气相臭氧氧化协同湿法吸收脱硝技术的性能和氮转化

孙也; 李帅帅; 庞琳琳; 胡小吐; 李杰; 刘勇; 钟璐; 朱天乐

doi:10.13205/j.hjgc.202211024

气相臭氧氧化协同湿法吸收脱硝技术的性能和氮转化

doi: 10.13205/j.hjgc.202211024

孙也¹,
李帅帅¹,
庞琳琳¹,
胡小吐²,
李杰³,
刘勇²,
钟璐²,
朱天乐^1, ,

1. 北京航空航天大学空间与环境学院, 北京 102206;
2. 广东佳德环保科技有限公司, 广州 510663;
3. 唐山燕山钢铁有限公司, 河北唐山 130220

基金项目:

广东省企业科技特派员项目（GDKTP2020032900）

详细信息

作者简介:
孙也(1985-),女,高级实验师,主要研究方向为大气污染控制工程。suny@buaa.edu.cn

通讯作者:
朱天乐(1963-),男,教授,主要研究方向为大气污染控制工程。zhutl@buaa.edu.cn

计量
- 文章访问数: 87
- HTML全文浏览量: 19
- PDF下载量: 6
- 被引次数: 0
出版历程
- 收稿日期: 2021-12-17
- 网络出版日期: 2023-03-24

NO REMOVAL AND NITROGEN CONVERSION PERFORMANCE BY O₃ OXIDATION COMBINED WITH WET ABSORPTION

1. School of Space and Environment, Beihang University, Beijing 102206, China;
2. Guangdong J-Tech Environment Science Co., Ltd, Guangzhou 510663, China;
3. Yanshan Iron and Steel Co., Ltd, Tangshan 130220, China

摘要

摘要: 气相臭氧氧化协同湿法吸收脱硝技术具有脱除效率高、设备简单、投资低、运行易控等优点，适用于钢铁烧结、焦炉和陶瓷等较低温度（<150℃）和较低NO_x浓度（<400 mg/m³）烟气的深度净化。从理论上分析了臭氧氧化协同湿法吸收脱硝反应过程物理化学行为，并采用傅里叶红外光谱和离子色谱等方法，分别考察了气相臭氧氧化NO和气相臭氧氧化协同湿法吸收脱硝的氮产物分布，计算氮转化率。结果表明：n（O₃）：n（NO）和水溶性是影响NO氧化程度和氧化产物吸收脱除效率的关键因素。当n（O₃）：n（NO）>1.5时，NO的氧化产物是与SO₂水溶性相当的N₂O₅和HNO₃，均可实现在传统脱硫吸收塔中同步高效脱除，而且产物为稳定性良好的NO₃^-。氮平衡分析结果表明，氮转化率接近99%，而不可检测的氮组分可以忽略不计或者不存在。
- 臭氧氧化 /
- 吸收 /
- 脱硝 /
- 化学行为 /
- 水溶性 /
- 氮转化
Abstract: The denitrification technology using ozone oxidation combined with wet absorption can be used in the purification of flue gas with relatively low temperature (<150℃) and NO_x concentration (<400 mg/m³), such as the flue gas from steel sintering, coke oven and ceramics industries. The technology has the advantages of higher SO₂ and NO_x removal efficiency, simpler equipment, relatively lower construction and operation cost. The physicochemical behaviors of ozone oxidation combined with the liquid phase absorption denitrification process was firstly analyzed. The distribution of nitrogen products from both gas-phase NO oxidation and gas-phase oxidation combined with wet absorption were investigated by Fourier infrared spectroscopy and ion chromatography, and the nitrogen conversion was calculated. The results showed that the O₃/NO molar ratio and water solubility were the key factors affecting the degree of NO oxidation and NO_x removal efficiency. When the O₃/NO molar ratio was higher than 1.5, NO oxidation products were mainly N₂O₅ and HNO₃, and their water solubility was equivalent to SO₂. Thus, NO_x could be effectively removed in the traditional desulfurization absorber, and the product was NO₃^- with good stability. The nitrogen conversion rate was close to 99%, and the undetectable nitrogen components could be ignored or never exist.
- ozone oxidation /
- absorption /
- denitrification /
- molecular diffusion /
- water solubility /
- nitrogen conversion

HTML全文

参考文献(22)

[1]	朱法华, 张静怡, 徐振. 我国工业烟气治理现状、困境及建议[J]. 中国环保产业, 2020(10):13-16.
[2]	田恬, 程茜, 赵雪, 等. 2019年脱硫脱硝行业发展评述及展望[J].中国环保产业, 2020(2):23-25,28.
[3]	王新东, 侯长江, 田京雷. 钢铁行业烟气多污染物协同控制技术应用实践[J]. 过程工程学报, 2020, 20(9):997-1007.
[4]	GUO Y Y, LI YR, ZHU T Y, et al. Effects of concentration and adsorption product on the adsorption of SO₂ and NO on activated carbon[J]. Energy & Fuels, 2013, 27(1):360-366.
[5]	侯长江, 田京雷, 王倩. 臭氧氧化脱硝技术在烧结烟气中的应用[J]. 河北冶金, 2019(3):67-70.
[6]	SI M, SHEN B X, ADWEK G, et al. Review on the NO removal from flue gas by oxidation methods[J]. Journal of Environmental Sciences, 2021, 101(3):49-71.
[7]	WANG Y, ZHU T L, WANG H. Oxidation and removal of NO from flue gas by DC corona discharge combined with alkaline absorption[J]. IEEE Transaction on Plasma Science, 2011, 39(2):704-710.
[8]	LI Y, CHE D F, YANG C L, et al. Engineering practice and economic analysis of ozone oxidation wet denitrification technology[J]. Chinese Journal of Chemical Engineering, 2021, 29(1):401-408.
[9]	CHASE J R W. NIST-JANAF thermochemical tables fourth edition[J]. Journal of Physical and Chemical Reference Data Monograph, 1998, 9:1-1951.
[10]	J. A. Dean. 兰氏化学手册[M].15版. 北京:科学出版社, 2003.
[11]	LIPPMANN H H, JESSER B, SCHURATH U. The rate constant of NO+O₃→NO₂+O₂ in the temperature range of 283-443 K[J]. International Journal of Chemical Kinetics, 1980, 12(8):547-554.
[12]	ATKINSON R, BAULCH D L, COX R A, et al. Evaluated kinetic and photochemical data for atmospheric chemistry:supplement Ⅳ:IUPAC subcommittee on gas kinetic data evaluation for atmospheric chemistry[J]. Atmospheric Environment, 1996, 30(22):3903-3904.
[13]	JI R J, WANG J, XU W Q, et al. Study on the key factors of NO oxidation using O₃:the oxidation product composition and oxidation selectivity[J]. Industrial & Engineering Chemistry Research, 2018, 57:14440-14447.
[14]	夏青, 陈常贵.《化工原理(下)》[M]. 天津:天津大学出版社, 2008, 93-95.
[15]	SANDER R. NIST chemistry webbook, SRD 69[DB/OL]. https://webbook.nist.gov/cgi/cbook.cgi?ID=C7446095&Units=SI&Mask=10#Solubility.
[16]	SUN C L, ZHAO N, ZHUANG Z K, et al.Mechanisms and reaction pathways for simultaneous oxidation of NO_x and SO₂ by ozone determined by in situ IR measurements[J]. Journal of Hazardous materials, 2014, 274(12):376-383.
[17]	JI R J, WANG J, XU W Q, et al. Study on the key factors of NO oxidation using O₃:the oxidation product composition and oxidation selectivity[J]. Industrial & Engineering Chemistry Research, 2018, 57, 14440-14447.
[18]	GUO S P, LV L N, ZHANG J, et al. Simultaneous removal of SO₂ and NO_x with ammonia combined with gas-phase oxidation of NO using ozone[J]. Chemical Industry & Chemical Engineering Quarterly, 2015, 21(2):305-310.
[19]	ZHANG J, ZHANG R, CHEN X, et al. Simultaneous removal of NO and SO₂ from flue gas by ozone oxidation and NaOH absorption[J]. Industrial & Engineering Chemistry Research, 2014, 53(15):6450-6456.
[20]	SUN B C, SHENG M P, GAO W L, et al. Absorption of nitrogen oxides into sodium hydroxide solution in a rotating packed bed with pre-oxidation by ozone[J]. Energy & Fuels, 2017, 31(10):11019-11025.
[21]	SUN W Y, DING S L, ZENG S S, et al. Simultaneous absorption of NO_x and SO₂ from flue gas with pyrolusite slurry combined with gas-phase oxidation of NO using ozone[J]. Journal of Hazardous materials, 2011, 192(1):124-130.
[22]	SUN C L, ZHAO N, WANG H Q, et al. Simultaneous absorption of NO_x and SO₂ using magnesia slurry combined with ozone oxidation[J]. Energy & Fuels, 2015, 29(5):3276-3283.