含蜡和防聚剂体系天然气水合物浆液生成及流动特性

doi:10.16085/j.issn.1000-6613.2017-1405

化工进展 ›› 2018, Vol. 37 ›› Issue (06): 2182-2191.DOI: 10.16085/j.issn.1000-6613.2017-1405

含蜡和防聚剂体系天然气水合物浆液生成及流动特性

史博会¹, 雍宇¹, 柳杨¹, 李墨竹¹, 丁麟¹, 吕晓方², 吴海浩¹, 宫敬¹

1 中国石油大学(北京)油气管道输送安全国家工程实验室/石油工程教育部重点实验室/城市油气输配技术北京市重点实验室, 北京 102249;
2 常州大学石油工程学院油气储运重点实验室, 江苏常州 213016

收稿日期:2017-07-12 修回日期:2018-02-18 出版日期:2018-06-05 发布日期:2018-06-05
通讯作者: 博会(1984-),女,博士,讲师,硕士生导师,主要从事油气多相管流及水合物流动保障技术的研究。
作者简介:博会(1984-),女,博士,讲师,硕士生导师,主要从事油气多相管流及水合物流动保障技术的研究。E-mail:bh.shi@cup.edu.cn。
基金资助:
国家重点研发计划（2016YFC0303704）、国家自然科学基金（51534007）、国家重大科技专项（2016ZX05028004-001，2016ZX05066005-001）及中国石油大学（北京）科研基金（C201602）项目。

Characteristics of natural gas hydrate slurry formation and flow in systems with wax and anti-agglomerates

SHI Bohui¹, YONG Yu¹, LIU Yang¹, LI Mozhu¹, DING Lin¹, LÜ Xiaofang², WU Haihao¹, GONG Jing¹

1 National Engineering Laboratory for Pipeline Safety/MOE Key Laboratory of Petroleum Engineering/Beijing Key Laboratory of Urban Oil and Gas Distribution Technology, China University of Petroleum(Beijing), Beijing 102249, China;
2 Key Laboratory of Oil and Gas Storage & Transportation Technology, Changzhou University, Changzhou 213016, Jiangsu, China

Received:2017-07-12 Revised:2018-02-18 Online:2018-06-05 Published:2018-06-05

摘要/Abstract

摘要： 研究含蜡和防聚剂体系天然气水合物浆液生成及流动特性，对于在深水含蜡油气田实施水合物浆液输送技术、解决海底管道多相混输流动保障问题具有重要意义。本文基于高压水合物环路开展的蜡晶存在与否，对含防聚剂天然气水合物浆液生成及流动影响进行实验，对比分析所获得的实验温度、压力、水合物生成体积分数、流量和压降等宏观参数变化，同时结合颗粒录影显微仪（PVM）、颗粒粒度分析仪（FBRM）等微观数据分析，研究了蜡晶对含防聚剂的天然气水合物浆液生成及流动特性的影响规律。结果表明：相比于无蜡体系，含蜡体系中蜡晶会在防聚剂的作用下吸附在油水界面，减小气水成核反应表面积，增大水合物生成传质阻力，从而抑制水合物生成成核，延长水合物生成诱导期，并使水合物生成量降低；蜡晶与水滴之间团聚物的形成，促进了其与水合物颗粒间的聚并，浆液体系黏度增加，流动性显著下降。含蜡和防聚剂体系天然气水合物浆液生成及流动涉及学科复杂，未来仍需基于已获得的蜡与水合物相关独立研究成果，进一步探讨蜡与水合物之间的耦合作用机理。

关键词: 水合物, 蜡, 成核, 浆液, 多相流

Abstract: The study of characteristics of natural gas hydrate slurry formation and flow with wax crystals and anti-agglomerates, is of great significance for the implementation of hydrate slurry technology in deep water waxy oil and gas fields to solve multiphase flow assurance issues. Based on the experiments of hydrate slurry formation and flow with and without wax crystals in the presence of anti-agglomerates carried out in a high-pressure hydrate flow loop, the variations of temperature, pressure, hydrate formation volume fraction, flow rate and pressure drop were compared and analyzed, and the effect of wax crystals on the characteristics of natural gas hydrate slurry formation and flow in the presence of anti-agglomerates was studied combined with the PVM and FBRM microscopic data analysis. The results indicated that the wax crystals would adsorb on the oil-water interfaces under the action of anti-agglomerates, reduce the reaction area of air-water nucleation and increase the mass transfer resistance of hydrate formation, thus inhibiting the formation and nucleation of hydrates leading to extension of the hydrate formation induction time and reduction of hydrate formation amount comparing with that in the wax free system. The aggregate formation coupling between the wax crystals and water droplets promoted the coalescence with hydrate particles, which increased the viscosity and decreased the fluidity of the hydrate slurry remarkably. The formation and flow of natural gas hydrate slurry with wax in the presence of anti-agglomerates was complex. And, the coupling mechanism between wax crystals and hydrates should be investigated further in the future, based on the existed independent research results of wax crystals and hydrates.

Key words: hydrate, wax, nucleation, slurry, multiphase flow

中图分类号:

TE866

史博会, 雍宇, 柳杨, 李墨竹, 丁麟, 吕晓方, 吴海浩, 宫敬. 含蜡和防聚剂体系天然气水合物浆液生成及流动特性[J]. 化工进展, 2018, 37(06): 2182-2191.

SHI Bohui, YONG Yu, LIU Yang, LI Mozhu, DING Lin, LÜ Xiaofang, WU Haihao, GONG Jing. Characteristics of natural gas hydrate slurry formation and flow in systems with wax and anti-agglomerates[J]. Chemical Industry and Engineering Progress, 2018, 37(06): 2182-2191.

参考文献

[1] 段纪淼,宫敬,张宇,等. 多相混输管道蜡沉积研究进展[J]. 油气储运, 2011, 30(4):241-248. DUAN J M, GONG J, ZHANG Y, et al. Research progress of wax deposition in multiphase mixed transmission pipeline[J]. Oil & Gas Storage and Transportation, 2011, 30(4):241-248.
[2] SLOAN E D, KOH C A. Clathrate hydrates of natural gases[M]. New York:CRC Press, 2007.
[3] 闫柯乐,邹兵,姜素霞,等. 水合物浆液流动与流变特性研究进展[J]. 化工进展, 2015, 34(7):1817-1825. YAN K L, ZOU B, JIANG S X, et al. Review on flow characteristics and rheological properties of hydrate slurry[J]. Chemical Industry and Engineering Progress, 2015, 34(7):1817-1825.
[4] 丁麟,史博会,吕晓方,等. 天然气水合物的生成对浆液流动稳定性影响综述[J]. 化工进展, 2016, 35(10):3118-3128. DING L, SHI B H, LÜ X F, et al. Investigation on the effects of natural gas hydrate formation on slurry flow stability[J]. Chemical Industry and Engineering Progress, 2016, 35(10):3118-3128.
[5] SUM A K, KOH C A, SLOAN E D. Developing a comprehensive understanding and model of hydrate in multiphase flow:from laboratory measurements to field applications[J]. Energy & Fuels, 2012, 26(7):4046-4052.
[6] 宫敬,史博会,吕晓方. 多相混输管道水合物生成及其浆液输送[J]. 中国石油大学学报(自然科学版), 2013, 37(5):163-167.GONG J,SHI B H,LÜ X F. Gas hydrate formation and hydrate slurry flow in multiphase transportation system[J]. Journal of China University of Petroleum(Edition of Natural Science), 2013, 37(5):163-167.
[7] GONG J, ZHANG Y, LIAO L, et al. Wax deposition in the oil/gas two-phase flow for a horizontal pipe[J]. Energy & Fuels, 2011, 25(4):1624-1632.
[8] MAHABADIAN M A, CHAPOY A, BURGASS R, et al. Mutual effects of paraffin waxes and clathrate hydrates:a multiphase integrated thermodynamic model and experimental measurements[J]. Fluid Phase Equilibria, 2016, 427:438-459.
[9] EDMONDS B, MOORWOOD R A S, SZCZEPANSKI R. A unified framework for calculating solid deposition from petroleum fluids including waxes, asphaltenes, hydrates and scales[J]. Fluid Phase Equilibria, 1999, 160(9):481-489.
[10] JI H Y. Thermodynamic modelling of wax and integrated wax-hydrate[D]. Scotland:Heriot-Watt University, 2004.
[11] MOHAMMADI A H, JI H Y, BURGASS R W, et al. Gas hydrates in oil systems[C]//SPE Europec/EAGE Annual Conference and Exhibition, 2006.
[12] 寇杰,王巍,杨文. 海底混输管道水合物生成对析蜡的影响[J]. 中国石油大学学报(自然科学版), 2013, 37(1):144-146. KOU J, WANG W, YANG W. Influence of hydrate formation on wax precipitation in subsea multiphase pipeline[J]. Journal of China University of Petroleum(Edition of Natural Science), 2013, 37(1):144-146.
[13] 寇杰,张楠,李云. 海底混输管道析蜡对水合物生成的影响[J]. 中国石油大学学报(自然科学版), 2016, 40(4):171-175. KOU J, ZHANG N, LI Y. Effect of wax formation on hydrate precipitation in subsea multiphase pipeline[J]. Journal of China University of Petroleum(Edition of Natural Science), 2016, 40(4):171-175.
[14] 刘火强. 海底混输管道水合物与蜡沉积关系研究[D]. 青岛:中国石油大学(华东), 2012. LIU H Q. Study on the relationship between hydrate formation and wax deposition in subsea pipeline[D]. Qingdao:China University of Petroleum (East China), 2012.
[15] GAO S. Investigation of interactions between gas hydrates and several other flow assurance elements[J]. Energy & Fuels, 2008, 22(5):3150-3153.
[16] DE OLIVEIRA M C K, TEIXEIRA A, VIEIRA L C, et al. Flow assurance study for waxy crude oils[J]. Energy & Fuels, 2012, 26(5):2688-2695.
[17] 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. CHEN G J, SUN C Y, MA Q L. Science and technology of gas hydrate[M]. Beijing:Chemical Industry Press, 2008.
[18] 吴强,张家豪,高霞,等. 热力学促进剂对瓦斯水合物相平衡的影响[J]. 黑龙江科技大学学报, 2016, 26(3):235-239. WU Q, ZHANG J H, GAO X, et al. Effect of thermodynamics promoters on phase equilibrium of mine gas hydrate[J]. Journal of Heilongjiang University of Science and Technology, 2016, 26(3):235-239.
[19] CHEN G J, GUO T M. A new approach to gas hydrate modelling[J]. Chemical Engineering Journal, 1998, 71(2):145-151.
[20] 马庆兰,陈光进,郭天民. 含极性抑制剂体系中水合物生成条件的研究[J]. 高校化学工程学报, 2000, 14(1):7-11. MA Q L, CHEN G J, GUO T M. Study on the hydrate formation conditions from system containing polar inhibitor[J]. Journal of Chemical Engineering of Chinese Universities, 2000, 14(1):7-11.
[21] 陈光进,马庆兰,郭天民. 水合物模型的建立及在含盐体系中的应用[J]. 石油学报, 2000, 21(1):64-70. CHEN G J, MA Q L, GUO T M. A new hydrate model and its extended application in electrolyte containing system[J]. Acta Petrolei Sinica, 2000, 21(1):64-70.
[22] DING L, SHI B H, LV X F, et al. Investigation of natural gas hydrate slurry flow properties and flow patterns using a high pressure flow loop[J]. Chemical Engineering Science, 2016, 146:199-206.
[23] DING L, SHI B H, LV X F, et al. Hydrate formation and plugging mechanisms in different gas-liquid flow patterns[J]. Industrial & Engineering Chemistry Research, 2017, 56(14):4173-4184.
[24] LV X F, SHI B H, WANG Y, et al. Experimental study on hydrate induction time of gas-saturated water-in-oil emulsion using a high-pressure flow loop[J]. Oil & Gas Science & Technology, 2014, 70(6):253-268.
[25] MAHABADIAN M A, CHAPOY A, BURGASS R, et al. Development of a multiphase flash in presence of hydrates:experimental measurements and validation with the CPA equation of state[J]. Fluid Phase Equilibria, 2016, 414(1):117-132.
[26] MICHELSEN M L. Calculation of multiphase equilibrium[J]. Computers & Chemical Engineering, 1994, 18(7):545-550.
[27] MICHELSEN M L. The isothermal flash problem. Part I. Stability[J]. Fluid Phase Equilibria, 1982, 9(1):1-19.
[28] 王巍. 海底混输管道水合物生成对析蜡的影响研究[D]. 青岛:中国石油大学(华东), 2011. WANG W. The study on the influence of hydrate on wax appearance in subsea multiphase pipeline[D]. Qingdao:China University of Petroleum(East China), 2011.
[29] 张凯. 海底管道液烃存在及蜡晶析出对水合物生成影响研究[D]. 青岛:中国石油大学(华东), 2011. ZHANG K. Study of the influence of liquid hydrocarbon existence and wax precipitation on hydrate formation in subsea pipeline[D]. Qingdao:China University of Petroleum(East China), 2011.
[30] SHI B H, CHAI S, LIU YANG, et al. Experimental study on natural gas hydrates nucleation induction time in the presence of wax crystal[C]//9th International Conference of Gas Hydrates, 2017.
[31] WANG P, WANG W, GONG J, et al. Effects of the dispersed phase on oil/water wax deposition[J]. Journal of Energy Resources Technology, 2013, 135(4):42-59.
[32] MA Q, WANG W, LIU Y, et al. Wax adsorption at paraffin oil-water interface stabilized by Span80[J]. Colloids & Surfaces A Physicochemical & Engineering Aspects, 2017, 518:73-79.
[33] SHI B H, GONG J, SUN C Y, et al. An inward and outward natural gas hydrates growth shell model considering intrinsic kinetics, mass and heat transfer[J]. Chemical Engineering Journal, 2011, 171(3):1308-1316.
[34] SARICA C, PANACHAROENSAWAD E. Review of paraffin deposition research under multiphase flow conditions[J]. Energy & Fuels, 2012, 26(7):3968-3978.
[35] AIYEJINA A, CHAKRABARTI D P, PILGRIM A, et al. Wax formation in oil pipelines:a critical review[J]. International Journal of Multiphase Flow, 2011, 37(7):671-694.
[36] SONG X, XIN F, YAN H, et al. Intensification and kinetics of methane hydrate formation under heat removal by phase change of n-tetradecane[J]. AIChE Journal, 2015, 61(10):3441-3450.
[37] OLIVEIRA M C K D, TEIXEIRA A, VIEIRA L C, et al. Flow assurance study for waxy crude oils[J]. Energy & Fuels,2011,26(5):2688-2695.
[38] CAMARGO R, PALERMO T, SINQUIN A, et al. Rheological characterization of hydrate suspensions in oil dominated systems[J]. Annals of the New York Academy of Sciences, 2010, 912(1):906-916.
[39] CAMARGO R, PALERMO T, MAUREL P, et al. Rheological properties of hydrate suspensions in an asphaltenic crude oil[C]//The 4th International Conference on Gas Hydrates, 2002.
[40] PAUCHARD V, DARBOURET M, PALERMO T, et al. Gas hydrate slurry flow in a black oil:prediction of gas hydrate particles agglomeration and linear pressure drop[C]//The 13th International Conference on Multiphase Production Technology, 2007.
[41] YANNICK P, SVEN N, PHILIPPE M, et al. Flow of hydrates dispersed in production lines[C]//Society of Petroleum Engineers, 2003.
[42] 陈刚,李小龙,张洁. 原油组分相互作用对析蜡的影响机理[J]. 石油学报(石油加工), 2013, 29(5):844-850. CHEN G, LI X L, ZHANG J. Mechanism of the effect of components interaction on wax precipitation process in crude oil[J]. Acta Petrolei Sinica(Petroleum Processing Section), 2013, 29(5):844-850.

含蜡和防聚剂体系天然气水合物浆液生成及流动特性

Characteristics of natural gas hydrate slurry formation and flow in systems with wax and anti-agglomerates

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]	张杰, 白忠波, 冯宝鑫, 彭肖林, 任伟伟, 张菁丽, 刘二勇. PEG及其复合添加剂对电解铜箔后处理的影响[J]. 化工进展, 2023, 42(S1): 374-381.
[2]	王云飞, 秦蕊, 郑利军, 李焱, 李清平. 旋转填充床CFD模拟研究进展[J]. 化工进展, 2023, 42(S1): 1-9.
[3]	黄益平, 李婷, 郑龙云, 戚傲, 陈政霖, 史天昊, 张新宇, 郭凯, 胡猛, 倪泽雨, 刘辉, 夏苗, 主凯, 刘春江. 三级环流反应器中气液流动与传质规律[J]. 化工进展, 2023, 42(S1): 175-188.
[4]	董佳宇, 王斯民. 超声强化对二甲苯结晶特性及调控机理实验[J]. 化工进展, 2023, 42(9): 4504-4513.
[5]	王谨航, 何勇, 史伶俐, 龙臻, 梁德青. 气体水合物阻聚剂研究进展[J]. 化工进展, 2023, 42(9): 4587-4602.
[6]	李由, 吴越, 钟禹, 林琦璇, 任俊莉. 酸性熔盐水合物预处理麦秆高效制备木糖及其对酶解效率的影响[J]. 化工进展, 2023, 42(9): 4974-4983.
[7]	赵健, 卓泽文, 董航, 高文健. 含蜡原油及其乳状液体系微观结构观测的新方法[J]. 化工进展, 2023, 42(8): 4372-4384.
[8]	尹新宇, 皮丕辉, 文秀芳, 钱宇. 特殊浸润性材料在防治油气管道中水合物成核与聚集的应用[J]. 化工进展, 2023, 42(8): 4076-4092.
[9]	张凯, 吕秋楠, 李刚, 李小森, 莫家媚. 南海海泥中甲烷水合物的形貌及赋存特性[J]. 化工进展, 2023, 42(7): 3865-3874.
[10]	杨扬, 孙志高, 李翠敏, 李娟, 黄海峰. 静态条件下表面活性剂OP-13促进HCFC-141b水合物生成[J]. 化工进展, 2023, 42(6): 2854-2859.
[11]	孙征楠, 李洪晶, 荆国林, 张福宁, 颜飚, 刘晓燕. EVA及其改性聚合物在原油降凝剂领域的应用[J]. 化工进展, 2023, 42(6): 2987-2998.
[12]	田启凯, 郑海萍, 张少斌, 张静, 余子夷. 混合增强的微流控通道进展[J]. 化工进展, 2023, 42(4): 1677-1687.
[13]	刘佳, 梁德青, 李君慧, 林德才, 吴思婷, 卢富勤. 油水体系水合物浆液流动保障研究进展[J]. 化工进展, 2023, 42(4): 1739-1759.
[14]	王唯, 张东旭, 李遵照, 王晓霖, 黄启玉. 油包水乳状液体系中水合物生长行为研究进展[J]. 化工进展, 2023, 42(3): 1155-1166.
[15]	赵西坡, 卞武勋, 冉宝清, 刘进超, 尹少鼎, 孙义明. 石蜡固-固相变材料的制备及性能[J]. 化工进展, 2023, 42(2): 897-906.