不同尺寸反应器内H2O2热分解氧化NO特性与氧化产物分析

doi:10.11949/j.issn.0438-1157.20180377

化工学报 ›› 2018, Vol. 69 ›› Issue (9): 4037-4043.DOI: 10.11949/j.issn.0438-1157.20180377

不同尺寸反应器内H₂O₂热分解氧化NO特性与氧化产物分析

赵海谦¹, 董明¹, 汪怀远², 刘立君¹, 李栋¹, 刘晓燕¹

1. 东北石油大学土木建筑工程学院, 黑龙江大庆 163318;
2. 东北石油大学化学化工学院, 黑龙江大庆 163318

收稿日期:2018-04-08 修回日期:2018-05-10 出版日期:2018-09-05 发布日期:2018-09-05
通讯作者: 刘晓燕
基金资助:
国家自然科学基金项目（51606036）；黑龙江省普通本科高等学校青年创新人才培养计划（UNPYSCT-2016085）；黑龙江省青年科学基金项目（QC2014C047）。

Characteristics and product generation pathway of NO oxidation by H₂O₂ thermal decomposition in different size reactors

ZHAO Haiqian¹, DONG Ming¹, WANG Huaiyuan², LIU Lijun¹, LI Dong¹, LIU Xiaoyan¹

1. School of Civil Engineering & Architecture, Northeast Petroleum University, Daqing 163318, Heilongjiang, China;
2. Chemistry and Chemical Engineering School, Northeast Petroleum University, Daqing 163318, Heilongjiang, China

Received:2018-04-08 Revised:2018-05-10 Online:2018-09-05 Published:2018-09-05
Supported by:
supported by the National Natural Science Foundation of China (51606036), Innovative Talents Training Plan for Youth Scholars in Heilongjiang Province (UNPYSCT-2016085) and Heilongjiang Science Funds for Youths (QC2014C047).

摘要/Abstract

摘要：

采用实验方法研究了不同尺寸滴管炉反应器内H₂O₂热分解氧化NO特性。对比了不同H₂O₂蒸发条件对NO氧化率的影响规律。分析了气体温度、H₂O₂溶液浓度、H₂O₂：NO摩尔比、NO初始浓度及气体流量对NO氧化率的影响。检测了氧化产物并分析了产物的生成路径。结果表明：H₂O₂的快速蒸发是其热分解氧化NO的前提。减小H₂O₂液滴尺寸或液膜厚度可加速H₂O₂蒸发与分解，提高NO氧化率，扩宽NO氧化的温度范围。保证蒸发速率可削弱H₂O₂浓度对NO氧化率的影响。当H₂O₂：NO < 10时，NO氧化率随H₂O₂：NO的增加而增加；当H₂O₂：NO>10时，NO氧化率几乎不随H₂O₂：NO变化。H₂O₂热分解对于较高浓度的NO具有更高的氧化效率。H₂O₂热分解氧化NO的主要产物为NO₂。HO₂·直接将NO氧化为NO₂，·OH则先将NO转化为HONO，然后进一步氧化为NO₂。

关键词: H₂O₂热分解, NO, 氧化, 蒸发条件, 反应器

Abstract:

Characteristics of NO oxidation by H₂O₂ thermal decomposition in different size reactors in drop tube furnaces were studied. The effects of different H₂O₂ evaporation conditions on NO oxidation ratio were compared. The effects of gas temperature, H₂O₂ concentration, H₂O₂:NO, initial NO concentration and gas flow rate on NO oxidation ratio were analyzed. The oxidation product was detected and the generation pathway of the product was analyzed. The results showed that the rapid evaporation of H₂O₂ was the precondition for NO oxidation by H₂O₂ thermal decomposition. Reducing H₂O₂ droplet size or liquid film thickness could accelerate H₂O₂ evaporation and decomposition rate which enhanced NO oxidation ratio and broadened the NO oxidation temperature range. Ensuring the evaporation rate of H₂O₂ decreased the effect of H₂O₂ concentration on NO oxidation. When H₂O₂:NO < 10, the NO oxidation ratio increased with the increase of H₂O₂:NO; when H₂O₂:NO>10, the NO oxidation ratio did not change with it. H₂O₂ thermal decomposition had higher oxidation efficiency for high concentrations of NO. The main product of NO oxidation by H₂O₂ thermal decomposition was NO₂. HO₂· directly oxidized from NO to NO₂. However, ·OH converted NO to HONO firstly, and then further oxidized HONO to NO₂.

Key words: H₂O₂ thermal decomposition, NO, oxidation, evaporation conditions, reactor

中图分类号:

X511

赵海谦, 董明, 汪怀远, 刘立君, 李栋, 刘晓燕. 不同尺寸反应器内H₂O₂热分解氧化NO特性与氧化产物分析[J]. 化工学报, 2018, 69(9): 4037-4043.

ZHAO Haiqian, DONG Ming, WANG Huaiyuan, LIU Lijun, LI Dong, LIU Xiaoyan. Characteristics and product generation pathway of NO oxidation by H₂O₂ thermal decomposition in different size reactors[J]. CIESC Journal, 2018, 69(9): 4037-4043.

参考文献 19

[1]	BEECKEN J, MELLQVIST J, SALO K, et al. Airborne emission measurements of SO2, NOx and particles from individual ships using a sniffer technique[J]. Atmospheric Measurement Techniques, 2014, 7(7):1957-1968.
[2]	中华人民共和国国家统计局. 中国统计年鉴[EB/OL]. http://www.stats.gov.cn/tjsj/ndsj/.2018-4-2. National Bureau of Statistics of China. China statistical yearbook[EB/OL]. http://www.stats.gov.cn/tjsj/ndsj/.2018-4-2.
[3]	YANG T, CUI C, SHEN Y, et al. A novel denitration cost optimization system for power unit boilers[J]. Applied Thermal Engineering, 2016, 96:400-410.
[4]	ZHANG X, SUN S, SUN R, et al. Effects of bias combustion on volatile nitrogen transformation[J]. Asia-Pacific Journal of Chemical Engineering, 2010, 5(3):473-478.
[5]	KO J H, PARK R S, JEON J K, et al. Effect of surfactant, HCl and NH3 treatments on the regeneration of waste activated carbon used in selective catalytic reduction unit[J]. Journal of Industrial and Engineering Chemistry, 2015, 32:109-112.
[6]	SADA E, KUMAZAWA H, KUDO I, et al. Absorption of lean NOx in aqueous solutions of NaClO2 and NaOH[J]. Industrial & Engineering Chemistry Process Design and Development, 1979, 18(2):275-278.
[7]	LIU Y, WANG Q, YIN Y, et al. Advanced oxidation removal of NO and SO2 from flue gas by using ultraviolet/H2O2/NaOH process[J]. Chemical Engineering Research and Design, 2014, 92(10):1907-1914.
[8]	ZAMANSKY V M, HO L, MALY P M, et al. Gas phase reactions of hydrogen peroxide and hydrogen peroxide/methanol mixtures with air pollutants[J]. Symposium (International) on Combustion, 1996, 26(2):2125-2132.
[9]	COLLINS M M, COOPER C D, DIETZ J D, et al. Pilot-scale evaluation of H2O2 injection to control NOx emissions[J]. Journal of Environmental Engineering, 2001, 127(4):329-336.
[10]	HAYWOOD J M, COOPER C D. The economic feasibility of using hydrogen peroxide for the enhanced oxidation and removal of nitrogen oxides from coal-fired power plant flue gases[J]. Journal of the Air & Waste Management Association, 1998, 48(3):238-246.
[11]	KASPER J M, CLAUSEN Ⅲ C A, COOPER C D. Control of nitrogen oxide emissions by hydrogen peroxide-enhanced gas-phase oxidation of nitric oxide[J]. Journal of the Air & Waste Management Association, 1996, 46(2):127-133.
[12]	LIMVORANUSORN P, COOPER C D, DIETZ J D, et al. Kinetic modeling of the gas-phase oxidation of nitric oxide using hydrogen peroxide[J]. Journal of Environmental Engineering, 2005, 131(4):518-525.
[13]	ALI-ZADE N I. Selective gas-phase oxidation of pyridine derivatives with hydrogen peroxide[J]. Kinetics and Catalysis, 2006, 47(1):64-69.
[14]	GLEMSER O, SAUER H. Handbook of Preparative Inorganic Chemistry[M]. New York:Academic Press, 1963.
[15]	BAULCH D L, COBOS C J, COX R A, et al. Evaluated kinetic data for combustion modelling[J]. Journal of Physical and Chemical Reference Data, 1992, 21(3):411-734.
[16]	WARNATZ J. Rate coefficients in the C/H/O system[M]//Combustion Chemistry. New York:Springer, 1984.
[17]	TSANG W, HERRON J T. Chemical kinetic data base for propellant combustion (Ⅰ):Reactions involving NO, NO2, HNO, HNO2, HCN and N2O[J]. Journal of Physical and Chemical Reference Data, 1991, 20(4):609-663.
[18]	LIGHTFOOT P D, COX R A, CROWLEY J N, et al. Organic peroxy radicals:kinetics, spectroscopy and tropospheric chemistry[J]. Atmospheric Environment. Part A. General Topics, 1992, 26(10):1805-1961.
[19]	赵海谦, 高继慧, 周伟, 等. Fe2+/H2O2体系内各种自由基在氧化NO中的作用[J]. 化工学报, 2015, 66(1):449-454. ZHAO H Q, GAO J H, ZHOU W, et al. Roles of varied radicals in NO oxidation by Fe2+/H2O2 system[J]. CIESC Journal, 2015, 66(1):449-454.

不同尺寸反应器内H₂O₂热分解氧化NO特性与氧化产物分析

Characteristics and product generation pathway of NO oxidation by H₂O₂ thermal decomposition in different size reactors

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