Experimental study on SO2 recovery using a sodium-zinc sorbent based flue gas desulfurization technology

doi:10.1016/j.cjche.2014.10.007

Chinese Journal of Chemical Engineering ›› 2015, Vol. 23 ›› Issue (1): 241-246.DOI: 10.1016/j.cjche.2014.10.007

• 能源、资源与环境技术 • 上一篇下一篇

Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology

Yang Zhang¹, Tao Wang², Hairui Yang¹, Hai Zhang¹, Xuyi Zhang¹

1 Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Thermal Engineering, Tsinghua University, Beijing 100084, China;
2 National Engineering Laboratory of Coal-Fired Pollution Reduction, School of Energy and Power Engineering, Shandong University, Jinan 250061, China

收稿日期:2013-04-09 修回日期:2013-09-09 出版日期:2015-01-28 发布日期:2015-01-24
通讯作者: Hai Zhang
基金资助:
Supported by the National High Technology Research and Development Program of China (2009AA05Z302).

Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology

Yang Zhang¹, Tao Wang², Hairui Yang¹, Hai Zhang¹, Xuyi Zhang¹

1 Key Laboratory for Thermal Science and Power Engineering of Ministry of Education, Department of Thermal Engineering, Tsinghua University, Beijing 100084, China;
2 National Engineering Laboratory of Coal-Fired Pollution Reduction, School of Energy and Power Engineering, Shandong University, Jinan 250061, China

Received:2013-04-09 Revised:2013-09-09 Online:2015-01-28 Published:2015-01-24
Contact: Hai Zhang
Supported by:
Supported by the National High Technology Research and Development Program of China (2009AA05Z302).

摘要/Abstract

摘要： A sodium-zinc sorbent based flue gas desulfurization technology (Na-Zn-FGD) was proposed based on the experiments and analyses of the thermal decomposition characteristics of CaSO₃ and ZnSO₃·2.5H₂O, the waste products of calcium-based semi-dry and zinc-based flue gas desulfurization (Ca-SD-FGD and Zn-SD-FGD) technologies, respectively. Itwas found that ZnSO₃·2.5H₂O first lost crystal H₂O at 100 ℃ and then decomposed into SO₂ and solid ZnO at 260 ℃ in the air, while CaSO₃ is oxidized at 450 ℃ before it decomposed in the air. The experimental results confirm that Zn-SD-FGD technology is good for SO₂ removal and recycling, but with problem in clogging and high operational cost. The proposed Na-Zn-FGD is clogging proof, and more cost-effective. In the newprocess, Na₂CO₃ is used to generate Na₂CO₃ for SO₂ absorption, and the intermediate product NaHSO₃ reacts with ZnO powders, producing ZnSO₃·2.5H₂O precipitate and Na₂CO₃ solution. The Na₂CO₃ solution is clogging proof, which is re-used for SO₂ absorption. By thermal decomposition of ZnSO₃·2.5H₂O, ZnO is re-generated and SO₂ with high purity is co-produced as well. The cycle consumes some amount of raw material Na₂CO₃ and a small amount of ZnO only. The newly proposed FGD technology could be a substitute of the traditional semi-dry FGD technologies.

关键词: Flue gas desulfurization, Waste treatment, ZnSO₃·, 2.5H₂O pyrolysis, Sodium-zinc sorbent based, SO₂ co-production

Abstract: A sodium-zinc sorbent based flue gas desulfurization technology (Na-Zn-FGD) was proposed based on the experiments and analyses of the thermal decomposition characteristics of CaSO₃ and ZnSO₃·2.5H₂O, the waste products of calcium-based semi-dry and zinc-based flue gas desulfurization (Ca-SD-FGD and Zn-SD-FGD) technologies, respectively. Itwas found that ZnSO₃·2.5H₂O first lost crystal H₂O at 100 ℃ and then decomposed into SO₂ and solid ZnO at 260 ℃ in the air, while CaSO₃ is oxidized at 450 ℃ before it decomposed in the air. The experimental results confirm that Zn-SD-FGD technology is good for SO₂ removal and recycling, but with problem in clogging and high operational cost. The proposed Na-Zn-FGD is clogging proof, and more cost-effective. In the newprocess, Na₂CO₃ is used to generate Na₂CO₃ for SO₂ absorption, and the intermediate product NaHSO₃ reacts with ZnO powders, producing ZnSO₃·2.5H₂O precipitate and Na₂CO₃ solution. The Na₂CO₃ solution is clogging proof, which is re-used for SO₂ absorption. By thermal decomposition of ZnSO₃·2.5H₂O, ZnO is re-generated and SO₂ with high purity is co-produced as well. The cycle consumes some amount of raw material Na₂CO₃ and a small amount of ZnO only. The newly proposed FGD technology could be a substitute of the traditional semi-dry FGD technologies.

Key words: Flue gas desulfurization, Waste treatment, ZnSO₃·, 2.5H₂O pyrolysis, Sodium-zinc sorbent based, SO₂ co-production

Yang Zhang, Tao Wang, Hairui Yang, Hai Zhang, Xuyi Zhang . Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology[J]. Chinese Journal of Chemical Engineering, 2015, 23(1): 241-246.

Yang Zhang, Tao Wang, Hairui Yang, Hai Zhang, Xuyi Zhang . Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology[J]. Chin.J.Chem.Eng., 2015, 23(1): 241-246.

参考文献

[1] S. Kiil, M.L. Michelsen, K. Dam-Johansen, Experimental investigation and modeling of a wet flue gas desulfurization pilot plant, Ind. Eng. Chem. Res. 37 (7) (1998) 2792-2806.

[2] K. Hjuler, K. Dam-Johansen, Wet oxidation of residual product from spray absorption of sulphur dioxide, Chem. Eng. Sci. 49 (24) (1994) 4515-4521.

[3] M. Xie, P. Li, H. Guo, L. Gao, J. Yu, Ternary system of Fe-based ionic liquid, ethanol and water for wet flue gas desulfurization, Chin. J. Chem. Eng. 20 (1) (2012) 140-145.

[4] Y. Wu, E.J. Anthony, L. Jia, Reactivation properties of four long-term sulfated limestones, Energy Fuel 20 (6) (2006) 2421-2425.

[5] F. Montagnaro, P. Salatino, F. Scala, Y.Wu, E.J. Anthony, L. Jia, Assessment of sorbent reactivation by water hydration for fluidized bed combustion application, J. Energy Resour. Technol. 128 (2006) 90-98.

[6] C. Chen, C. Zhao, S. Liu, C. Wang, Direct sulfation of limestone based on oxy-fuel combustion technology, Environ. Eng. Sci. 26 (10) (2009) 1481-1488.

[7] J. Zhang, C. You, H. Qi, B. Hou, C. Chen, X. Xu, Effect of operating parameters and reactor structure onmoderate temperature dry desulfurization, Environ. Sci. Technol. 40 (13) (2006) 4300-4305.

[8] J. Zhang, C. You, S. Zhao, C. Chen, H. Qi, Characteristics and reactivity of rapidly hydrated sorbent for semidry flue gas desulfurization, Environ. Sci. Technol. 42 (5) (2008) 1705-1710.

[9] Y. Li, C. You, C. Song, Adhesive carrier particles for rapidly hydrated sorbent for moderate-temperature dry flue gas desulfurization, Environ. Sci. Technol. 44 (12) (2010) 4692-4696.

[10] L. Duan, X. Chen, Y. Li, C. Liang, C. Zhao, Investigation on SO₂ emission from 410 t/h circulating fluidized bed boiler burning petroleum coke and coal, Asia Pac. J. Chem. Eng. 5 (2) (2010) 274-280.

[11] F.J.G. Ortiz, P. Ollero, Flue-gas desulfurization in an advanced in-duct desulfurization process: an empirical model from an experimental pilot-plant study, Ind. Eng. Chem. Res. 42 (25) (2003) 6625-6637.

[12] P. Ollero, F.J.G. Ortiz, A. Cabanillas, J. Otero, Flue-gas desulfurization in circulating fluidized beds: An empirical model from an experimental pilot-plant study, Ind. Eng. Chem. Res. 40 (23) (2001) 5640-5648.

[13] R. Hallaj, M. Nikazar, B. Dabir, Thermogravimetric study and modeling of direct sulfation of limestone by sulfur dioxide, Chin. J. Chem. Eng. 12 (4) (2004) 566-569.

[14] J.M. Bigham, D.A. Kost, R.C. Stehouwer, J.H. Beeghly, R. Fowler, S.J. Traina, W.E. Wolfe, W.A. Dick, Mineralogical and engineering characteristics of dry flue gas desulfurization products, Fuel 84 (14-15) (2005) 1839-1848.

[15] D.A. Kost, J.M. Bigham, R.C. Stehouwer, J.H. Beeghly, R. Fowler, S.J. Traina, W.E. Wolfe, W.A. Dick, Chemical and physical properties of dry flue gas desulfurization products, J. Environ. Qual. 34 (2) (2005) 676-686.

[16] R. Liu, B. Guo, A. Ren, J. Bian, The chemical and oxidation characteristics of semi-dry flue gas desulfurization ash from a steel factory, Waste Manag. Res. 28 (10) (2010) 865-871.

[17] R.C. Stehouwer, P. Sutton,W.A. Dick, Transport and plant uptake of soil-applied dry flue gas desulfurization by-products, Soil Sci. 161 (9) (1996) 562-574.

[18] X.C. Qiao, C.S. Poon, C. Cheeseman, Use of flue gas desulphurisation (FGD)waste and rejected fly ash in waste stabilization/solidification systems, Waste Manag. 26 (2) (2006) 141-149.

[19] Y.B. Lee, J.M. Bigham,W.A. Dick, F.S. Jones, C. Ramsier, Influence of soil pH and application rate on the oxidation of calcium sulfite derived from flue gas desulfurization, J. Environ. Qual. 36 (1) (2007) 298-304.

[20] L. Liu, S. Zhang, X. Lü, X. Yu, S. Zhi, Ozonation of sulfur dioxide in sulphuric acid solution, Chin. J. Chem. Eng. 21 (7) (2013) 808-812.

[21] N. Zou, Adsorption of SO₂ from jarosite roasting with zinc dust slurry in Laibin smelter, Nonferrous Met. 54 (4) (2002) 111-113.

[22] Y.X. Li, S.B. Zhang, H.X. Guo, B. Zhong, Application of the shrinking core model to the kinetics of zinc oxide desulfurization, Chin. J. Chem. Eng. 5 (4) (1997) 296-303.

[23] N. Chen, Experimental research and commercial operation of zinc oxide process for treating low-SO₂ gas, Sulphuric Acid Ind. 4 (2004) 9-14.

[24] M. Huang, J. Zhang, SO₂ removal with ash containing zinc oxide, Chem. Ind. Eng. Prog. 26 (5) (2007) 720-724 (in Chinese).

[25] J. Zhang, Z. Tong, The study of acidic decomposition zinc sulfite, Nat. Sci. J. Xiangtan Univ. 24 (1) (2002) 71-74 (in Chinese).

[26] J. Zhang, Z. Tong, The study on reaction of zinc sulfite by blasting air, Nat. Sci. J. Xiangtan Univ. 24 (2) (2002) 49-53 (in Chinese).

[27] S.Wang, X. Xu, Q. Yao, Experimental investigation of the optimumreaction temperature of flue gas desulfurization reaction involving CaO particles, J. Eng. Therm. Energy Power 19 (5) (2004) 454-457 (in Chinese).

[28] Y. Wang, F. Qian, Study on stability of sulfite in dregs produced by LIFAC, J. Beijing Inst. Light Ind. 19 (2) (2001) 32-35 (in Chinese).

[29] A. Wang, H. Qi, C. You, P. Lu, X. Xu, Experimental investigation on improving the calcium conversion rate of absorbent by steam, J. Eng. Thermophys. 21 (6) (2000) 769-773 (in Chinese).

[30] T. Dogu, The importance of pore structure and diffusion in the kinetics of gas-solid non-catalytic reactions: reaction of calcined limestone with SO₂, Chem. Eng. J. 21 (3) (1981) 213-222.

[31] D. Zhang, S. Yani, Sulphur transformation during pyrolysis of an Australian lignite, Proc. Combust. Inst. 33 (2) (2011) 1747-1753.

[32] H. Shang, T. Ouyang, F. Yang, Y. Kou, A biomass-supported Na₂CO₃ sorbent for flue gas desulfurization, Environ. Sci. Technol. 37 (11) (2003) 2596-2599.

[33] C.Wang, H. Liu, X. Li, J. Shi, G. Ouyang, M. Peng, C. Jiang, H.N. Cui, A new concept of desulfurization: the electrochemically driven and green conversion of SO₂ to NaHSO4 in aqueous solution, Environ. Sci. Technol. 42 (22) (2008) 8585-8590.

Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology

Experimental study on SO₂ recovery using a sodium-zinc sorbent based flue gas desulfurization technology

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

参考文献

相关文章 15

编辑推荐

Metrics

本文评价

[1]	Eileen Katherine Coronado-Aldana, Cindy Lizeth Ferreira-Salazar, Nubia Yineth Piñeros-Castro, Rubén Vázquez-Medina, Felipe A. Perdomo. Thermodynamic analysis, synthesis, characterization, and evaluation of 1-ethyl-3-methylimidazolium chloride: Study of its effect on pretreated rice husk[J]. 中国化学工程学报, 2023, 60(8): 143-154.
[2]	Runze Chen, Yuran Chen, Xuemin Liang, Yapeng Kong, Yangyang Fan, Quan Liu, Zhenyu Yang, Feiying Tang, Johnny Muya Chabu, Maru Dessie Walle, Liqiang Wang. Oxidative exfoliation of spent cathode carbon: A two-in-one strategy for its decontamination and high-valued application[J]. 中国化学工程学报, 2023, 59(7): 262-269.
[3]	Haike Li, Xindong Li, Guozai Ouyang, Lang Li, Zhaohuang Zhong, Meng Cai, Wenhao Li, Wanfu Huang. Tannic acid/Fe³⁺ interlayer for preparation of high-permeability polyetherimide organic solvent nanofiltration membranes for organic solvent separation[J]. 中国化学工程学报, 2023, 57(5): 17-29.
[4]	Shanshan Mao, Tao Shen, Qing Zhao, Tong Han, Fan Ding, Xin Jin, Manglai Gao. Selective capture of silver ions from aqueous solution by series of azole derivatives-functionalized silica nanosheets[J]. 中国化学工程学报, 2023, 57(5): 319-328.
[5]	Zhong Ma, Guofu Liu, Hui Zhang, Yonggang Lu. Investigation of the redox performance of pyrite cinder calcined at different temperature in chemical looping combustion[J]. 中国化学工程学报, 2022, 48(8): 98-105.
[6]	Zhibin Ma, Xueli Zhang, Guangjun Lu, Yanxia Guo, Huiping Song, Fangqin Cheng. Hydrothermal synthesis of zeolitic material from circulating fluidized bed combustion fly ash for the highly efficient removal of lead from aqueous solution[J]. 中国化学工程学报, 2022, 47(7): 193-205.
[7]	Danlong Li, Yannan Liang, Hainan Wang, Ruoqian Zhou, Xiaokang Yan, Lijun Wang, Haijun Zhang. Investigation on the effects of fluid intensification based preconditioning process on the decarburization enhancement of fly ash[J]. 中国化学工程学报, 2022, 44(4): 275-283.
[8]	Heping Xie, Yunpeng Wang, Tao Liu, Yifan Wu, Wenchuan Jiang, Cheng Lan, Zhiyu Zhao, Liangyu Zhu, Dongsheng Yang. Electrochemical CO₂ mineralization for red mud treatment driven by hydrogen-cycled membrane electrolysis[J]. 中国化学工程学报, 2022, 43(3): 14-23.
[9]	Zhong Ma, Chuan Yuan, Shuai Zhang, Yonggang Lu, Junhui Xiong. Effect of supports on the redox performance of pyrite cinder in chemical looping combustion[J]. 中国化学工程学报, 2021, 37(9): 168-174.
[10]	Mohamed A. El-Nemr, Ibrahim M. A. Ismail, Nabil M. Abdelmonem, Ahmed El Nemr, Safaa Ragab. Amination of biochar surface from watermelon peel for toxic chromium removal enhancement[J]. 中国化学工程学报, 2021, 36(8): 199-222.
[11]	Dauda Mohammed, Muhammad H. Al-Malack, Basheer Chanbasha. Sulfamic acid functionalized slag for effective removal of organic dye and toxic metal from the aqueous samples[J]. 中国化学工程学报, 2021, 33(5): 306-318.
[12]	Zhiying Guo, Liping Ma, Quxiu Dai, Xinbo Yang, Ran Ao, Jie Yang, Jing Yang, Wengang Li. Modified corn-core powder for enhancing sludge dewaterability: Synthesis, characterization and sludge dewatering performance[J]. 中国化学工程学报, 2021, 32(4): 368-377.
[13]	Chunguang Song, Hongling Zhang, Yuming Dong, Lili Pei, Honghui Liu, Junsheng Jiang, Hongbin Xu. Investigation on the fabrication of lightweight aggregate with acid-leaching tailings of vanadium-bearing stone coal minerals and red mud[J]. 中国化学工程学报, 2021, 32(4): 353-359.
[14]	Hamed Rezaie Azizabadi, Masoud Ziabasharhagh, Mostafa Mafi. Introducing a proper hydrogen liquefaction concept for using wasted heat of thermal power plants-case study: Parand gas power plant[J]. 中国化学工程学报, 2021, 40(12): 187-196.
[15]	Yubo Liu, Jialiang Zhang, Xu Yang, Wenguang Yang, Yongqiang Chen, Chengyan Wang. Efficient recovery of valuable metals from waste printed circuit boards by microwave pyrolysis[J]. 中国化学工程学报, 2021, 40(12): 262-268.