Comparison of absorption efficiency of three hydrogen sulfide absorbents and optimization of absorption conditions of potassium iodate system

doi:10.11949/0438-1157.20191151

Abstract

Abstract:

Hydrogen sulfide is corrosive and toxic, and the use of absorbents to absorb hydrogen sulfide gas is an important desulfurization treatment. The absorption efficiency of different absorbent is different. The absorption efficiency of three different hydrogen sulfide absorbent, namely ferric chloride system, potassium iodate system and alkaline potassium ferricyanide system, was firstly compared. Based on this, the absorption parameters of potassium iodate system were optimized, and the effects of concentration, temperature, pH, gas flow rate and time on the hydrogen sulfide gas absorption efficiency were discussed. The optimum absorption conditions were obtained by orthogonal test: temperature 55℃, pH 6.01, H₂S flow rate 0.3 L·min^-1, absorption time 1 min, the third-order absorption efficiency of 8%(mass) potassium iodate is 51.56%. The results of this study provide a theoretical reference for the absorption of hydrogen sulfide and support for the study of indirect electrolysis process.

Key words: gas, absorption, optimization, hydrogen sulfide, absorption efficiency, potassium iodate

摘要：

硫化氢具有腐蚀性与毒性，采用吸收剂吸收硫化氢气体是重要的脱硫处理方式。不同的吸收剂在吸收效率上存在较大差别。首先对比了三氯化铁体系、碘酸钾体系和碱性铁氰化钾体系三种不同硫化氢吸收剂的吸收效率。在此基础上重点优化了碘酸钾体系吸收条件参数，讨论了包含浓度、温度、pH、气体流量及时间等因素对硫化氢吸收效率的影响。并建立了四因素三水平正交试验研究较优吸收条件，得到正交试验优化吸收条件为：温度55℃，pH 6.01，硫化氢流量0.3 L·min^-1，吸收时间1 min，该条件下8%（质量）碘酸钾体系的三级吸收效率为51.56%。研究结果对硫化氢吸收处理提供了理论参考，也为间接电解法循环处理研究提供了支持。

关键词: 气体, 吸收, 优化, 硫化氢, 吸收效率, 碘酸钾

CLC Number:

TQ 125.1

Xue LYU, Yue MOU, Yiwen MIU, Hanlu LIAO, Jiansu RAN, Jie ZHENG. Comparison of absorption efficiency of three hydrogen sulfide absorbents and optimization of absorption conditions of potassium iodate system[J]. CIESC Journal, 2020, 71(10): 4696-4703.

吕雪, 牟玥, 缪逸文, 廖寒露, 冉建速, 郑杰. 三种硫化氢吸收剂吸收效率对比及碘酸钾体系吸收条件优化研究[J]. 化工学报, 2020, 71(10): 4696-4703.

Figures/Tables 10

References 34

1	唐慧, 王泰人. 油田气净化脱酸技术探讨[J]. 现代化工, 2019, 39(S1): 85-88.
	Tang H, Wang T R. Discussion on oilfield gas purification and deacidification technology[J]. Modern Chemical Industry, 2019, 39(S1): 85-88.
2	Claudia N O, Jason J L, Anton D V, et al. Selective removal of hydrogen sulfide from simulated biogas streams using sterically hindered amine adsorbents[J]. Chemical Engineering Journal, 2020, 379: 122349.
3	申梦瑶. 利用离子液体类吸收剂脱除焦炉煤气中硫化氢的研究[D]. 北京: 北京化工大学, 2018.
	Shen M Y. Study on the removal of hydrogen sulfide in coke oven gas by ionic liquid based absorbents[D]. Beijing: Beijing University of Chemical Technology, 2018.
4	Asbel D H, Noora K, Pekka S, et al. Effect of H₂S and thiophene on the steam reforming activity of nickel and rhodium catalysts in a simulated coke oven gas stream[J]. Applied Catalysis B: Environmental, 2019, 258: 117977.
5	张评, 冯权莉. 电解铝废气处理的研究进展[J]. 化工科技, 2018, 26(5): 63-67.
	Zhang P, Feng Q L. Research progress on treatment of waste gas in electrolytic aluminum industry[J]. Science & Technology in Chemical Industry, 2018, 26(5): 63-67.
6	Liu X P, Wang B H, Wang D D, et al. Study on the desulfurization performance of metal-based low transition temperature mixtures: Removal of hydrogen sulfide and sulfur recovery[J]. Fuel Processing Technology, 2019, 193: 372-377.
7	Maryam D, Raheleh S, Alimorad R. Adsorption of hydrogen sulfide over a novel metal organic framework-metal oxide nanocomposite: TOUO-x (TiO₂ /UiO-66)[J]. Journal of Solid State Chemistry, 2019, 278: 120866.
8	Liu X P, Li J P, Wang R. Study on the desulfurization performance of hydramine/ionic liquid solutions at room temperature and atmospheric pressure[J]. Fuel Processing Technology, 2017, 167: 382-387.
9	沈鑫甫. 中学教师实用化学辞典[M]. 北京: 北京科学技术出版社, 2002: 190-191.
	Shen X F. Dictionary of Practical Chemistry for Middle School Teachers[M]. Beijing: Beijing Science and Technology Press, 2002: 190-191.
10	Mizuta S, Kondo W, Fujii K, et al. Hydrogen production from hydrogen sulfide by the iron-chlorine hybrid process[J]. Industrial & Engineering Chemistry Research, 1991, 30(7): 1601-1608.
11	俞英, 王崇智, 赵永丰, 等. 氧化-电解法从硫化氢获取廉价氢气方法的研究[J]. 太阳能学报, 1997, (4): 53-61.
	Yu Y, Wang C Z, Zhao Y F, et al. Study on cheap hydrogen from hydrogen sulfide by oxidization-electrolysis method[J]. Acta Energiae Solaris Sinica, 1997, (4): 53-61.
12	鄂利海, 雒怀庆, 栾耕时. Fe(III)盐溶液吸收法处理H₂S气体的研究[J]. 抚顺石油学院学报, 2001, (1): 12-16.
	E L H, Luo H Q, Luan G S. Process of H₂S treatment using aqueous ferric salt solution absorption[J]. Journal of Liaoning Shihua University, 2001, (1): 12-16.
13	李海燕, 宋增红, 刘爱华, 等. 电解硫化氢制氢气和硫磺的影响因素研究[J]. 硫酸工业, 2018, (4): 40-43.
	Li H Y, Song Z H, Liu A H, et al. Study on influence factors of hydrogen and sulphur by electrolysis of hydrogen sulfide[J]. Sulphuric Acid Industry, 2018, (4): 40-43.
14	Huang H Y, Shang J, Yu Y, et al. Chung. Recovery of hydrogen from hydrogen sulfide by indirect electrolysis process[J]. International Journal of Hydrogen Energy, 2019, 44: 5108-5113.
15	周秀华, 王其峰. 加碘盐中碘酸钾含量的简易化验[J]. 海湖盐与化工, 1994, (6): 42-45+47.
	Zhou X H, Wang Q F. Simple assay of potassium iodate in iodized salt[J]. Journal of Salt Science and Chemical Industry, 1994, (6): 42-45+47.
16	Kalina D, Mass Jr E T. Indirect hydrogen sulfide conversion(Ⅰ): An acidic electrochemical process[J]. International Journal of Hydrogen Energy, 1985, 10(3): 157-162.
17	Kalina D, Mass Jr E T. Indirect hydrogen sulfide conversion(Ⅱ): A basic electrochemical process[J]. International Journal of Hydrogen Energy, 1985, 10(3): 163-167.
18	李秀玲, 赵朝成. 核桃壳质活性炭的制备及吸附恶臭气体的研究[J]. 环境科技, 2009, 22(6): 32-34.
	Li X L, Zhao C C. Study on preparation of activated carbons from walnut shells and odor gas adsorption[J]. Environmental Science and Technology, 2009, 22(6): 32-34.
19	李秀玲, 辛磊, 赵朝成. KIO₃改性炭基催化剂的制备及其吸附性能评价[J]. 炭素技术, 2019, 38(2): 52-57.
	Li X L, Xin L, Zhao C C. Preparation and adsorption performance evaluation of carbon-based catalysts modified by KIO₃[J]. Carbon Techniques, 2019, 38(2): 52-57.
20	马世昌. 化学物质辞典[M]. 西安: 陕西科学技术出版社, 1999: 591.
	Ma S C. Dictionary of Chemical Substances[M]. Xi 'an: Shaanxi Science and Technology Press, 1999: 591.
21	Otto H L, Winand M. The preparation of Curie quantities of S35-labelled element sulphur[J]. The International Journal of Applied Radiation and Isotopes, 1961, 10: 130.
22	余丽. 基于丝网印刷电极硫化氢、重金属离子的快速检测[D]. 合肥: 合肥工业大学, 2013.
	Yu L. Rapid detection of hydrogen sulfide and heavy metal ions based on screen-printed electrode[D]. Hefei: Hefei University of Technology, 2013.
23	徐后传. 碳材料修饰电极快速检测硫化氢和亚硝酸盐及其在食品检测中的应用研究[D]. 合肥: 合肥工业大学, 2015.
	Xu H Z. Rapid electrochemical sensing of hydrogen sulfide and nitrite in food based on carbon material modified electrodes[D]. Hefei: Hefei University of Technology, 2015.
24	韩磊. 新型间接电解硫化氢铁系吸收液及电解池设计研究[D]. 北京: 中国石油大学(北京), 2016.
	Han L. Design of a new type of indirect electrolytic hydrogen sulfide absorption liquid and electrolytic cell[D]. Beijing: China University of Petroleum (Beijing), 2016.
25	赵艳青, 张永春, 陈绍云, 等. 液态氧化法选择性脱除烟道气中硫化氢的研究[J]. 低温与特气, 2011, 29(3): 8-12.
	Zhao Y Q, Zhang Y C, Chen S Y, et al. The study of selective removal H₂S from flue-gas by wet air oxidation[J]. Low Temperature and Specialty Gases, 2011, 29(3): 8-12.
26	王凯, 王磊, 魏莉, 等. 新型硫化氢吸收剂试验研究[J]. 山东化工, 2017, 46(17): 27-28+31.
	Wang K, Wang L, Wei L, et al. Experimental study on the new type of H₂S absorption[J]. Shandong Chemical Industry, 2017, 46(17): 27-28+31.
27	张存胜, 王文娟, 苏海佳, 等. 改性活性炭脱除沼气中硫化氢的性能及其再生研究[J]. 现代化工, 2016, 36(12): 59-62.
	Zhang C S, Wang W J, Su H J, et al. Desulfurization of biogas by modified activated carbon and its regeneration[J]. Modern Chemical Industry, 2016, 36(12): 59-62.
28	沈力. 聚合硫酸铁-硫酸铜溶液吸收硫化氢的研究[D]. 吉林: 吉林大学, 2014.
	Shen L. The study on the absorption of hydrogen sulfide by polyferric sulphate-copper sulfate[D]. Jilin: Jilin University, 2014.
29	李发永, 曹作刚, 张海鹏, 等. 由硫化氢制取硫磺及氢气扩大实验研究[J]. 化工进展, 2001, (7): 38-41.
	Li F Y, Cao Z G, Zhang H P, et al. Experimental study on transforming refinery acid tail gas into sulphur and hydrogen[J]. Chemical Industry and Engineering Progress, 2001, (7): 38-41.
30	陈凯, 史有刚, 高圣新, 等. 油水井酸化用硫化氢吸收剂的研制及性能[J]. 石油与天然气化工, 2010, 39(3): 226-229+179-180.
	Chen K, Shi Y G, Gao S X, et al. Synthesis and evaluation of hydrogen sulfide scavenger for well acidizing[J]. Chemical Engineering of Oil & Gas, 2010, 39(3): 226-229+179-180.
31	董如何, 肖必华, 方永水. 正交试验设计的理论分析方法及应用[J]. 安徽建筑工业学院学报(自然科学版), 2004, (6): 103-106.
	Dong R H, Xiao B H, Fang Y S. Theoretical analysis method and application of orthogonal experimental design[J]. Journal of Anhui Jianzhu University, 2004, (6): 103-106.
32	王艳, 张爱珍, 任春生. 正交试验设计与优化的理论基础与应用进展[J]. 分析试验室, 2008, 27(S2): 333-334.
	Wang Y, Zhang A Z, Ren C S. The theoretical basis and application progress of orthogonal experimental design and optimization[J]. Chinese Journal of Analysis Laboratory, 2008, 27(S2): 333-334.
33	邓利民, 李世伟, 侯映天, 等. 两种Betti碱对硫化氢吸收性能研究[J]. 化学研究与应用, 2017, 29(12): 1909-1915.
	Deng L M, Li S W, Hou Y T, et al. Preparation of two Betti alkalis and survey about absorption of hydrogen sulfide by betti alkalis[J]. Chemical Research and Application, 2017, 29(12): 1909-1915.
34	张永, 王学谦, 宁平, 等. 碳酸钠溶液吸收处理硫化氢试验研究[J]. 云南化工, 2006, (2): 32-34.
	Zhang Y, Wang X Q, Ning P, et al. Study on the absorption of hydrogen sulfide by sodium carbonate solution[J]. Yunnan Chemical Technology, 2006, (2): 32-34.

序号	碘酸钾质量浓度	三级吸收效率 η/%	反应前 pH	反应后pH
序号	碘酸钾质量浓度	三级吸收效率 η/%	反应前 pH	1^#吸收管	2^#吸收管	3^#吸收管
1	0.01	5.79	4.42	1.71	1.64	1.60
2	0.03	12.53	5.25	1.38	1.25	1.22
3	0.05	18.33	5.48	1.35	1.18	1.18
4	0.06	21.39	5.83	1.19	1.14	1.13
5	0.08	26.35	6.27	1.13	1.00	0.94

序号	碘酸钾质量浓度	三级吸收效率 η/%	反应前 pH	反应后pH
序号	碘酸钾质量浓度	三级吸收效率 η/%	反应前 pH	1^#吸收管	2^#吸收管	3^#吸收管
1	0.01	5.79	4.42	1.71	1.64	1.60
2	0.03	12.53	5.25	1.38	1.25	1.22
3	0.05	18.33	5.48	1.35	1.18	1.18
4	0.06	21.39	5.83	1.19	1.14	1.13
5	0.08	26.35	6.27	1.13	1.00	0.94

实验号	因素水平				三级吸收效率/%
实验号	A	B	C	D	三级吸收效率/%
1	1(0.3)	1（1)	1(26.5)	1(1.93)	51.26
2	1	2(2)	2(40)	2(6.01)	52.27
3	1	3(3)	3(55)	3(10.11）	50.12
4	2(0.67）	1	2	3	32.87
5	2	2	3	1	38.96
6	2	3	1	2	30.34
7	3（1）	1	3	2	45.36
8	3	2	1	3	30.10
9	3	3	2	1	22.83
k₁	51.21	43.16	37.23	37.68
k₂	34.06	40.44	35.99	42.65
k₃	32.76	34.43	44.81	37.70
极差R	18.45	8.73	8.83	4.97
优化水平	A1	B1	C3	D2
因素影响顺序	A>C>B>D

实验号	因素水平				三级吸收效率/%
实验号	A	B	C	D	三级吸收效率/%
1	1(0.3)	1（1)	1(26.5)	1(1.93)	51.26
2	1	2(2)	2(40)	2(6.01)	52.27
3	1	3(3)	3(55)	3(10.11）	50.12
4	2(0.67）	1	2	3	32.87
5	2	2	3	1	38.96
6	2	3	1	2	30.34
7	3（1）	1	3	2	45.36
8	3	2	1	3	30.10
9	3	3	2	1	22.83
k₁	51.21	43.16	37.23	37.68
k₂	34.06	40.44	35.99	42.65
k₃	32.76	34.43	44.81	37.70
极差R	18.45	8.73	8.83	4.97
优化水平	A1	B1	C3	D2
因素影响顺序	A>C>B>D

[1]	Xin YANG, Wen WANG, Kai XU, Fanhua MA. Simulation analysis of temperature characteristics of the high-pressure hydrogen refueling process [J]. CIESC Journal, 2023, 74(S1): 280-286.
[2]	Weiqi JIN, Yuerong WU, Xia WANG, Li LI, Su QIU, Pan YUAN, Minghe WANG. Progress in infrared imaging detection technology and domestic equipment for industrial gas leakage in chemical industry parks [J]. CIESC Journal, 2023, 74(S1): 32-44.
[3]	Congqi HUANG, Yimei WU, Jianye CHEN, Shuangquan SHAO. Simulation study of thermal management system of alkaline water electrolysis device for hydrogen production [J]. CIESC Journal, 2023, 74(S1): 320-328.
[4]	Zhenghao JIN, Lijie FENG, Shuhong LI. Energy and exergy analysis of a solution cross-type absorption-resorption heat pump using NH₃/H₂O as working fluid [J]. CIESC Journal, 2023, 74(S1): 53-63.
[5]	He JIANG, Junfei YUAN, Lin WANG, Guyu XING. Experimental study on the effect of flow sharing cavity structure on phase change flow characteristics in microchannels [J]. CIESC Journal, 2023, 74(S1): 235-244.
[6]	Zehao MI, Er HUA. DFT and COSMO-RS theoretical analysis of SO₂ absorption by polyamines type ionic liquids [J]. CIESC Journal, 2023, 74(9): 3681-3696.
[7]	Song HE, Qiaomai LIU, Guangshuo XIE, Simin WANG, Juan XIAO. Two-phase flow simulation and surrogate-assisted optimization of gas film drag reduction in high-concentration coal-water slurry pipeline [J]. CIESC Journal, 2023, 74(9): 3766-3774.
[8]	Meisi CHEN, Weida CHEN, Xinyao LI, Shangyu LI, Youting WU, Feng ZHANG, Zhibing ZHANG. Advances in silicon-based ionic liquid microparticle enhanced gas capture and conversion [J]. CIESC Journal, 2023, 74(9): 3628-3639.
[9]	Zhewen CHEN, Junjie WEI, Yuming ZHANG. System integration and energy conversion mechanism of the power technology with integrated supercritical water gasification of coal and SOFC [J]. CIESC Journal, 2023, 74(9): 3888-3902.
[10]	Jiaqi YUAN, Zheng LIU, Rui HUANG, Lefu ZHANG, Denghui HE. Investigation on energy conversion characteristics of vortex pump under bubble inflow [J]. CIESC Journal, 2023, 74(9): 3807-3820.
[11]	Chen HAN, Youmin SITU, Bin ZHU, Jianliang XU, Xiaolei GUO, Haifeng LIU. Study of reaction and flow characteristics in multi-nozzle pulverized coal gasifier with co-processing of wastewater [J]. CIESC Journal, 2023, 74(8): 3266-3278.
[12]	Guoze CHEN, Dong WEI, Qian GUO, Zhiping XIANG. Optimal power point optimization method for aluminum-air batteries under load tracking condition [J]. CIESC Journal, 2023, 74(8): 3533-3542.
[13]	Wenzhu LIU, Heming YUN, Baoxue WANG, Mingzhe HU, Chonglong ZHONG. Research on topology optimization of microchannel based on field synergy and entransy dissipation [J]. CIESC Journal, 2023, 74(8): 3329-3341.
[14]	Ruihang ZHANG, Pan CAO, Feng YANG, Kun LI, Peng XIAO, Chun DENG, Bei LIU, Changyu SUN, Guangjin CHEN. Analysis of key parameters affecting product purity of natural gas ethane recovery process via ZIF-8 nanofluid [J]. CIESC Journal, 2023, 74(8): 3386-3393.
[15]	Xingzhi HU, Haoyan ZHANG, Jingkun ZHUANG, Yuqing FAN, Kaiyin ZHANG, Jun XIANG. Preparation and microwave absorption properties of carbon nanofibers embedded with ultra-small CeO₂ nanoparticles [J]. CIESC Journal, 2023, 74(8): 3584-3596.