Prediction model of hydrate formation in bubbly flow and experimental study

doi:10.16085/j.issn.1000-6613.2022-0913

Abstract

Abstract:

Considering the risks of hydrate formation and plug in the gas hydrate wellbore, experiments were conducted to investigate methane hydrate formation in bubbly flow using flow loop. Experimental results showed that the increases of flow velocities enhance the hydrate formation rates but the increases of xanthan gum concentrations reduced the hydrae formation rates. Based on gas-liquid mass transfer mechanism, a hydrate formation prediction model in bubbly flow was developed considering the influences of rheology of continuous-phase, and the breakage, coalescence and deformation of gas bubbles on the gas-liquid interfacial area and the gas-liquid mass transfer rate. Coupling with experimental data, an empirical formula of the overall mass transfer coefficient was proposed to describe the effect of interactions between gas bubbles on the gas-liquid mass transfer rates. Compared with experimental data, the developed model predicted the quantity of hydrate formation and the hydrate formation rate with the discrepancies within ±5% and ±15% respectively. The developed model contributed to forecast the hydrate risk in the oil, gas and natural gas hydrate wellbore and laid a theoretical foundation for developing an efficiency and economic hydrate management plan in wellbore.

Key words: bubbly flow, hydrate flow assurance, hydrate formation, mass transfer

摘要：

针对可燃冰钻采井筒内易发生水合物生成和堵塞的工程问题，本文开展了泡状流条件下甲烷水合物生成实验，发现流速增加会提高水合物生成速率，黄原胶质量分数的增加会降低水合物生成速率。基于传质理论，构建了适用于可燃冰钻采井筒内泡状流条件下水合物生成预测模型，模型考虑了连续相流体流变性、气泡破裂、聚并和形变等因素对泡状流中气液界面分布和气液间传质规律的影响，并耦合实验数据，提出了气泡群间的综合传质系数经验公式，用于描述气泡间相互作用对气液间传质速率的影响。对比实验结果，所建立模型对水合物生成量和水合物生成速率的预测误差分别在±5%和±15%以内，满足工程计算需求。该模型的构建有助于精准预测油气和可燃冰钻采井筒内水合物风险，为建立经济、高效的井筒水合物防治方案奠定理论基础。

关键词: 泡状流, 水合物流动保障, 水合物生成, 传质

CLC Number:

FU Weiqi, ZHAO Zixian, YU Jing, WEI Wei, WANG Zhiyuan, HUANG Bingxiang. Prediction model of hydrate formation in bubbly flow and experimental study[J]. Chemical Industry and Engineering Progress, 2022, 41(11): 5746-5754.

付玮琪, 赵子贤, 于璟, 魏伟, 王志远, 黄炳香. 泡状流中水合物生成预测模型及实验[J]. 化工进展, 2022, 41(11): 5746-5754.

Figures/Tables 7

References 25

1	李清平, 周守为, 赵佳飞, 等. 天然气水合物开采技术研究现状与展望[J]. 中国工程科学, 2022, 24(3): 214-224.
	LI Qingping, ZHOU Shouwei, ZHAO Jiafei, et al. Research status and prospects of natural gas hydrate exploitation technology[J]. Strategic Study of CAE, 2022, 24(3): 214-224.
2	张剑波, 张伟国, 王志远, 等. 深水气井测试水合物沉积堵塞预测与防治技术[C]//第三十届全国水动力学研讨会暨第十五届全国水动力学学术会议论文集(上册). 合肥, 2019: 135-145.
	ZHANG Jianbo, ZHANG Weiguo, WANG Zhiyuan, et al. Prediction and prevention of hydrate deposition and blockage during deepwater gas well testing[C]// Proceedings of the 30th National Symposium on hydrodynamics and the 15th National Symposium on Hydrodynamics (Volume I). Hefei: 2019: 135-145.
3	杨唐杨, 于常宏, 纪佳凯, 等. 含CaCl₂的深水油基钻井液中甲烷水合物的生成规律研究[J]. 新能源进展, 2021, 9(6): 533-539.
	YANG Tangyang, YU Changhong, JI Jiakai, et al. Study on methane hydrate formation in deepwater oil-based drilling fluid containing CaCl₂ [J]. Advances in New and Renewable Energy, 2021, 9(6): 533-539.
4	FU Weiqi, WANG Zhiyuan, SUN Baojiang, et al. A mass transfer model for hydrate formation in bubbly flow considering bubble-bubble interactions and bubble-hydrate particle interactions[J]. International Journal of Heat and Mass Transfer, 2018, 127: 611-621.
5	FU Weiqi, YU Jing, XIAO Yang, et al. A pressure drop prediction model for hydrate slurry based on energy dissipation under turbulent flow condition[J]. Fuel, 2022, 311: 122188.
6	FU Weiqi, YU Jing, XU Yonghe, et al. A pressure drop prediction model for hydrate slurry based on energy dissipation under laminar flow condition[J]. SPE Journal, 2022, 27(4): 2257-2267.
7	VYSNIAUSKAS A, BISHNOI P R. A kinetic study of methane hydrate formation[J]. Chemical Engineering Science, 1983, 38(7): 1061-1072.
8	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.
9	隋金昊, 王智, 梁璇玑, 等. 动力学抑制剂与乙二醇协同作用下甲烷水合物再生成[J]. 化工进展, 2022, 41(10): 5368-5375.
	SUI Jinhao, WANG Zhi, LIANG Xuanji, et al. Paried KHI-MEG for synergistic inhibition of methane hydrate reformation[J]. Chemical Industry and Engineering Progress, 2022, 41(10): 5368-5375.
10	闫明月, 王岳, 刘嘉琪, 等. 表面活性剂对甲烷水合物生成影响研究进展[J]. 应用化工, 2021, 50(8): 2317-2325.
	YAN Mingyue, WANG Yue, LIU Jiaqi, et al. Research progress on influence factors of methane hydrate formation in surfactant solution[J]. Applied Chemical Industry, 2021, 50(8): 2317-2325.
11	MOHEBBI V, NADERIFAR A, BEHBAHANI R M, et al. Investigation of kinetics of methane hydrate formation during isobaric and isochoric processes in an agitated reactor[J]. Chemical Engineering Science, 2012, 76: 58-65.
12	GONG Jing, SHI Bohui, ZHAO Jiankui. Natural gas hydrate shell model in gas-slurry pipeline flow[J]. Journal of Natural Gas Chemistry, 2010, 19(3): 261-266.
13	宫敬, 史博会, 陈玉川, 等. 含天然气水合物的海底多相管输及其堵塞风险管控[J]. 天然气工业, 2020, 40(12): 133-142.
	GONG Jing, SHI Bohui, CHEN Yuchuan, et al. Submarine multiphase pipeline transport containing natural gas hydrate and its plugging risk prevention and control[J]. Natural Gas Industry, 2020, 40(12): 133-142.
14	王志远, 张洋洋, 张剑波, 等. 深水气井水合物流动障碍形成机制与防治方法研究进展[J]. 中国科学基金, 2021, 35(6): 992-1005.
	WANG Zhiyuan, ZHANG Yangyang, ZHANG Jianbo, et al. Research progress on formation mechanism and prevention methods of hydrate flow barrier in deep-water gas wells[J]. Bulletin of National Natural Science Foundation of China, 2021, 35(6): 992-1005.
15	DI LORENZO Mauricio, AMAN Zachary M, KOZIELSKI Karen, et al. Underinhibited hydrate formation and transport investigated using a single-pass gas-dominant flowloop[J]. Energy & Fuels, 2014, 28(11): 7274-7284.
16	WANG Zhiyuan, ZHANG Jianbo, SUN Baojiang, et al. A new hydrate deposition prediction model for gas-dominated systems with free water[J]. Chemical Engineering Science, 2017, 163: 145-154.
17	RUTHIYA Keshav C, VAN DER SCHAAF John, KUSTER Ben F M, et al. Influence of particles and electrolyte on gas hold-up and mass transfer in a slurry bubble column[J]. International Journal of Chemical Reactor Engineering, 2006, 4(1): 1-35.
18	FU Weiqi, WANG Zhiyuan, DUAN Wenguang, et al. Characterizing methane hydrate formation in the non-Newtonian fluid flowing system[J]. Fuel, 2019, 253: 474-487.
19	KAWASE Yoshinori, HASHIGUCHI Nanae. Gas—liquid mass transfer in external-loop airlift columns with Newtonian and non-Newtonian fluids[J]. The Chemical Engineering Journal and the Biochemical Engineering Journal, 1996, 62(1): 35-42.
20	FU Weiqi, WANG Zhiyuan, SUN Baojiang, et al. Multiple controlling factors for methane hydrate formation in water-continuous system[J]. International Journal of Heat and Mass Transfer, 2019, 131: 757-771.
21	ALOPAEUS Ville, KOSKINEN Jukka, KESKINEN Kari I, et al. Simulation of the population balances for liquid-liquid systems in a nonideal stirred tank. Part 2—Parameter fitting and the use of the multiblock model for dense dispersions[J]. Chemical Engineering Science, 2002, 57(10): 1815-1825.
22	HIBIKI Takashi, ISHII Mamoru. Interfacial area concentration in steady fully-developed bubbly flow[J]. International Journal of Heat and Mass Transfer, 2001, 44(18): 3443-3461.
23	LIU Liu, YAN Hongjie, ZHAO Guojian. Experimental studies on the shape and motion of air bubbles in viscous liquids[J]. Experimental Thermal and Fluid Science, 2015, 62: 109-121.
24	BESAGNI G, INZOLI F, ZIEGENHEIN T, et al. Bubble aspect ratio in dense bubbly flows: experimental studies in low Morton-number systems[J]. Journal of Physics: Conference Series, 2017, 923: 012014.
25	FU Weiqi, CHEN Bengang, ZHANG Kaibo, et al. Rheological behavior of hydrate slurry with xanthan gum and carboxmethylcellulose under high shear rate conditions[J]. Energy & Fuels, 2022, 36(6): 3169-3183.

序号	压力/MPa	温度/K	流速/m·s^-1	含气率（体积分数）/%	黄原胶质量分数/%
1	8.078	278.2	0.952	4.48	0
2	6.044	278.2	1.024	3.01	0
3	6.031	277.29	1.031	3.09	0
4	8.609	277.10	1.401	3.60	0
5	8.068	277.44	1.276	4.43	0.1
6	7.487	277.78	1.446	4.63	0.1
7	7.943	277.42	1.589	4.43	0.1
8	8.887	277.59	1.189	4.32	0.2
9	6.956	276.86	1.337	4.64	0.2
10	7.531	277.84	1.525	4.19	0.2
11	7.975	276.29	1.043	4.00	0.3
12	7.906	277.01	1.237	4.00	0.3
13	7.806	277.45	1.439	3.97	0.3

序号	压力/MPa	温度/K	流速/m·s^-1	含气率（体积分数）/%	黄原胶质量分数/%
1	8.078	278.2	0.952	4.48	0
2	6.044	278.2	1.024	3.01	0
3	6.031	277.29	1.031	3.09	0
4	8.609	277.10	1.401	3.60	0
5	8.068	277.44	1.276	4.43	0.1
6	7.487	277.78	1.446	4.63	0.1
7	7.943	277.42	1.589	4.43	0.1
8	8.887	277.59	1.189	4.32	0.2
9	6.956	276.86	1.337	4.64	0.2
10	7.531	277.84	1.525	4.19	0.2
11	7.975	276.29	1.043	4.00	0.3
12	7.906	277.01	1.237	4.00	0.3
13	7.806	277.45	1.439	3.97	0.3

[1]	SHENG Weiwu, CHENG Yongpan, CHEN Qiang, LI Xiaoting, WEI Jia, LI Linge, CHEN Xianfeng. Operating condition analysis of the microbubble and microdroplet dual-enhanced desulfurization reactor [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 142-147.
[2]	HUANG Yiping, LI Ting, ZHENG Longyun, QI Ao, CHEN Zhenglin, SHI Tianhao, ZHANG Xinyu, GUO Kai, HU Meng, NI Zeyu, LIU Hui, XIA Miao, ZHU Kai, LIU Chunjiang. Hydrodynamics and mass transfer characteristics of a three-stage internal loop airlift reactor [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 175-188.
[3]	YANG Hanyue, KONG Lingzhen, CHEN Jiaqing, SUN Huan, SONG Jiakai, WANG Sicheng, KONG Biao. Decarbonization performance of downflow tubular gas-liquid contactor of microbubble-type [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 197-204.
[4]	CHEN Kuangyin, LI Ruilan, TONG Yang, SHEN Jianhua. Structure design of gas diffusion layer in proton exchange membrane fuel cell [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 246-259.
[5]	SHAO Boshi, TAN Hongbo. Simulation on the enhancement of cryogenic removal of volatile organic compounds by sawtooth plate [J]. Chemical Industry and Engineering Progress, 2023, 42(S1): 84-93.
[6]	LI Dong, WANG Qianqian, ZHANG Liang, LI Jun, FU Qian, ZHU Xun, LIAO Qiang. Performance of series stack of non-aqueous nano slurry thermally regenerative flow batteries [J]. Chemical Industry and Engineering Progress, 2023, 42(8): 4238-4246.
[7]	LI Ruidong, HUANG Hui, TONG Guohu, WANG Yueshe. Hygroscopic properties and corrosion behavior of ammonium salt in a crude oil distillation column [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2809-2818.
[8]	ZHANG Kai, JIN Hanyu, LIU Siyu, WANG Shuai. Simulation of mass transfer process under the bubble interaction in bubbling fluidization [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2828-2835.
[9]	MA Zhejie, ZHANG Wenli, ZHAO Xuankai, LI Ping. Progress on the influence of oxygen mass transfer resistance in PEMFC cathode catalyst layer [J]. Chemical Industry and Engineering Progress, 2023, 42(6): 2860-2873.
[10]	CHEN Weiliang, GAO Xin, LI Hong, LI Xingang. Influence mechanism of skeleton structure of foamed SiC corrugated structured packing on the mass transfer performance [J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2289-2297.
[11]	LI Xue, WANG Yanjun, WANG Yuchao, TAO Shengyang. Recent advances in bionic surfaces for fog collection [J]. Chemical Industry and Engineering Progress, 2023, 42(5): 2486-2503.
[12]	TIAN Qikai, ZHENG Haiping, ZHANG Shaobin, ZHANG Jing, YU Ziyi. Advances in mixing enhanced microfluidic channels [J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1677-1687.
[13]	LIU Jia, LIANG Deqing, LI Junhui, LIN Decai, WU Siting, LU Fuqin. A review of flow assurance studies on hydrate slurry in oil-water system [J]. Chemical Industry and Engineering Progress, 2023, 42(4): 1739-1759.
[14]	SHANG Yu, XIAO Man, CUI Qiufang, TU Te, YAN Shuiping. Recovery characteristics of PVDF/BN-OH flat composite membrane for waste heat of hot stripped gas in CO₂ capture process [J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1618-1628.
[15]	WANG Wei, ZHANG Dongxu, LI Zunzhao, WANG Xiaolin, HUANG Qiyu. Research progress on the growth behavior of hydrates in water-in-oil emulsion systems [J]. Chemical Industry and Engineering Progress, 2023, 42(3): 1155-1166.