2019, 38(10): 4786-4796.

Qing KAN,Lan YANG,Lu LIU,Xiaoxun MA. Effect of additive CH₃COONH₄ on removal of NO and SO₂ by dielectric barrier-corona discharge coupling method[J]. Chemical Industry and Engineering Progress, 2019, 38(10): 4786-4796.

图/表 17

图1 介质阻挡耦合电晕放电装置流程 1—NO；2—O2；3—N2；4—CO2；5—SO2；6—质量流量计；7—四通阀；8—混合器；9—水蒸气发生器；10—添加剂发生器；11—放电反应器；12—高压电源；13—质谱仪；14—烟气分析仪

图2 O2浓度对脱除NO、SO2的影响

图3 CO2浓度对脱除NO、SO2的影响

图4 NO、SO2浓度随时间的变化曲线

图5 NO、SO2浓度对彼此脱除的影响

图6 CH3COONH4加热温度对脱除NO的影响

图7 CH3COONH4添加量对NO、SO2脱除率的影响

图8 O2含量随放电时间的变化曲线

图9 在Ar/O2/NO体系中添加CH3COONH4时不同质荷比的离子电流随时间的变化曲线

图10 在Ar/O2/SO2体系中添加CH3COONH4时不同质荷比的离子电流随时间的变化曲线

图11 添加CH3COONH4后O2浓度对NO和SO2脱除率的影响

图12 添加CH3COONH4后CO2浓度对NO和SO2脱除率的影响

表1 不同体系中NO的脱除率

体系	NO脱除率/%
体系	添加0.27% CH₃COONH₄	未添加 CH₃COONH₄
N₂/O₂/NO	87.16	64.41
N₂/O₂/9%CO₂/NO	72.14	42.66
N₂/O₂/9%CO₂/0.3%H₂O/NO	71.01	37.79

表2 不同体系中SO2的脱除率

体系	SO₂脱除率/%
体系	添加0.27% CH₃COONH₄	未添加 CH₃COONH₄
N₂/O₂/SO₂	92.98	16.17
N₂/O₂/9%CO₂/SO₂	92.17	12.03
N₂/O₂/9%CO₂/0.3%H₂O/SO₂	94.53	21.18

图13 N2/O2/CO2/H2O/NO/SO2/CH3COONH4体系中NO、SO2浓度对彼此脱除的影响

图14 N2/O2/CO2/H2O/NO/SO2/CH3COONH4体系中CH3COONH4添加量对脱除NO的影响

图15 N2/O2/CO2/H2O/NO/SO2体系中引入CH3COONH4后固体产物红外谱图

参考文献 24

1	李戌敏 . 烟气脱硝技术在火电厂项目中的应用[J]. 技术与市场, 2017, 24(2): 73-74.
	LI Xumin . Application of flue gas denitrification technology in thermal power plant project [J]. Technology and Market, 2017, 24(2): 73-74.
2	高岩, 栾涛, 徐宏明, 等 . 焙烧温度对选择性催化还原催化剂表征及活性的影响[J]. 中国电机工程学报, 2013, 32(s1): 143-148.
	GAO Yan , LUAN Tao , XU Hongming , et al . Effect of calcination temperature on the characterization and activity of selective catalytic reduction catalysts [J]. Proceedings of CSEE, 2013, 32(s1):143-148.
3	刘新, 王树东 . 非热等离子体烟气脱硝中的二氧化硫、氨和温度的效应[J]. 化工学报, 2006, 57(10): 2411-2415.
	LIU Xin , WANG Shudong . Effects of sulfur dioxide, ammonia and temperature in non-thermal plasma flue gas denitration [J]. Journal of Industry and Engineering(China)，2006, 57(10): 2411-2415.
4	丁凝, 黄海涛, 李歆, 等 . 电晕等离子体烟气脱硫脱硝机理及影响因素探讨[J]. 安全与环境工程, 2008, 15(1): 25-29.
	DING Ning , HUANG Haitao , LI Xin , et al . Discussion on mechanism and influencing factors of corona plasma flue gas desulfurization and denitration [J]. Safety and Environmental Engineering, 2008, 15(1): 25-29.
5	杜旭 . 烟气成分对介质阻挡放电脱硫脱硝的影响[D]. 北京: 华北电力大学, 2012.
	DU Xu . Effect of flue gas composition on desulfurization and denitration by dielectric barrier discharge [D]. Beijing: North China Electric Power University, 2012.
6	LI Hua , TANG Xiaolong , YI Honghong , et al . Study on oxidation and decomposition properties of no in plasma [J]. Thermal Power Generation, 2010, 39(5): 9-17.
7	郭彬, 栾涛 . 介质阻挡放电低温等离子体脱硝性能研究[J]. 核聚变与等离子体物理, 2017 , 37(2): 236-243.
	GUO Bin , LUAN Tao . Study on denitrification performance of low temperature plasma by dielectric barrier discharge [J]. Nuclear Fusion and Plasma Physics, 2017, 37(2): 236-243.
8	DE BO I , HEYMAN J , VINCKE J . Dimethyl sulfide removal from synthetic waste gas using a flat poly(dimethyl siloxane)-coated composite membrane bioreactor [J]. Environmental Science & Technology, 2003, 37(18): 4228.
9	王承智, 胡莜敏, 石荣, 等 . 等离子体技术应用于气相污染物治理综述[J]. 环境污染与防治, 2006, 28(3): 205.
	WANG Chengzhi , HU Youmin , SHI Rong , et al . Review of plasma technology applied in the treatment of gaseous pollutants [J]. Environmental Pollution and Prevention, 2006, 28(3): 205.
10	孙保明, 尹水娥, 肖海平, 等 . 介质阻挡放电脱硫脱硝过程特性[J]. 化工学报, 2010, 61(2): 469-476.
	SUN Baoming , YIN Shuie , XIAO Haiping , et al . Characteristics of desulfurization and denitrification process by dielectric barrier discharge [J]. CIESC Journal , 2010, 61(2): 469-476.
11	KUNHARDT E . Generation of large volume atmospheric pressure non-equilibrium plasmas [J]. IEEE Trans. on Plasma Science, 2000, 28(1): 189-200.
12	SUZUKI N , NISHIMURA K , TOKUNAGA O , et al . Radiation treatment of exhaust gases: NO decompositionin NO-N₂ and NO-rare gas mixtures [J]. Journal of Nuclear Science and Technology, 1978, 15(8): 597-601.
13	YANG Lan , LIAN Ke , ZHANG Xiang , et al . Nitric oxide removal from flue gas using dielectric barrier discharge coupled with negative pulse corona [J]. Chemical Engineering Research & Design, 2019, 143: 170-179.
14	TSAI C H , YANG H H , JOU C J, et al . Reducing nitric oxide into nitrogen via a radio-frequency discharge [J]. Journal of Hazardous Materials, 2007, 143(1/2):409.
15	FUTAMURA S , ZHANG A , YAMAMOTO T . Behavior of N₂ and nitrogen oxides innon-thermal plasma chemical processing of hazardous air pollutants [J]. IEEE Transactions on Industry Applications, 2000, 36(6): 1507-1514.
16	孙明 . OH, NH₂自由基提高脉冲放电等离子体烟气脱硫效率的研究[D]. 大连: 大连理工大学, 2004.
	SUN Ming . OH, NH₂ radicals improve the efficiency of flue gas desulfurization in pulsed discharge plasma [D]. Dalian: Dalian University of Technology, 2004.
17	ZHAO Guibin , HU Xudong , ARGYLE M D , et al . Effect of CO₂ on nonthermal-plasma reactions of nitrogen oxides in N₂: ppm-level concentrations[J]. Industrial & Engineering Chemistry Research, 2005, 44(14): 3945-3946.
18	YIN Shuie , SUN Baomin , GAO Xudong , et al . Effect of relative humidity on removal of NO and SO₂ from flue gas in dielectric barrier discharge reactor [J]. Journal of Chinese Society of Power Engineering, 2010, 30(1):41-46.
19	ZHU Y M . Optimization off pulsed corona discharged for flue gas treatment [J]. Advances Environmental Science, 1997, 5(5): 75.
20	浦鹏, 刘啸, 彭亚东, 等 . 助剂(C₂H₄、NH₃)添加对AC/DC流光放电等离子体脱硝效果的影响[J]. 环境工程学报, 2017, 11(1): 483-489.
	PU Peng , LIU Xiao , PENG Yadong , et al . Effect of additives (C₂H₄, NH₃) addition on denitrification of AC/DC streamer discharge plasma [J]. Journal of Environmental Engineering, 2017, 11(1): 483- 489.
21	DINELL G . Pulse power electrostatic technologies for the control of flue gas emissions [J]. Journal of Electrostatics, 1990, 25(1): 23-40.
22	罗渝然 . 化学键能数据手册[J]. 科学通报, 2005, 50(8): 759.
	LUO Yuran . Chemical bond data sheet [J]. Chinese Science Bulletin, 2005, 50(8): 759.
23	李艳荣, 张香, 杨岚, 等 . 钠添加剂对介质阻挡-电晕放电耦合法尿素脱除NO的影响[J]. 化工进展, 2018, 37(5): 1978-1984.
	LI Yanrong , ZHANG Xiang , YANG Lan , et al . Effects of sodium additives on urea removal of NO by dielectric barrier-corona discharge coupling [J]. Chemical Industry and Engineering Progress, 2018, 37(5): 1978-1984.
24	冉艳雄 . Ni基催化剂上乙酸蒸汽重整反应机理研究[D]. 太原: 太原理工大学, 2017.
	RAN Yanxiong . Study on reaction mechanism of acetic acid steam reforming over Ni-based catalyst [D]. Taiyuan: Taiyuan University of Technology, 2017.

[1]	张辛亥, 赵思琛, 朱辉, 王凯, 张首石. 活性碳纤维负载型脱硫剂在矿井气体环境条件下的应用[J]. 化工进展, 2022, 41(S1): 415-423.
[2]	任高林, 张学伟, 魏强, 王永亮, 雷晨辉, 徐一慧, 马文鑫. 10种石灰石浆液箱搅拌机的选型与计算[J]. 化工进展, 2021, 40(S1): 50-60.
[3]	窦金孝,赵永奇,段晓谞,柴红宁,余江龙. 络合亚铁乙二醇-四丁基溴化铵低共熔溶剂协同吸收SO₂和NO[J]. 化工进展, 2020, 39(2): 453-460.
[4]	刘露, 骆嘉钦, 阚青, 马晓迅. 乙醇胺对介质阻挡耦合电晕放电同时脱除NO、SO₂的影响[J]. 化工进展, 2020, 39(11): 4685-4692.
[5]	李艳荣, 张香, 杨岚, 贺建勋, 闵小建, 樊英杰, 马晓迅. 钠添加剂对介质阻挡-电晕放电耦合法尿素脱除NO的影响[J]. 化工进展, 2018, 37(05): 1978-1984.
[6]	武传朋, 张晨昕, 郭大为, 毛安国. 还原法脱除烟气中SO_x和/或NO_x的研究进展[J]. 化工进展, 2017, 36(S1): 457-463.
[7]	范学友，贾勇，钟秦. 氨吸收法同时脱硫脱硝的实验研究[J]. 化工进展, 2012, 31(01 ): 213-216.
[8]	费广平，李瑞军，解东来，乔伟艳. 利用热导检测器实时检测混合气体组分含量的方法及装置 [J]. 化工进展, 2009, 28(12): 2257-.

添加剂CH₃COONH₄对介质阻挡-电晕放电耦合法脱除NO、SO₂的影响

Effect of additive CH₃COONH₄ on removal of NO and SO₂ by dielectric barrier-corona discharge coupling method

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 17

参考文献 24

相关文章 8

编辑推荐

Metrics

本文评价