[1]柳 扬,吕晓方,史博会,等.含蜡W/O体系水合物成核特性与诱导期模型[J].常州大学学报(自然科学版),2021,33(05):77-86.[doi:10.3969/j.issn.2095-0411.2021.05.010]
 LIU Yang,LYU Xiaofang,SHI Bohui,et al.Hydrate Nucleation Characteristics of Waxy W/O(Water-in-Oil) Systems and Its Induction Time Model[J].Journal of Changzhou University(Natural Science Edition),2021,33(05):77-86.[doi:10.3969/j.issn.2095-0411.2021.05.010]
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含蜡W/O体系水合物成核特性与诱导期模型()
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常州大学学报(自然科学版)[ISSN:2095-0411/CN:32-1822/N]

卷:
第33卷
期数:
2021年05期
页码:
77-86
栏目:
石油及天然气工程
出版日期:
2021-09-28

文章信息/Info

Title:
Hydrate Nucleation Characteristics of Waxy W/O(Water-in-Oil) Systems and Its Induction Time Model
文章编号:
2095-0411(2021)05-0077-10
作者:
柳 扬1 吕晓方1 史博会2 陈玉川2 周诗岽1 雷 云1 于鹏飞1 闫柯乐3
(1. 常州大学 石油工程学院, 江苏 常州 213164; 2. 中国石油大学(北京)机械与储运工程学院, 北京 102249; 3. 中国石油化工股份有限公司 青岛安全工程研究院, 山东 青岛 266071)
Author(s):
LIU Yang1 LYU Xiaofang1 SHI Bohui2 CHEN Yuchuan2 ZHOU Shidong1 LEI Yun1 YU Pengfei1 YAN Kele3
(1. School of Petroleum Engineering, Changzhou University, Changzhou 213164, China; 2. School of Mechanical and Storage & Transportation Engineering, China University of Petroleum-Beijing, Beijing 102249, China; 3. Research Institute of Safety Enginee
关键词:
水合物 成核驱动力 传质 诱导期 模型
Keywords:
hydrates nucleation driving force mass transfer induction time model
分类号:
TH 3
DOI:
10.3969/j.issn.2095-0411.2021.05.010
文献标志码:
A
摘要:
明确含蜡W/O(油包水型乳状液)体系水合物成核特性是保障深海油气开采及集输管道安全的关键, 水合物生成诱导期是描述成核特性的基础参数。基于反应釜中含蜡及不含蜡W/O体系水合物生成诱导期实验, 首先定义实验体系诱导期为体系达到相平衡温度时刻与观测到升温峰时刻间的时间间隔; 其次发现含蜡体系诱导期显著长于不含蜡体系的诱导期, 且随着W/O体系含蜡量增加, 诱导期延长。根据蜡晶油水界面吸附理论以及水合物界面成核特性, 认为油水界面吸附的蜡晶将增加成核的传质阻力, 延长诱导期。与气-水体系相比, W/O体系水合物成核除了受到本征驱动力驱动, 还受到异相成核作用以及传质作用等的影响。最后, 基于上述机理, 首次建立了反应釜中考虑蜡晶对传质影响的W/O体系水合物诱导期模型, 预测相对误差小于15%。
Abstract:
Clarifying the characteristics and mechanisms of hydrate nucleation in W/O emulsion systems is essential to guarantee the safety of deep-water oil and gas development as well as gathering lines. Hydrate formation induction time is the critical parameter to describe hydrate nucleation. Based on the hydrate formation induction time experiments of W/O systems with and without wax in the autoclave, firstly, the time interval between the time point when the system reached its phase equilibrium temperature and the time point when an obvious temperature increase peak was observed and defined as the induction time of the experimental system. Thereafter, it was found that the induction time of wax-containing systems was significantly longer than that of the wax-free system. Meanwhile, the induction time increased with increasing wax content of W/O systems. According to the theory of wax adsorption at the water-oil interface and interfacial nucleation characteristics of hydrates, it was supposed that the adsorbed wax crystals on the surface of water droplets would increase the resistance of hydrate nucleation, and prolong the induction time. Compared to the gas-water system, hydrate nucleation in W/O systems was not only driven by the intrinsic driving force, but also the heterogeneous nucleation and mass transfer effect. Finally,a model, which considered the effect of wax crystal on the mass transfer process during hydrate nucleation, was first developed to predict the induction time of W/O systems in the autoclave, and showed good predicting accuracy(relative deviation is less than 15%).

参考文献/References:

[1]宫敬, 王玮. 海洋油气混输管道流动安全保障[M]. 北京: 科学出版社, 2016.
[2]SLOAN E D, KOH C A, SUM A K. Natural gas hydrates in flow assurance[M]. Oxford: Gulf Professional Publishing, 2010.
[3]宋光春, 李玉星, 王武昌, 等. 油气管道水合物堵塞机理研究进展[J]. 化工进展, 2018, 37(7): 2473-2481.
[4]吕晓方, 左江伟, 路大勇, 等. 流动体系CO2水合物诱导时间影响因素敏感性分析[J]. 常州大学学报(自然科学版), 2019, 31(6): 60-68.
[5]GAO S Q. Investigation of interactions between gas hydrates and several other flow assurance elements[J]. Energy and Fuels, 2008, 22(5): 3150-3153.
[6]DE OLIVEIRA M C K, TEIXEIRA A, VIEIRA L C, et al. Flow assurance study for waxy crude oils[J]. Energy and Fuels, 2012, 26(5): 2688-2695.
[7]ZHENG H M, HUANG Q Y, WANG W, et al. Induction time of hydrate formation in water-in-oil emulsions[J]. Industrial & Engineering Chemistry Research, 2017, 56(29): 8330-8339.
[8]SHI B H, CHAI S, DING L, et al. An investigation on gas hydrate formation and slurry viscosity in the presence of wax crystals[J]. AIChE Journal, 2018, 64(9): 3502-3518.
[9]CHEN Y C, SHI B H, LIU Y, et al. Experimental and theoretical investigation of the interaction between hydrate formation and wax precipitation in water-in-oil emulsions[J]. Energy and Fuels, 2018, 32(9): 9081-9092.
[10]LIU Y, SHI B H, DING L, et al. Investigation of hydrate agglomeration and plugging mechanism in low-wax-content water-in-oil emulsion systems[J]. Energy and Fuels, 2018, 32(9): 8986-9000.
[11]史博会, 柴帅, 柳扬, 等. 含蜡晶天然气水合物浆液黏度的影响因素[J]. 天然气工业, 2017, 37(5): 97-105.
[12]RIPMEESTER J A, ALAVI S. Some current challenges in clathrate hydrate science: nucleation, decomposition and the memory effect[J]. Current Opinion in Solid State and Materials Science, 2016, 20(6): 344-351.
[13]LYU Y N, SUN C Y, LIU B, et al. A water droplet size distribution dependent modeling of hydrate formation in water/oil emulsion[J]. AIChE Journal, 2017, 63(3): 1010-1023.
[14]LYU 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 and Technology-Revue d’IFP Energies Nouvelles, 2015, 70(6): 1111-1124.
[15]吕晓方. 高压多相体系水合物浆液生成/分解及流动规律研究[D]. 北京: 中国石油大学(北京), 2015.
[16]DALMAZZONE D, HAMED N, DALMAZZONE C. DSC measurements and modelling of the kinetics of methane hydrate formation in water-in-oil emulsion[J]. Chemical Engineering Science, 2009, 64(9): 2020-2026.
[17]KASHCHIEV D, FIROOZABADI A. Induction time in crystallization of gas hydrates[J]. Journal of Crystal Growth, 2003, 250(3/4): 499-515.
[18]KASHCHIEV D, VERDOES D, VAN ROSMALEN G M. Induction time and metastability limit in new phase formation[J]. Journal of Crystal Growth, 1991, 110(3): 373-380.
[19]NATARAJAN V, BISHNOI P R, KALOGERAKIS N. Induction phenomena in gas hydrate nucleation[J]. Chemical Engineering Science, 1994, 49(13): 2075-2087.
[20]VISINTIN R F G, LOCKHART T P, LAPASIN R, et al. Structure of waxy crude oil emulsion gels[J]. Journal of Non-Newtonian Fluid Mechanics, 2008, 149(1/2/3): 34-39.
[21]MA Q L, WANG W, LIU Y, et al. Wax adsorption at paraffin oil-water interface stabilized by Span80[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2017, 518: 73-79.
[22]CHEN G J, GUO T M. A new approach to gas hydrate modelling[J]. Chemical Engineering Journal, 1998, 71(2): 145-151.
[23]LIU Y, SHI B H, DING L, et al. Study of hydrate formation in water-in-waxy oil emulsions considering heat transfer and mass transfer[J]. Fuel, 2019, 244: 282-295.
[24]STOPOREV A S, MANAKOV A Y, KOSYAKOV V I, et al. Nucleation of methane hydrate in water-in-oil emulsions: role of the phase boundary[J]. Energy and Fuels, 2016, 30(5): 3735-3741.
[25]MOHAMMADI A H, JI H Y, BURGASS R W, et al. Gas hydrates in oil systems[C]. Vienna: SPE Europec/EAGE Annual Conference and Exhibition, 2006.
[26]VáZQUEZ G, CANCELA M A, RIVEROL C, et al. Application of the Danckwerts method in a bubble column[J]. Chemical Engineering Journal, 2000, 78(1): 13-19.
[27]SARDEING R, PAINMANAKUL P, HéBRARD G. Effect of surfactants on liquid-side mass transfer coefficients in gas-liquid systems: a first step to modeling[J]. Chemical Engineering Science, 2006, 61(19): 6249-6260.
[28]DRELICH A, GOMEZ F, CLAUSSE D, et al. Evolution of water-in-oil emulsions stabilized with solid particles[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2010, 365(1/2/3): 171-177.
[29]NESTERENKO A, DRELICH A, LU H L, et al. Influence of a mixed particle/surfactant emulsifier system on water-in-oil emulsion stability[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2014, 457(1): 49-57.
[30]柳扬. 蜡与水合物共存W/O体系流动及沉积规律研究[D]. 北京: 中国石油大学(北京), 2019.
[31]PAL R, YAN Y H, MASLIYAH J. Rheology of clay-in-oil suspensions with added water droplets[J]. Chemical Engineering Science, 1992, 47(5): 967-970.

备注/Memo

备注/Memo:
收稿日期:2021-03-29。基金项目:国家自然科学基金资助项目(52004039, 51804046, 51974037)。作者简介:柳扬(1993—), 男, 安徽六安人, 博士, 讲师。E-mail: liu.y@cczu.edu.cn
更新日期/Last Update: 1900-01-01