张超越,白净,魏源霞,史海港,李攀,常春

• 1:郑州大学化工与能源学院
• 2:河南省杰出外籍科学家工作室

摘要(Abstract)：

为了快速制备甲烷水合物以利于天然气水合物法储运,在自行搭建的液相连续撞击流反应器内考察了纯水和纯水+十二烷基硫酸钠(SDS) 2种体系中撞击强度、反应器内温度、初始压力对甲烷水合物快速生成的影响。实验结果表明:2种体系内撞击强度的增加可明显加快甲烷水合物的生成,在撞击强度为0.38、反应的前30 min,水合速率达到最大,速率分别为0.48,1.3 mol·h~(-1),甲烷水合率分别为28.4%,45.8%。反应器内温度的降低、初始压力的升高均可加速甲烷水合物的生成,在温度为275.15 K、压力为6 MPa、反应的前30 min,水合速率最大为1 mol·h~(-1),甲烷水合率为49.4%。同时还考察了SDS质量浓度对甲烷水合物快速生成过程的影响,确定了最佳SDS质量浓度为600 mg·L~(-1)。

关键词(KeyWords)： 甲烷水合物;撞击流;水合速率;甲烷水合率

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金(U1404519,52006200)

作者(Author): 张超越,白净,魏源霞,史海港,李攀,常春

参考文献(References)：

• [1] LU Y, GE B, ZHONG D L. Investigation of using graphite nanofluids to promote methane hydrate formation:Application to solidified natural gas storage[J]. Energy, 2020, 199:117424.
• [2] GUDMUNDSSON J S, PARLAKTUNA M. Storing natural gas as frozen hydrate[J]. SPE Production&Facilities, 1994, 9(1):69-73.
• [3] LIU H, ZHAN S, LI R, et al. High-efficiency natural-gas storage method involving formation of gas hydrate in water/oil-cyclopentane emulsion[J]. Chemical Engineering Journal, 2020, 400:125369.
• [4] LIU X, CAO Q, XU D, et al. Carboxylate surfactants as efficient and renewable promoters for methane hydrate formation[J].Energy&Fuels, 2021, 35(6):5153-5162.
• [5] XIAO P, YANG X M, SUN C Y, et al. Enhancing methane hydrate formation in bulk water using vertical reciprocating impact[J].Chemical Engineering Journal, 2018, 336:649-658.
• [6] LINGA P, KUMAR R, LEE J D, et al. A new apparatus to enhance the rate of gas hydrate formation:Application to capture of carbon dioxide[J]. International Journal of Greenhouse Gas Control, 2010, 4(4):630-637.
• [7] ROSSI F, FILIPPONI M, CASTELLANI B. Investigation on a novel reactor for gas hydrate production[J]. Applied Energy, 2012,99(5):167-172.
• [8]张东亮.中国煤气化工艺(技术)的现状与发展[J].煤化工, 2004(2):1-5.ZHANG D L. Present status and future development of coal gasification technology in China[J]. Coal Chemical Industry, 2004(2):1-5.
• [9] BERMAN Y, TAMIR A. Kinetics of droplets’ sedimentation in a continuous gravity settler[J]. Chemical Engineering Science, 2003,58(10):2089-2102.
• [10] BERMAN Y, TAMIR A. Extraction in thin liquid films generated by impinging streams[J]. AIChE Journal, 2000, 46(4):769-778.
• [11] MURAKAMI T, KURITSUKA H, FUJII H, et al. Forming a structure-H hydrate using water and methylcyclohexane jets impinging on each other in a methane atmosphere[J]. Energy&Fuels, 2009(23):1619-1625.
• [12] BAI J, XIE G B, LI L Q, et al. Kinetics investigation of carbon dioxide hydrate formation process in a new impinging stream reactor[J]. International Journal of Chemical Reactor Engineering, 2019, 18(1):20190132.
• [13] BAI J, ZHEN X, XIE G B, et al. Kinetics investigation of hydrate-based CO2 capture from simulated flue gas by using an improved combinatorial promoter[J]. Energy&Fuels, 2018, 32(10):10822-10829.
• [14] LINGA P, DARABOINA N, RIPMEESTER J A, et al. Enhanced rate of gas hydrate formation in a fixed bed column filled with sand compared to a stirred vessel[J]. Chemical Engineering Science, 2012, 68(1):617-623.
• [15]方书起,张欣悦,李思齐,等.撞击流式反应器内水合物法分离沼气中CO2研究[J].化工学报, 2020, 71(5):2099-2108.FANG S Q, ZHANG X Y, LI S Q, et al. Separation of CO2 from biogas by hydrates in impingement flow reactor[J]. CIESC Journal,2020, 71(5):2099-2108.
• [16] BAI J, LIANG D Q, LI D L, et al. Continuous formation process of CO2 gas hydrate via a vortex and impinging stream reactor[J].Energy&Fuels, 2010, 24(2):1207-1212.
• [17]陈英楠,李永红,李鑫钢,等.流动状态对甲烷水合物生成速率影响的研究[J].现代化工, 2014, 34(8):152-155.CHEN Y N, LI Y H, LI X G, et al. Study on the effect of flow state on methane hydrate formation rate[J]. Modern Chemical Industry, 2014, 34(8):152-155.
• [18] MAHDI A K, MOSTAFA A, et al. Methane hydrate formation in the presence of ZnO nanoparticle and SDS application[J]. Journal of Natural Gas Science and Engineering, 2018,54(4):120-130.
• [19]赵健龙,马贵阳,潘振,等.烷基多糖苷对甲烷水合物生成影响[J].化学工程, 2018, 46(9):17-22.ZHAO J L, MA G Y, PAN Z, et al. Effect of alkyl polyglycosides on formation of methane hydrate[J]. Chemical Engineering, 2018,46(9):17-22.
• [20] GANJI H, MANTEGHIAN M, SADAGHIANI ZADEH K, et al. Effect of different surfactants on methane hydrate formation rate,stability and storage capacity[J]. Fuel, 2007, 86(3):434-441.
• [21]白净,李凌乾,刘风莉,等.机械扰动强化气体水合物快速生成研究进展[J].化工进展, 2018, 37(1):60-67.BAI J, LI L Q, LIU F L, et al. Research progress on rapid formation of gas hydrate enhanced by mechanical disturbance[J].Chemical Industry and Engineering Progress, 2018, 37(1):60-67.
• [22]朱建华,陈光进,罗艳托.甲烷-四氢呋喃-水体系水合物生成动力学的实验和模型化研究[J].化工学报, 2006, 57(5):1154-1158.ZHU J H, CHEN G J, LUO Y T. Experimental and modeling study of hydrate formation kinetics in methane-tetrahydrofuran-water system[J]. Journal of Chemical Industry and Engineering(China), 2006, 57(5):1154-1158.
• [23] ZHONG D L, HE S Y, SUN D J, et al. Comparison of methane hydrate formation in stirred reactor and porous media in the presence of SDS[J]. Energy Procedia, 2014(61):1573-1576.