大气压介质阻挡放电及协同催化剂脱硝研究进展

doi:10.16085/j.issn.1000-6613.2022-0351

化工进展 ›› 2022, Vol. 41 ›› Issue (12): 6644-6655.DOI: 10.16085/j.issn.1000-6613.2022-0351

大气压介质阻挡放电及协同催化剂脱硝研究进展

张维¹(), 汪宗御¹^,²(), 郭玉¹, 杨孟飞¹, 李政楷¹, 常超¹, 张继锋¹^,², 纪玉龙¹()

^1.大连海事大学轮机工程学院，辽宁大连 116026
^2.浙江清华长三角研究院，浙江嘉兴 314006

收稿日期:2022-03-08 修回日期:2022-05-26 出版日期:2022-12-20 发布日期:2022-12-29
通讯作者: 汪宗御,纪玉龙
作者简介:张维（1991—），男，博士研究生，研究方向为等离子体脱硝。E-mail：zhangwei090530@126.com。
基金资助:
中国博士后科学基金(2021M690496);国家重点研发计划(SQ2019YFE011597);国家自然科学基金(51876019);大连市杰出青年科技人才支持计划(2020RJ03);中央高校基本科研业务费(3132019331)

Research progress of NO _x removal by combination of atmospheric pressure dielectric barrier discharge and catalysis

ZHANG Wei¹(), WANG Zongyu¹^,²(), GUO Yu¹, YANG Mengfei¹, LI Zhengkai¹, CHANG Chao¹, ZHANG Jifeng¹^,², JI Yulong¹()

^1.Marine Engineering, Dalian Maritime University, Dalian 116026, Liaoning, China
^2.Yangtze Delta Region Institute of Tsinghua University, Jiaxing 314006, Zhejiang, China

Received:2022-03-08 Revised:2022-05-26 Online:2022-12-20 Published:2022-12-29
Contact: WANG Zongyu, JI Yulong

摘要/Abstract

摘要：

受绿色生态和可持续发展战略理念的驱动，废气排放对环境造成的危害备受关注。NO _x 作为废气的主要污染物之一，是废气污染物控制的重点与难点。基于此，本文介绍了传统后处理脱硝技术的优缺点及应用现状,回顾了介质阻挡放电（DBD）基础研究，分析了DBD脱硝性能，重点阐述了DBD协同催化剂脱硝及脱硝机理。分析指出：①DBD驱动电源与反应器结构是制约脱硝性能的关键因素；②单独DBD技术脱硝性能较差，而DBD协同催化填充床技术展现出优异的脱硝性能和较高的N₂选择性；③等离子体协同催化脱硝机理研究主要包括等离子体特征参数诊断、流体模型验证、等离子体传播机制分析以及原位表征，而在等离子体催化理论计算方面的研究较为缺乏。因此，未来DBD协同催化脱硝技术应立足如下几个方面发展：研发高功率、低能耗电源，提升废气NO _x 处理量；优化反应器结构，提升脱硝的效率与选择性；设计与构筑适宜于DBD环境的脱硝催化剂；深入全面分析DBD协同催化剂脱硝机理。

关键词: 介质阻挡放电, 催化剂, 填充床, 选择性, 脱硝机理

Abstract:

Driven by the concept of green ecology and sustainable development strategy, exhaust emissions to the environment has attracted much attention. As one of the main pollutants of exhaust gas, NO _x is the focus and difficulty of exhaust gas pollutant control. The advantages, disadvantages and application status of traditional post-treatment de-NO _x technologies are introduced. The basic researches of dielectric barrier discharge are reviewed. The synergistic de-NO _x performance and mechanism by DBD and catalyst are analyzed. It is pointed out that:①the DBD power supply and the reactor structure are the key factors restricting the de-NO _x performance; ②the de-NO _x performance of DBD only is not satisfactory, but the combination of DBD with catalytic packed bed exhibits excellent de-NO _x efficiency and high N₂ selectivity; ③the researches on de-NO _x mechanism of plasma-assisted catalyst mainly include plasma characteristic parameter diagnosis, fluid model verification, plasma propagation mechanism analysis and in-situ characterization. However, the research on the theoretical calculation of plasma catalysis is limited. Therefore, we propose that the future development of DBD de-NO _x technology should be based on ①the high-power and high-efficiency power supply to improve the NO _x treatment capacity; ②the reactor structure optimization to improve the de-NO _x efficiency and N₂ selectivity; ③suitable design and construct of the de-NO _x catalyst for DBD environment; ④the comprehensive analysis of the de-NO _x mechanism of DBD synergistic catalyst.

Key words: dielectric barrier discharge, catalyst, packed bed, selectivity, de-NO _x mechanism

中图分类号:

X511

张维, 汪宗御, 郭玉, 杨孟飞, 李政楷, 常超, 张继锋, 纪玉龙. 大气压介质阻挡放电及协同催化剂脱硝研究进展[J]. 化工进展, 2022, 41(12): 6644-6655.

ZHANG Wei, WANG Zongyu, GUO Yu, YANG Mengfei, LI Zhengkai, CHANG Chao, ZHANG Jifeng, JI Yulong. Research progress of NO _x removal by combination of atmospheric pressure dielectric barrier discharge and catalysis[J]. Chemical Industry and Engineering Progress, 2022, 41(12): 6644-6655.

图/表 13

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技术	主要反应原理	脱硝率	优缺点	应用现状	文献
SCR		80%~95%（中高温）	较成熟，但占用空间大，投资及运行成本高，催化剂昂贵且易中毒，并伴有氨逃逸	多用于排放量较大的燃煤电力、柴油机脱硝	[8]
SNCR		<80%（850~1100℃）	较成熟，投资及运行成本较低，氨逃逸较严重	多用于脱硝标准低的中小型煤电等行业	[9]
吸附法	碳基、沸石、分子筛等吸附NO NH₃还原吸附剂再生	80%~90%（常温）	设备简单，但吸附量小，吸附剂用量大，利用率低，再生困难	适用于NO _x 排放浓度较低的领域	[10]
氧化吸收法		>85%（常温）	操作简单，效率高，但投资及运行成本较高；NaClO₂、HClO₃价格昂贵，易腐蚀设备；H₂O₂易分解、耗量大	多用于石化行业及可用空间较小的旧船改造	[7]

技术	主要反应原理	脱硝率	优缺点	应用现状	文献
SCR		80%~95%（中高温）	较成熟，但占用空间大，投资及运行成本高，催化剂昂贵且易中毒，并伴有氨逃逸	多用于排放量较大的燃煤电力、柴油机脱硝	[8]
SNCR		<80%（850~1100℃）	较成熟，投资及运行成本较低，氨逃逸较严重	多用于脱硝标准低的中小型煤电等行业	[9]
吸附法	碳基、沸石、分子筛等吸附NO NH₃还原吸附剂再生	80%~90%（常温）	设备简单，但吸附量小，吸附剂用量大，利用率低，再生困难	适用于NO _x 排放浓度较低的领域	[10]
氧化吸收法		>85%（常温）	操作简单，效率高，但投资及运行成本较高；NaClO₂、HClO₃价格昂贵，易腐蚀设备；H₂O₂易分解、耗量大	多用于石化行业及可用空间较小的旧船改造	[7]

DBD结构设计	参数指标	主导因素	放电性能影响	应用现状
电极材料	紫铜、不锈钢、铝合金、钨等	电导率、焦耳热、二次电子发射系数	较弱	紫铜
电极结构	圆棒、螺纹、齿状等	电场强度、放电均匀度	较弱	圆棒/螺纹
电极直径	mm~cm量级	电场强度	显著	—
电介质材料	聚四氟乙烯、石英玻璃、陶瓷、聚合物/陶瓷复合材料	介电常数、电荷累积、击穿强度	显著	复合材料
放电间隙	mm量级	处理时间、单位体积功率、电源	显著	mm量级
装配形式	电极分段式结构、单体结构、多体复合结构	放电均匀度、能耗、等离子体空间分布能耗	显著	多段式结构多体复合结构

DBD结构设计	参数指标	主导因素	放电性能影响	应用现状
电极材料	紫铜、不锈钢、铝合金、钨等	电导率、焦耳热、二次电子发射系数	较弱	紫铜
电极结构	圆棒、螺纹、齿状等	电场强度、放电均匀度	较弱	圆棒/螺纹
电极直径	mm~cm量级	电场强度	显著	—
电介质材料	聚四氟乙烯、石英玻璃、陶瓷、聚合物/陶瓷复合材料	介电常数、电荷累积、击穿强度	显著	复合材料
放电间隙	mm量级	处理时间、单位体积功率、电源	显著	mm量级
装配形式	电极分段式结构、单体结构、多体复合结构	放电均匀度、能耗、等离子体空间分布能耗	显著	多段式结构多体复合结构

参数指标	电介质材料
参数指标	石英玻璃	耐热玻璃	莫来石	陶瓷
相对介电常数	3.8	4.6	6	9.6
激励电压	++++	+++	++	+
气隙电压	++++	+	++	+
电介质电压	++++	++++	++	+
微放电通道	++	+	+	++++
寿命	+	++	++	++++
电流	++	+	+	++++
电荷累积	++	+	+	++++
焦耳热损耗	++++	++++	+++	+
表面粗糙度	+	+	+++	++++

大气压介质阻挡放电及协同催化剂脱硝研究进展

Research progress of NO _x removal by combination of atmospheric pressure dielectric barrier discharge and catalysis

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模拟废气成分	反应条件	NO脱除效率/%	N₂选择性/%	文献
NO（500μL/L）、O₂（8%）、N₂	25℃、0.5L/min	22	0	[43]
NO（500μL/L）、O₂（8%）、N₂	25℃、0.5L/min	40	—	[44]
NO（500μL/L）、O₂（5%）、N₂	20℃、625mL/min	47	27	[45]
NO（400μL/L）、O₂（5%）、N₂	20℃、1L/min	56	11.2	[46]
NO（500μL/L）、O₂（5%）、N₂	20℃、0.1L/min	34	2	[47]

催化剂	模拟废气成分	反应条件	施加能量	脱除效率/%	N₂选择性/%	文献
V₂O₅-WO₃/TiO₂	NO（300μL/L）、O₂（10%）、N₂	100℃、2L/min	30J/L	88（NO _x ）	88	［56］
V₂O₅/TiO₂	NO（400μL/L）、O₂（10%）、N₂	150℃、5L/min	80J/L	80（NO _x ）	80	［60］
TiO₂	NO（570μL/L）、O₂（21%）、N₂	25℃、5L/min	9kV	55（NO）	—	［61］
HZSM-5	NO（540μL/L）、O₂（2.9%）、N₂	25℃、1L/min	900J/L	50（NO）	26	［57］
Mn-Cu/ZSM5	NO（500μL/L）、O₂（6%）、N₂	25℃、2L/min	480J/L	60（NO）	30	［62］
木纤维	NO（300μL/L）、O₂（5%）、N₂	25℃、1L/min	900J/L	77（NO）	59	［58］
竹炭	NO（500μL/L）、O₂（8%）、N₂	25℃、0.5L/min	800J/L	74（NO）	68	［43］
MnCe/Ti	NO（400μL/L）、O₂（6%）、N₂	25℃、5L/min	280J/L	86.9（NO）	—	［36］
MOFs-CuBTC	NO（500μL/L）、O₂（8%）、N₂	25℃、0.5L/min	700J/L	99.87（NO）	99.87	［44］

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大气压介质阻挡放电及协同催化剂脱硝研究进展

Research progress of NO x removal by combination of atmospheric pressure dielectric barrier discharge and catalysis

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Research progress of NO _x removal by combination of atmospheric pressure dielectric barrier discharge and catalysis