膜吸收法脱除含硫化氢气体的实验研究
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摘要
以聚丙烯中空纤维膜为反应器,采用N-甲基二乙醇胺(MDEA)为吸收剂,进行膜吸收脱除污泥消化过程产生的低浓度H_2S废气的研究。结果表明,随着MDEA浓度、液体流量及液气比的增大,H_2S脱除率和总传质系数均增大;但随着气体流量的增加,H_2S脱除率下降,而总传质系数增加;随着吸收剂循环次数的增加,H_2S脱除率逐渐减小,但循环13次后H_2S浓度仍低于20 mg/m~3;膜接触器在较优操作参数下连续运行20 h后,H_2S脱除率仍保持在99.6%以上,表现出较好的稳定性。经低浓度MDEA溶液浸泡30 d的膜丝接触角从初始的110°下降至100°左右,仍表现出较好的疏水性,但部分膜孔有形状变形及孔径变大现象,膜表面出现MDEA分子,这可能是连续实验后期H_2S脱除率略有下降的主要原因。
The removal of H_2S in low concentration from sludge digestion by membrane absorption was studied.MDEA was selected as the absorbent and polypropylene hollow fiber membrane was chosen as the reactor.The results showed that the H_2S removal efficiency and overall mass transfer coefficient increased with the increase of MDEA concentration,liquid velocity and liquid-gas ratio.While the H_2S removal efficiency decreased and the overall mass transfer coefficient increased with the increase of gas velocity.With the increase of absorbent cycle times,the H_2S removal efficiency decreased gradually,but the concentration of H_2S still below 20 mg/m~3 after 13 cycles.Under favorable operating parameters,the H_2S removal efficiency remained above 99.6% after 20 h continuous operation and indicates good stability of membrane contactor.After 30 d decreased from 110° to 100° and still showed good hydrophobicity.Meanwhile,the deformation of some membrane holes,the increase of pore size and MDEA molecules appear on the membrane surface should be the main reasons for the little decrease of H_2S removal efficiency in the late stage of continuous experiment.
The removal of H_2S in low concentration from sludge digestion by membrane absorption was studied.MDEA was selected as the absorbent and polypropylene hollow fiber membrane was chosen as the reactor.The results showed that the H_2S removal efficiency and overall mass transfer coefficient increased with the increase of MDEA concentration,liquid velocity and liquid-gas ratio.While the H_2S removal efficiency decreased and the overall mass transfer coefficient increased with the increase of gas velocity.With the increase of absorbent cycle times,the H_2S removal efficiency decreased gradually,but the concentration of H_2S still below 20 mg/m~3 after 13 cycles.Under favorable operating parameters,the H_2S removal efficiency remained above 99.6% after 20 h continuous operation and indicates good stability of membrane contactor.After 30 d decreased from 110° to 100° and still showed good hydrophobicity.Meanwhile,the deformation of some membrane holes,the increase of pore size and MDEA molecules appear on the membrane surface should be the main reasons for the little decrease of H_2S removal efficiency in the late stage of continuous experiment.
引文
[1] 邱天然,王曼娜,王学军,等.膜技术在沼气纯化中的应用:现状与未来[J].膜科学与技术,2015,35(6):113-120.
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[6] 安家荣,马鹏飞,唐建峰,等.MDEA复配胺液脱除天然气中H2S性能[J].化工进展,2016,35(12):3866-3871.
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[8] 孙亚伟,谢美连,刘庆岭,等.膜法分离燃煤电厂烟气中CO2的研究现状及进展[J].化工进展,2017,36(5):1880-1889.
[9] Kumar P S,Hagendoorn J A,Feron P H M,et al.New absorption liquids for the removal of CO2 from dilute gas streams using membrane contactors[J].Chemical Engineering Science,2002,57(9):1639-1651.
[10] Herzog H.What future for carbon capture and sequestration[J].Environmental Science & Technology,2001,35(7):148A-153A.
[11] 岳琳,曹利,黄学敏.膜吸收法分离燃煤烟气中CO2的实验研究[J].环境污染与防治,2017,39(8):905-910.
[12] Ashrafizadeh S N,Khorasani Z. Ammonia removal from aqueous solutions using hollow-fiber membrane contactors[J].Chemical Engineering Journal,2010,162(1):242-249.
[13] Zhao J F,Sun G P,Zhang G Q,et al.Optimization of the flash gas treatment process for a high-H2S natural gas purification plant[J].Natural Gas Industry,2013,33(7):108-112.
[14] Rami F,M Al-Marzouqi.Insights on natural gas purification:Simultaneous absorption of CO2 and H2S using membrane contactors[J].Separation and Purification Technology,2011,76(3):351-361.
[15] 张娇静,宋华,白冰,等.有机醇胺溶液中H2S气体溶解性能评价[J].化工进展,2012,31(7):1432-1436.
[16] Saeid R,Shinya Y,Masaaki,et al.CO2 absorption by using PVDF hollow fiber membrane contactors with various membrane structures[J].Separation and Purification Technology,2008,69(2):210-220.
[17] Wang D L,Teo W K,Li K.Selective removal of trace H2S from gas streams containing CO2 using hollow fiber membrane modules/contractors[J].Separation and Purification Technology,2004,35(2):125-131.
[18] Song H,Xu F,Li F,et al.Exploration and research prospect of natural gas desulfuzation mechanism of MDEA method[J].Contemporary Chemical Industry,2014,43(5):750-751.
[19] 张卫风,马伟春,邱雪菲,等.醇胺吸收液的浸润性对膜吸收法脱除CO2性能的影响[J].化工进展,2017,36(12):4686-4691.
[20] Lü Y X,Yu X H,Tu S T,et al.Wetting of polypropylene hollow fiber membrane contactors[J].Journal of Membrane Science,2010,362(1/2):444-452.
[2] Li H,Li C C,Liu W J,et al.Optimized alkaline pretreatment of suldge before anaerobic digestion[J].Bioresource Technology,2012,123:189-194.
[3] 邹雪娜,褚立强,徐徜徉.CO2/CH4分离膜技术在沼气提纯中的应用研究进展[J].膜科学与技术,2014,34(5):125-132.
[4] 晏水平,陈竞,艾平,等.利用膜吸收技术分离沼气中CO2[J].农业工程学报,2012,28(11):196-204.
[5] 杜耀,方圆,沈东升,等.填埋场中硫化氢恶臭污染防治技术研究进展[J].农业工程学报,2015,31(S1):269-275.
[6] 安家荣,马鹏飞,唐建峰,等.MDEA复配胺液脱除天然气中H2S性能[J].化工进展,2016,35(12):3866-3871.
[7] 关毅鹏,陈颖,张召才,等.膜吸收法烟气同时脱硫脱硝试验研究[J].膜科学与技术,2014,34(1):111-115.
[8] 孙亚伟,谢美连,刘庆岭,等.膜法分离燃煤电厂烟气中CO2的研究现状及进展[J].化工进展,2017,36(5):1880-1889.
[9] Kumar P S,Hagendoorn J A,Feron P H M,et al.New absorption liquids for the removal of CO2 from dilute gas streams using membrane contactors[J].Chemical Engineering Science,2002,57(9):1639-1651.
[10] Herzog H.What future for carbon capture and sequestration[J].Environmental Science & Technology,2001,35(7):148A-153A.
[11] 岳琳,曹利,黄学敏.膜吸收法分离燃煤烟气中CO2的实验研究[J].环境污染与防治,2017,39(8):905-910.
[12] Ashrafizadeh S N,Khorasani Z. Ammonia removal from aqueous solutions using hollow-fiber membrane contactors[J].Chemical Engineering Journal,2010,162(1):242-249.
[13] Zhao J F,Sun G P,Zhang G Q,et al.Optimization of the flash gas treatment process for a high-H2S natural gas purification plant[J].Natural Gas Industry,2013,33(7):108-112.
[14] Rami F,M Al-Marzouqi.Insights on natural gas purification:Simultaneous absorption of CO2 and H2S using membrane contactors[J].Separation and Purification Technology,2011,76(3):351-361.
[15] 张娇静,宋华,白冰,等.有机醇胺溶液中H2S气体溶解性能评价[J].化工进展,2012,31(7):1432-1436.
[16] Saeid R,Shinya Y,Masaaki,et al.CO2 absorption by using PVDF hollow fiber membrane contactors with various membrane structures[J].Separation and Purification Technology,2008,69(2):210-220.
[17] Wang D L,Teo W K,Li K.Selective removal of trace H2S from gas streams containing CO2 using hollow fiber membrane modules/contractors[J].Separation and Purification Technology,2004,35(2):125-131.
[18] Song H,Xu F,Li F,et al.Exploration and research prospect of natural gas desulfuzation mechanism of MDEA method[J].Contemporary Chemical Industry,2014,43(5):750-751.
[19] 张卫风,马伟春,邱雪菲,等.醇胺吸收液的浸润性对膜吸收法脱除CO2性能的影响[J].化工进展,2017,36(12):4686-4691.
[20] Lü Y X,Yu X H,Tu S T,et al.Wetting of polypropylene hollow fiber membrane contactors[J].Journal of Membrane Science,2010,362(1/2):444-452.