油水体系内水合物的生成:温度、压力和搅拌速率影响
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摘要
水合物在管道内的生成对流动安全保障构成了极大威胁。为研究水合物在油水体系内的生成特性,本文以天然气、柴油、水为实验介质,在高压可视反应釜内开展了一系列不同温度、压力和搅拌速率的水合物生成实验。根据测试实验中温度、压力的变化趋势,首先分析了两种不同实验步骤下水合物的生成过程。然后,基于从反应釜可视窗处观察到的实验现象,研究了温度、压力和搅拌速率对水合物生成和分布位置、水合物生成形态及水合物形态演化过程的影响。实验中,可以观察到水合物的聚集、沉积和壁面膜生长现象。同时,实验还研究了温度、压力和搅拌转速对诱导时间、壁面水合物膜生长速率及气体消耗速率等水合物生成动力学参数的影响。本文研究成果可为油气管道水合物防治技术的发展提供理论支持。
Hydrate formation in pipelines poses a great threat to pipeline flow assurance. To investigate the characteristics of hydrate formation in oil-water systems, a high-pressure cell equipped with visual windows was used where a series of hydrate formation experiments were performed from natural gas +diesel oil + water systems at different temperatures, pressures and rotation rates. According to the temperature and pressure profiles in test experiments, the processes of hydrate formation under two kinds of experimental procedures were analyzed first. Then, based on the experimental phenomena observed through the visual windows, the influences of temperature, pressure and rotation rate on the places of hydrate formation and distribution, hydrate morphologies and hydrate morphological evolvements were investigated. Hydrate agglomeration, hydrate deposition and hydrate film growth on the wall were observed in the experiments. In addition, the influences of temperature, pressure and rotation rate on the kinetic parameters of hydrate formation such as induction time, hydrate film growth rate and gas consumption rate were also studied. The results and conclusions in this paper can provide theoretical supports for the development of hydrate management strategies in oil and gas pipelines.
Hydrate formation in pipelines poses a great threat to pipeline flow assurance. To investigate the characteristics of hydrate formation in oil-water systems, a high-pressure cell equipped with visual windows was used where a series of hydrate formation experiments were performed from natural gas +diesel oil + water systems at different temperatures, pressures and rotation rates. According to the temperature and pressure profiles in test experiments, the processes of hydrate formation under two kinds of experimental procedures were analyzed first. Then, based on the experimental phenomena observed through the visual windows, the influences of temperature, pressure and rotation rate on the places of hydrate formation and distribution, hydrate morphologies and hydrate morphological evolvements were investigated. Hydrate agglomeration, hydrate deposition and hydrate film growth on the wall were observed in the experiments. In addition, the influences of temperature, pressure and rotation rate on the kinetic parameters of hydrate formation such as induction time, hydrate film growth rate and gas consumption rate were also studied. The results and conclusions in this paper can provide theoretical supports for the development of hydrate management strategies in oil and gas pipelines.
引文
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[16]丁麟,史博会,吕晓方,等.天然气水合物形成与生长影响因素综述[J].化工进展,2016,35(1):57-64.DING L,SHI B H,LüX F,et al.Review of influence factors of natural gas hydrate formation and growth[J].Chemical Industry and Engineering Progress,2016,35(1):57-64.
[17]ENGLEZOS P,KALOGERAKIS N,DHOLABHAI P D,et al.Kinetics of formation of methane and ethane gas hydrates[J].Chemical Engineering Science,1987,42(11):2647-2658.
[18]WANG W C,JIANG K,LI Y X,et al.Kinetics of methane gas hydrate formation with microscale sand in an autoclave with windows[J].Fuel,2017,209:85-95.
[19]SONG G C,LI Y X,WANG W C,et al.Experimental study of hydrate dissociation in oil-dominated systems using a high-pressure visual cell[J].Journal of Natural Gas Science and Engineering,2017,45:26-37.
[20]POINDEXTER M K,ZAKI N N,KILPARTRICK P K,et al.Factors contributing to petroleum foaming.Part 1:Crude oil systems[J].Energy&Fuels,2002,16(3):700-710.
[21]MORRISSY S A,LIM V W,MAY E F,et al.Micromechanical cohesive force measurements between precipitated asphaltene solids and cyclopentane hydrates[J].Energy&Fuels,2015,29:6277-6285.
[22]ZHAO X,QIU Z S,HUANG W A.Characterization of kinetics of hydrate formation in the presence of kinetic hydrate inhibitors during deepwater drilling[J].Journal of Natural Gas Science&Engineering,2015,22:270-278.
[23]AMAN Z M,LORENZO M D,KOEIZLSKI K,et al.Hydrate formation and deposition in a gas-dominant flowloop:initial studies of the effect of velocity and subcooling[J].Journal of Natural Gas Science&Engineering,2016,35:1490-1498.
[24]CAMEIRAO A,FEZOUA A,OUABBAS Y,et al.Agglomeration of gas hydrate in a water-in-oil emulsion:experimental and modeling studies[C]//International Conference on Gas Hydrates,2011.Edinburg,United Kingdom.
[2]陈光进,孙长宇,马庆兰.气体水合物科学与技术[M].北京:化学工业出版社,2008:223-225.CHEN G J,SUN C Y,MA Q L.Gas hydrates science and technology[M].Beijing:Chemical Industry Press,2008:223-225.
[3]HAMMERSCHMIDT E G.Formation of gas hydrates in natural gas transmission lines[J].Industrial&Engineering Chemistry,1934,26(8):851-855.
[4]SLOAN E D.Natural gas hydrates in flow assurance[M].New York:Elsevier Science Ltd.,2010:1-36.
[5]SONG G C,LI Y X,WANG W C,et al.Investigation of hydrate plugging in natural gas+diesel oil+water systems using a highpressure flow loop[J].Chemical Engineering Science,2017,158:480-489.
[6]WANG W C,FAN S S,LIANG D Q,et al.Experimental study on flow characteristics of tetrahydrofuran hydrate slurry in pipelines[J].Journal of Natural Gas Chemistry,2010,19(3):318-322.
[7]CHEN J,SUN C Y,PENG B Z,et al.Screening and compounding of gas hydrate anti-agglomerants from commercial additives through morphology observation[J].Energy&Fuels,2013,27(5):2488-2496.
[8]GRASSO G A.Investigation of hydrate formation and transportability in multiphase flow system[D].Golden:Colorado School of Mines,2015.
[9]LüX F,SHI B H,WANG Y,et al.Experimental study on hydrate induction time of gas-saturated water-in-oil emulsion using a highpressure flow loop[J].Oil&Gas Science&Technology,2015,70(6):253-268.
[10]ARJMANDI M,TOHID B,DANESH A,et al.Is subcooling the right driving force for testing low-dosage hydrate inhibitors?[J].Chemical Engineering Science,2005,60(5):1313-1321.
[11]LI X G,CHEN C,CHEN Y N,et al.Kinetics of methane clathrate hydrate formation in water-in-oil emulsion[J].Energy&Fuels,2015,29(4):2277-2288.
[12]MOFRAD H R,GANJI H,NAZARI K,et al.Rapid formation of dry natural gas hydrate with high capacity and low decomposition rate using a new effective promoter[J].Journal of Petroleum Science&Engineering,2016,147:756-759.
[13]FU Z S,LIU M,XU J T,et al.Stabilization of water-in-octane nanoemulsion.PartⅠ:stabilized by mixed surfactant systems[J].Fuel,2010,89(10):2838-2843.
[14]TURNER D J,MILLER K T,SLOAN E D.Methane hydrate formation and an inward growing shell model in water-in-oil dispersions[J].Chemical Engineering Science,2009,64(18):3996-4004.
[15]潘振,王喆,商丽艳,等.油水乳液体系中甲烷水合物生成研究进展[J].化工进展,2017,36(12):4392-4402.PAN Z,WANG Z,SHANG L Y,et al.Research progress on methane hydrate formation in oil and water emulsion[J].Chemical Industry and Engineering Progress,2017,36(12):4392-4402.
[16]丁麟,史博会,吕晓方,等.天然气水合物形成与生长影响因素综述[J].化工进展,2016,35(1):57-64.DING L,SHI B H,LüX F,et al.Review of influence factors of natural gas hydrate formation and growth[J].Chemical Industry and Engineering Progress,2016,35(1):57-64.
[17]ENGLEZOS P,KALOGERAKIS N,DHOLABHAI P D,et al.Kinetics of formation of methane and ethane gas hydrates[J].Chemical Engineering Science,1987,42(11):2647-2658.
[18]WANG W C,JIANG K,LI Y X,et al.Kinetics of methane gas hydrate formation with microscale sand in an autoclave with windows[J].Fuel,2017,209:85-95.
[19]SONG G C,LI Y X,WANG W C,et al.Experimental study of hydrate dissociation in oil-dominated systems using a high-pressure visual cell[J].Journal of Natural Gas Science and Engineering,2017,45:26-37.
[20]POINDEXTER M K,ZAKI N N,KILPARTRICK P K,et al.Factors contributing to petroleum foaming.Part 1:Crude oil systems[J].Energy&Fuels,2002,16(3):700-710.
[21]MORRISSY S A,LIM V W,MAY E F,et al.Micromechanical cohesive force measurements between precipitated asphaltene solids and cyclopentane hydrates[J].Energy&Fuels,2015,29:6277-6285.
[22]ZHAO X,QIU Z S,HUANG W A.Characterization of kinetics of hydrate formation in the presence of kinetic hydrate inhibitors during deepwater drilling[J].Journal of Natural Gas Science&Engineering,2015,22:270-278.
[23]AMAN Z M,LORENZO M D,KOEIZLSKI K,et al.Hydrate formation and deposition in a gas-dominant flowloop:initial studies of the effect of velocity and subcooling[J].Journal of Natural Gas Science&Engineering,2016,35:1490-1498.
[24]CAMEIRAO A,FEZOUA A,OUABBAS Y,et al.Agglomeration of gas hydrate in a water-in-oil emulsion:experimental and modeling studies[C]//International Conference on Gas Hydrates,2011.Edinburg,United Kingdom.