臭氧氧化结合硫代硫酸钠溶液喷淋同时脱硫脱硝

doi:10.11949/j.issn.0438-1157.20151536

化工学报 ›› 2016, Vol. 67 ›› Issue (5): 2041-2047.DOI: 10.11949/j.issn.0438-1157.20151536

臭氧氧化结合硫代硫酸钠溶液喷淋同时脱硫脱硝

杨业, 徐超群, 朱燕群, 林法伟, 马强, 王智化, 岑可法

浙江大学能源清洁利用国家重点实验室, 浙江杭州 310027

收稿日期:2015-10-12 修回日期:2015-11-25 出版日期:2016-05-05 发布日期:2016-05-05
通讯作者: 朱燕群
基金资助:
国家重点基础研究发展计划项目(2012CB214906);国家杰出青年科学基金项目(51422605)。

Simultaneous removal of SO₂ and NO_x by combination of ozone oxidation and Na₂S₂O₃solution spray

YANG Ye, XU Chaoqun, ZHU Yanqun, LIN Fawei, MA Qiang, WANG Zhihua, CEN Kefa

State Key Laboratory of Clean Energy Utilization, Zhejiang University, Hangzhou 310027, Zhejiang, China

Received:2015-10-12 Revised:2015-11-25 Online:2016-05-05 Published:2016-05-05
Supported by:
supported by the National Basic Research Program of China (2012CB214906) and the National Science Fund for Distinguished Young Scholars of China (51422605).

摘要/Abstract

摘要：

采用臭氧氧化结合湿法喷淋硫代硫酸钠溶液的方法开展模拟烟气同时脱硫脱硝实验研究。结果表明,采用臭氧氧化结合Na₂S₂O₃-NaOH溶液湿法喷淋可以实现NO_x和SO₂协同脱除:在O₃/NO摩尔比为1.1～1.2时,溶液中Na₂S₂O₃浓度的增加会提高系统的NO_x脱除效率,烟气中SO₂的存在会促进NO_x的脱除,当SO₂浓度为1030 mg·m^-3、2.0%Na₂S₂O₃溶液作为喷淋液时可实现较高的SO₂脱除效率,同时NO_x脱除效率可达70%以上;喷淋液pH在2.5～9范围内变化时提高浆液pH有利于NO_x的脱除,当pH 9时脱硝效率可达75%。180 min连续同时脱硫脱硝实验结果表明,硫代硫酸钠可有效促进NO_x的脱除,并实现SO₂较高的脱除效率,同时可实现系统同时脱硫脱硝连续稳定运行,喷淋吸收后烟气中NO_x的主要转化产物为NO₂^-, 该方法作为一种有效的同时脱硫脱硝技术,具有一定的工业应用推广前景。

关键词: 臭氧氧化, 污染, 烟道气, 同时脱硫脱硝, 硫代硫酸钠, 吸收

Abstract:

Ozone oxidation and Na₂S₂O₃ solution spray was combined to remove SO₂ and NO_x simultaneously. This coupling was studied experimentally. The results show that: SO₂ and NO_x can be eliminated simultaneously; at O₃/NO mole ratio 1.1—1.2, the NO_x removal efficiency increases with increasing concentration of Na₂S₂O₃; existence of SO₂ can facilitate removal of NO_x; the NO_x removal efficiency reaches 70% with low emission of SO₂ at Na₂S₂O₃concentration 2.0% and at SO₂ gas concentration 1030 mg·m^-3. Furthermore, the NO_x removal efficiency is enhanced with the pH of solution from 2.5 to 9, and reaches 75% at pH 9. The result of 3 hours running experiment indicates that NO_x and SO₂ can be removed efficiently and simultaneously and the stable and continuous operation is possible, because sodium thiosulfate can facilitate removal of NO_x and the NO_x is dominantly converted into NO₂^-. This process could be an efficient approach for eliminating SO₂ and NO_xsimultaneously and could have potential industrial application.

Key words: ozone oxidation, pollution, flue gas, simultaneous removal of SO₂ and NO_x, sodium thiosulfate, absorption

中图分类号:

X511

杨业, 徐超群, 朱燕群, 林法伟, 马强, 王智化, 岑可法. 臭氧氧化结合硫代硫酸钠溶液喷淋同时脱硫脱硝[J]. 化工学报, 2016, 67(5): 2041-2047.

YANG Ye, XU Chaoqun, ZHU Yanqun, LIN Fawei, MA Qiang, WANG Zhihua, CEN Kefa. Simultaneous removal of SO₂ and NO_x by combination of ozone oxidation and Na₂S₂O₃solution spray[J]. CIESC Journal, 2016, 67(5): 2041-2047.

参考文献 24

[1]	环境保护部, 中华人民共和国国家质量监督检疫总局. 火电厂大气污染物排放标准: GB 13223—2011 [S]. 北京: 中国环境科学出版社, 2011. Ministry of Environmental Protection, General Administration of Quality Supervision of the People's Republic of China. Emission standard of air pollutants for thermal power plants: GB 13223—2011[S]. Beijing: China Environmental Science Press, 2011.
[2]	CHENG J, ZHOU J H, LIU J Z, et al. Sulfur removal at high temperature during coal combustion in furnaces: a review [J]. Progress in Energy and Combustion Science, 2003, 29 (5): 381-405. DOI: 10.1016/S0360-1285(03)00030-3.
[3]	陈国庆, 高继慧, 黄启龙, 等. 钙基脱硫工艺协同脱硝技术研究进展 [J]. 化工进展, 2015, 34 (10): 3755-3761. DOI: 10.16085/j.issn.1000-6613.2015.10.036. CHEN G Q, GAO J H, HUANG Q L, et al. Research progress of SO2 and NOx synergistic removal by calcium-based desulfurization [J]. Chemical Industry and Engineering Progress, 2015, 34 (10): 3755-3761. DOI: 10.16085/j.issn.1000-6613.2015.10.036.
[4]	MAN C K, GIBBINS J R, WITKAMP J G, et al. Coal characterization for NOx prediction in air-staged combustion of pulverised coals [J]. Fuel, 2005, 84 (17): 2190-2195. DOI: 10.1016/j.fuel.2005.06.011.
[5]	MONLINA A, EDDINGS E G, PERSHING D W, et al. Nitric oxide destruction during coal and char oxidation under pulverized-coal combustion conditions [J]. Conbustion and Flame, 2004, 136 (3): 303-312. DOI: 10.1016/j.combustflame.2003.10.009.
[6]	CAI L G, SHANG X, GAO S Q, et al. Low-NOx coal combustion via combining decoupling combustion and gas reburning [J]. Fuel, 2013, 112:695-703. DOI: 10.1016/j.fuel.2011.12.028.
[7]	WANG Z H, ZHOU J H, ZHU Y Q, et al. Simultaneous removal of NOx,SO2 and Hg in nitrogen flow in a narrow reactor by ozone injection: experimental results [J]. Fuel Process Technology, 2007, 88 (8):817-823. DOI: 10.1016/j.fuproc.2007.04.001.
[8]	张相, 朱燕群, 王智化, 等. 臭氧氧化多种污染物协同脱除及副产物提纯的试验研究 [J]. 工程热物理学报, 2012, 33 (7): 1259-1262. ZHANG X, ZHU Y Q, WANG Z H, et al. Experimental research for multi-pollution control by ozone and by-product purification [J]. Journal of Engineering Thermophysics, 2012, 33 (7): 1259-1262.
[9]	SKALSKA K, MILLER J S, WILK M, et al. Nitrogen oxides ozonation as a method for NOx emission abatement [J]. Ozone: Science & Engineering, 2012, 34 (4): 252-258. DOI: 10.1080/01919512.2012.686869.
[10]	SKALSKA K, MILLER J S, LEDAKOWICZ S. Kinetics of nitric oxide oxidation [J]. Chemical Papers, 2010, 64 (2): 269-272. DOI: 10.2478/s11696-009-0105-8.
[11]	MOK Y S, LEE H J. Removal of sulfur dioxide and nitrogen oxides by using ozone injection and absorption-reduction technique [J]. Fuel Processing Technology, 2006, 87 (7): 591-597. DOI: 10.1016/j.fuproc.2005.10.007.
[12]	STANMATE E, CHEN W, JORGENSEN L, et al. IR and UV gas absorption measurements during NOx reduction on an industrial natural gas fired power plant [J]. Fuel, 2010, 89 (5):978-985. DOI: 10.1016/j.fuel.2009.11.044.
[13]	王智化. 燃煤多种污染物一体化协同脱除机理及反应射流直接数值模拟DNS的研究 [D]. 杭州: 浙江大学, 2005. WANG Z H. Mechanism study on multi-pollution control simultaneously during coal combustion and direct numerical simulation of reaction jets flow[D]. Hangzhou: Zhejiang University, 2005.
[14]	HIROTA K, KOJIMA T. Decomposition behavior of PCDD/F isomers in incinerator gases under electron-beam irradiation [J]. Bulletin of the Chemical Society of Japan, 2005, 78 (9): 1685-1690. DOI: 10.1246/bcsj.78.1685.
[15]	WANG Q, YAN J H, TU X, et al. Thermal treatment of municipal solid waste incinerator fly ash using DC double arc argon plasma [J]. Fuel, 2009, 88 (5): 955-958. DOI: 10.1016/j.fuel.2008.12.011.
[16]	CHIEN T W, CHU H. Removal of SO2 and NO from flue gas by wet scrubbing using an aqueous NaClO2 solution [J]. Journal of Hazardous Materials, 2000, 80 (1-3): 43-57. DOI: 10.1016/S0304-3894(00)00274-0.
[17]	张相. 臭氧结合钙基吸收多种污染物及副产物提纯的试验与机理研究 [D]. 杭州: 浙江大学, 2012. ZHANG X. Experimental and mechanism investigation on multi-pollutant absorption by ozone with calcium based scrubbing and by-product treatment [D]. Hangzhou: Zhejiang University, 2012.
[18]	MOK Y S. Absorption-reduction technique assisted by ozone injection and sodium sulfide for NOx removal from exhaust gas [J]. Chemical Engineering Journal, 2006, 118 (1/2): 63-67. DOI: 10.1016/j.cej.2006.01.011.
[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. DOI: 10.1021/ie403423p.
[20]	曹向禹, 崔崇威, 黄君礼. 硫代硫酸钠还原二氧化氯的动力学 [J]. 高校化学工程学报, 2007,21 (5): 803-807. CAO X Y, CUI C W, HUANG J L. Kinetics of chlorine dioxide reduction by thiosulfate [J]. Journal of Chemical Engineering of Chinese Universities, 2007, 21 (5): 803-807.
[21]	张明慧, 马强, 徐超群, 等. 臭氧氧化结合湿法喷淋对玻璃窑炉烟气同时脱硫脱硝实验研究 [J]. 燃料化学学报, 2015, 43 (1): 88-93. ZHANG M H, MA Q, XU C Q, et al. Simultaneous removal of NOx and SO2 from glass furnace flue gas by ozone oxidation and spray tower [J]. Journal of Fuel Chemistry and Technology, 2015, 43 (1): 88-93.
[22]	杜振. 湿式氨法烟气脱硫脱硝过程中NOx吸收的实验研究[D]. 杭州: 浙江大学, 2011. DU Z. Study of NOx absorption in ammonia-based wet flue gas desulfurization and denitrification process[D]. Hangzhou: Zhejiang University, 2011.
[23]	刘颖祖, 朱燕群, 马强, 等. 臭氧多脱副产物亚硝酸钙的复盐沉淀试验研究 [J]. 化工学报, 2014, 65 (12): 4965-4970. DOI: 10.3969/j.issn.0438-1157.2014.12.043. LIU Y Z, ZHU Y Q, MA Q, et al. Double-salt precipitation of Ca(NO2)2 derived from multi-pollution control process by ozone [J]. CIESC Journal, 2014, 65 (12): 4965-4970. DOI: 10.3969/j.issn.0438-1157.2014.12.043.
[24]	中华人民共和国卫生部, 中国国家标准化管理委员会. 臭氧发生器安全与卫生标准: GB 28232—2011 [S]. 北京: 中国标准出版社, 2011. Ministry of Health, Inspection and Quarantine of the People's Republic of China. Safety and sanitation standard for ozone generator: GB 28232—2011[S]. Beijing: Standards Press of China, 2011.

臭氧氧化结合硫代硫酸钠溶液喷淋同时脱硫脱硝

Simultaneous removal of SO₂ and NO_x by combination of ozone oxidation and Na₂S₂O₃solution spray

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臭氧氧化结合硫代硫酸钠溶液喷淋同时脱硫脱硝

Simultaneous removal of SO2 and NOx by combination of ozone oxidation and Na2S2O3 solution spray

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Simultaneous removal of SO₂ and NO_x by combination of ozone oxidation and Na₂S₂O₃solution spray