Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor

doi:10.1016/j.cjche.2016.08.032

›› 2017, Vol. 25 ›› Issue (2): 175-179.DOI: 10.1016/j.cjche.2016.08.032

• Selected Papers from the International Chemical Separation Technology Conference (ICSTC) • 上一篇下一篇

Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor

Liangliang Zhang¹, Shuying Wu¹, Zuozhong Liang¹, Hong Zhao^1,2, Haikui Zou¹, Guangwen Chu¹

1 Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, China;
2 Suzhou Research Institute of Beijing University of Chemical Technology, Suzhou 215100, China

收稿日期:2016-06-15 修回日期:2016-08-31 出版日期:2017-02-28 发布日期:2017-03-14
通讯作者: Liangliang Zhang
基金资助:
Supported by the National Natural Science Foundation of China (21406008).

Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor

Liangliang Zhang¹, Shuying Wu¹, Zuozhong Liang¹, Hong Zhao^1,2, Haikui Zou¹, Guangwen Chu¹

1 Research Center of the Ministry of Education for High Gravity Engineering and Technology, Beijing University of Chemical Technology, Beijing 100029, China;
2 Suzhou Research Institute of Beijing University of Chemical Technology, Suzhou 215100, China

Received:2016-06-15 Revised:2016-08-31 Online:2017-02-28 Published:2017-03-14
Supported by:
Supported by the National Natural Science Foundation of China (21406008).

摘要/Abstract

摘要： Using catalytic oxidative absorption for H₂S removal is of great interest due to its distinct advantages. However, traditional scrubbing process faces a great limitation in the confined space. Therefore, there is an urgent demand to develop high-efficiency process intensification technology for such a system. In this article, H₂S absorption experimental research was conducted in a rotating packed bed (RPB) reactor with ferric chelate absorbent and a mixture of N₂ and H₂S, which was used to simulate natural gas. The effects of absorbent pH value, gas-liquid ratio, gravity level of RPB, absorption temperature and character of the packing on the desulfurization efficiency were investigated. The results showed that H₂S removal efficiency could reach above 99.6% under the most of the experimental condition and above 99.9% under the optimal condition. A long-time continuous experiment was conducted to investigate the stability of the whole process combining absorption and regeneration. The result showed that the process could well realize simultaneous desulfurization and absorbent regeneration, and the H₂S removal efficiency kept relatively stable in thewhole duration of 72 h. It can be clearly seen that high gravity technology desulfurization process,which is simple, high-efficiency, and space intensive, has a good prospect for industrial application of H₂S removal in confined space.

关键词: Confined space, RPB, Desulfurization, Catalytic oxidative, Absorption

Abstract: Using catalytic oxidative absorption for H₂S removal is of great interest due to its distinct advantages. However, traditional scrubbing process faces a great limitation in the confined space. Therefore, there is an urgent demand to develop high-efficiency process intensification technology for such a system. In this article, H₂S absorption experimental research was conducted in a rotating packed bed (RPB) reactor with ferric chelate absorbent and a mixture of N₂ and H₂S, which was used to simulate natural gas. The effects of absorbent pH value, gas-liquid ratio, gravity level of RPB, absorption temperature and character of the packing on the desulfurization efficiency were investigated. The results showed that H₂S removal efficiency could reach above 99.6% under the most of the experimental condition and above 99.9% under the optimal condition. A long-time continuous experiment was conducted to investigate the stability of the whole process combining absorption and regeneration. The result showed that the process could well realize simultaneous desulfurization and absorbent regeneration, and the H₂S removal efficiency kept relatively stable in thewhole duration of 72 h. It can be clearly seen that high gravity technology desulfurization process,which is simple, high-efficiency, and space intensive, has a good prospect for industrial application of H₂S removal in confined space.

Key words: Confined space, RPB, Desulfurization, Catalytic oxidative, Absorption

Liangliang Zhang, Shuying Wu, Zuozhong Liang, Hong Zhao, Haikui Zou, Guangwen Chu. Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor[J]. , 2017, 25(2): 175-179.

参考文献

[1] H. Huo, Q. Zhang, F. Liu, K. He, Climate and environmental effects of electric vehicles versus compressed natural gas vehicles in China:A life-cycle analysis at provincial level, Environ. Sci. Technol. 47(3) (2013) 1711-1718.
[2] Y.W. Ma, Z.Z. Chen, H.J. Gong, Study on selective hydrogen sulfide removal over carbon dioxide by catalytic oxidative absorption method with chelated iron as the catalyst, Renew. Energy 1(2016) 1-8.
[3] A. Pieplu, O. Saur, J.C. Lavalley, Claus catalysis and H₂S selective oxidation, Catal. Rev. Sci. Eng. 40(4) (1998) 409-450.
[4] J. Lu, Y. Zheng, D. He, Selective absorption of H₂S fromgas mixtures into aqueous solutions of blended amines of methyldiethanolamine and 2-tertiarybutylamino-2-ethoxyethanol in a packed column, Sep. Purif. Technol. 52(2006) 209-217.
[5] B.N. Markus, F. Anton, K. Ulrich, T. Thomas, Modelling selective H₂S absorption and desorption in an aqueous MDEA-solution using a rate-based non-equilibrium approach, Chem. Eng. Process. 43(6) (2004) 701-715.
[6] D.W. Neumann, S. Lynn, Oxidative absorption of H₂S and O₂ by iron chelate solution, AIChE J. 30(1984) 62-69.
[7] G. Edith, T. Turek, Removal of hydrogen sulfide by permanganate based sorbents:Experimental investigation and reactormodeling, Chem. Eng. Sci. 151(2016) 51-63.
[8] C.A.P. Zevenhoven, K.P. Yrjas, M.M. Hupa, Hydrogen sulfide capture by limestone and dolomite at elevated pressure. 2. Sorbent particle conversion modeling, Ind. Eng. Chem. Res. 35(3) (1996) 943-949.
[9] A.M. Montebello, T. Bezerra, R. Rovira, L. Rago, J. Lafuente, X. Gamisans, Operational aspects, pH transition and microbial shifts of a H₂S desulfurizing biotrickling filter with random packing material, Chemosphere 93(2013) 2675-2682.
[10] I. Diaz, S.I. Perez, E.M. Ferrero, M. Fdz-Polanco, Effect of oxygen dosing point and mixing on the microaerobic removal of hydrogen sulphide in sludge digesters, Bioresour. Technol. 102(2011) 3768-3775.
[11] A.M. Montebello, M. Fernandez, F. Almenglo, M. Ramirez, D. Cantero, M. Baeza, Simultaneous methylmercaptan and hydrogen sulfide removal in the desulfurization of biogas in aerobic and anoxic biotrickling filters, Chem. Eng. J. 200(2012) 237-246.
[12] W.B. Richard, L. Kaaeid, Natural gas processing with membranes:An overview, Ind. Eng. Chem. Res. 44(2005) 3348-3354.
[13] D. McManus, A.E. Martell, The evolution, chemistry and applications of chelated iron hydrogen sulfide removal and oxidation processes, J. Mol. Catal. A:Chem. 117(1997) 289-297.
[14] A.S.Michael, I.D.Norman, D.C. Peter, CatalyticH₂S conversion and SO₂ production over iron oxide and iron oxide/γ-Al₂O₃ in liquid sulfur, Ind. Eng. Chem. Res. 46(2007) 7721-7728.
[15] M. Miltner, A. Makaruk, J. Krischan, M. Harasek, Chemical-oxidative scrubbing for the removal of hydrogen sulphide from raw biogas:Potentials and economics, Water Sci. Technol. 66(2012) 1354-1360.
[16] D.Chen, A.E.Martell, D.Mcmanus, Studiesonthemechanismof chelatedegradationinironbased, liquid redox H₂S removal process, Can. J. Chem. Eng. 73(1995) 264-274.
[17] H.J. Wubs, A. Beenackers, Kinetics of H₂S absorption into aqueous ferric solution of EDTA and HEDTA, AIChE J. 40(1994) 433-444.
[18] S.Munjal,M.P. Dudukovic, P. Ramachandran, Mass transfer in rotating packed beds:I. Development of gas-liquid and liquid-solid mass-transfer coefficients, Chem. Eng. Sci. 44(1989) 2245-2256.
[19] F. Guo, C. Zheng, K. Guo, Y.D. Feng, N.C. Gardner, Hydrodynamics and mass transfer in cross-flow rotating packed bed, Chem. Eng. Sci. 52(1997) 3853-3859.
[20] J.R. Burns, C. Ramshaw, Process intensification:Visual study of liquid maldistribution in rotating packed beds, Chem. Eng. Sci. 51(1996) 1347-1352.
[21] H.J. Yang, G.W. Chu, Y. Xiang, J.F. Chen, Characterization ofmicromixing efficiency in rotating packed beds by chemical methods, Chem. Eng. J. 121(2006) 147-152.
[22] F.Yi, H.K. Zou, G.W. Chu, L. Shao, J.F.Chen,Modelingandexperimental studies onabsorption of CO₂ by Benfield solution in rotating packed bed, Chem. Eng. J. 145(2009) 377-384.
[23] H. Zhao, L. Shao, J.F. Chen, High-gravity process intensification technology and application, Chem. Eng. J. 156(2010) 588-593.
[24] J.F. Chen, C. Zheng, G.T. Chen, Interaction of macro- and micromixing on particlesize distribution in reactive precipitation, Chem. Eng. Sci. 51(1996) 1957-1966.
[25] C.C. Lin, Y.R. Su, Performance of rotating packed beds in removing ozone from gaseous streams, Sep. Purif. Technol. 61(2008) 311-316.
[26] J.F. Chen, L. Shao, Mass production of nanoparticles by high gravity reactive precipitation technology with low cost, China Particuol. 1(2003) 64-69.
[27] Y. Luo, G.W. Chu, L. Sang, H.K. Zou, Y. Xiang, J.F. Chen, A two-stage blade-packing rotating packed bed for intensification of continuous distillation, Chin. J. Chem. Eng. 24(1) (2016) 109-115.
[28] Y.P. Feng, Requirements and analysis methods of sulfides content in ammonia synthesis feed gas, J. Chem. Ind. Eng. (China) 24(1) (2003) 26-30.

Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor

Hydrogen sulfide removal by catalytic oxidative absorption method using rotating packed bed reactor

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]	Lijuan Zhao, Zhe Tan, Xiaoguang Zhang, Qijun Zhang, Wei Wang, Qiang Deng, Jie Ma, De'an Pan. Research on process modeling and simulation of spent lead paste desulfurization enhanced reactor[J]. 中国化学工程学报, 2023, 60(8): 293-303.
[2]	Bing Liu, Yingjiao Li, Moses Arowo, Guangwen Chu, Yong Luo, Liangliang Zhang, Haikui Zou, Baochang Sun. Sulfonation of 1, 4-diaminoanthraquinone leuco by chlorosulfonic acid: Kinetics and process intensification[J]. 中国化学工程学报, 2023, 58(6): 163-169.
[3]	Yutong Jiang, Yifeng Chen, Fuliu Yang, Jixue Fan, Jun Li, Zhuhong Yang, Xiaoyan Ji. Efficient SO₂ removal using aqueous ionic liquid at low partial pressure[J]. 中国化学工程学报, 2023, 58(6): 355-363.
[4]	Feng Pan, Sugang Ma, Yu Ge, Chuanlin Fan, Qingshan Zhu. Fluidization thermal decomposition of sodium fluosilicate[J]. 中国化学工程学报, 2023, 57(5): 329-337.
[5]	Wen Tian, Junyi Ji, Hongjiao Li, Changjun Liu, Lei Song, Kui Ma, Siyang Tang, Shan Zhong, Hairong Yue, Bin Liang. Measurements of the effective mass transfer areas for the gas–liquid rotating packed bed[J]. 中国化学工程学报, 2023, 55(3): 13-19.
[6]	Zida Ma, Yuxia Li, Mengmeng Jin, Xiaoqin Liu, Linbing Sun. Fabrication of adsorbents with enhanced Cu^I stability: Creating a superhydrophobic microenvironment through grafting octadecylamine[J]. 中国化学工程学报, 2023, 55(3): 41-48.
[7]	Yuandong Cui, Bin He, Yu Lei, Yu Liang, Wanting Zhao, Jian Sun, Xiaomin Liu. Lignin derived absorbent for efficient and sustainable CO₂ capture[J]. 中国化学工程学报, 2023, 54(2): 89-97.
[8]	Yilin Song, Yize Zhang, Hao Zhou. Experimental study on the desulfurization and evaporation characteristics of Ca(OH)₂ droplets[J]. 中国化学工程学报, 2023, 54(2): 127-135.
[9]	Xiaodong Yang, Na Yang, Ziqiang Gong, Feifei Peng, Bin Jiang, Yongli Sun, Luhong Zhang. The superhydrophobic sponge decorated with Ni-Co double layered oxides with thiol modification for continuous oil/water separation[J]. 中国化学工程学报, 2023, 54(2): 296-305.
[10]	Jing Gao, Zhijun Ma, Fuli Liu, Cunxin Chen. Synthesis of carbon-coated cobalt ferrite core–shell structure composite: A method for enhancing electromagnetic wave absorption properties by adjusting impedance matching[J]. 中国化学工程学报, 2022, 47(7): 206-217.
[11]	Yaran Yin, Xianming Zhang, Chunying Zhu, Taotao Fu, Youguang Ma. Formation characteristics of Taylor bubbles in a T-junction microchannel with chemical absorption[J]. 中国化学工程学报, 2022, 46(6): 214-222.
[12]	Linlan Wu, Zhengxin Jiao, Suhang Xun, Minqiang He, Lei Fan, Chao Wang, Wenshu Yang, Wenshuai Zhu, Huaming Li. Photocatalytic oxidative of Keggin-type polyoxometalate ionic liquid for enhanced extractive desulfurization in binary deep eutectic solvents[J]. 中国化学工程学报, 2022, 44(4): 205-211.
[13]	Liwang Wang, Hualin Wang, Liang Ma, Zhanghuang Yang, Erwen Chen. Gas cyclone-liquid jet absorption separator used for treatment of tail gas containing HCl in titanium dioxide industry[J]. 中国化学工程学报, 2022, 44(4): 435-446.
[14]	Xiaomeng Zhao, Xingyu Li, Changjun Liu, Shan Zhong, Houfang Lu, Hairong Yue, Kui Ma, Lei Song, Siyang Tang, Bin Liang. The quasi-activity coefficients of non-electrolytes in aqueous solution with organic ions and its application on the phase splitting behaviors prediction for CO₂ absorption[J]. 中国化学工程学报, 2022, 43(3): 316-323.
[15]	Cuiting Yang, Bowen Wu, Zewei Liu, Guang Miao, Qibin Xia, Zhong Li, Michael J. Janik, Guoqing Li, Jing Xiao. Catalytic adsorptive desulfurization of mercaptan, sulfide and disulfide using bifunctional Ti-based adsorbent for ultra-clean oil[J]. 中国化学工程学报, 2022, 42(2): 25-34.