含粉砂盐水体系甲烷水合物生成与固相沉积规律研究

doi:10.11949/0438-1157.20231297

化工学报

• •

含粉砂盐水体系甲烷水合物生成与固相沉积规律研究

刘礼豪¹(), 黄婷², 雍宇³, 罗昕浩¹, 赵泽明¹, 宋尚飞¹(), 史博会¹, 陈光进¹, 宫敬¹

^1.中国石油大学（北京）机械与储运工程学院，油气管道输送安全国家工程研究中心，城市燃气输配技术北京市重点实验室，石油工程教育部重点实验室，北京 102249
^2.中海油研究总院有限责任公司水合物和海洋资源战略研究中心，北京 100028
^3.国家管网西南管道公司，四川成都 610095

收稿日期:2023-12-05 修回日期:2024-03-28 出版日期:2024-03-29
通讯作者: 宋尚飞
作者简介:刘礼豪（1997—），男，博士研究生， liuliao72@163.com
基金资助:
国家自然科学基金项目(52104069);北京市自然科学基金项目(3232030);国家重点研发计划项目(2022YFC2806200);中国博士后科学基金项目(2022M713460);中国石油大学科学基金项目(2462023BJRC018)

Study on CH₄-hydrate formation and solid-phase deposition in salt-sand coexisting flow systems

Lihao LIU¹(), Ting HUANG², Yu YONG³, Xinhao LUO¹, Zeming ZHAO¹, Shangfei SONG¹(), Bohui SHI¹, Guangjin CHEN¹, Jing GONG¹

^1.National Engineering Research Center of Oil and Gas Pipeline Transportation Safety, Beijing Key Laboratory of Urban Oil and Gas Distribution Technology, MOE Key Laboratory of Petroleum Engineering, College of Mechanical and Transportation Engineering, China University of Petroleum-Beijing, Beijing 102249, China
^2.Gas Hydrate and Marine Resources Strategic Research Center, CNOOC Research Institute Company Limited, Beijing 100028, China
^3.Pipe China Southwest Pipeline Company, Chengdu 610095, Sichuan, China

Received:2023-12-05 Revised:2024-03-28 Online:2024-03-29
Contact: Shangfei SONG

摘要/Abstract

摘要：

管道中水合物再生与粉砂沉积堵塞是影响可燃冰开采的关键问题，且管道中海水具有一定矿化度，因此，本研究利用高压环路开展了水-粉砂-NaCl-CH₄体系水合物生成与水合物-粉砂沉积实验。实验揭示了水合物生成到稳定固相沉积的四阶段演变过程。研究发现，在含有粉砂的盐水体系中，甲烷水合物的诱导期相较于纯水体系可显著延长2-3倍。特别是在低含砂浓度（0.1wt%）和高流量（1600kg/h）的条件下，诱导期延长至3.3倍。分析认为NaCl和粉砂对水分子簇结构的扰乱是抑制水合物成核的关键机理。此外，NaCl通过压缩颗粒双电层厚度，削弱砂粒亲水性，通过纳米气泡桥接促使固相颗粒聚集并黏附于管壁，加速水合物-砂沉积层的形成。研究成果有助于保障可燃冰开发排采系统中多相流动的安全与稳定。

关键词: 甲烷水合物, 诱导期, 沉积, 流动保障, 可燃冰

Abstract:

The reformation of hydrates and the blockage caused by hydrate-sand deposition in pipelines are critical issues affecting the exploitation of methane hydrate. Given that the seawater in the pipelines possesses a certain degree of salinity, this study conducted experiments on the formation of hydrates and the deposition of hydrate-silt aggregates in the water-sand-NaCl-CH4 system using a high-pressure loop. The experiments revealed a four-stage evolution process from hydrate formation to stable solid-phase deposition. The study found that in a saline system containing sand, the induction time of hydrate formation can be significantly extended by 2-3 times compared to that in a pure water system. This extension is particularly notable under conditions of low sand concentration (0.1wt%) and high flow rate (1600kg/h), reaching a maximum of 3.3 times. Analysis suggests that the disruption of water molecule cluster structures by NaCl and sand is a crucial mechanism inhibiting hydrate nucleation. Furthermore, NaCl compresses the thickness of the particle's double electric layer, weakening the hydrophilicity of sand particles. This, coupled with nanobubble bridging, prompts the aggregation of solid particles and their adhesion to the pipe wall, accelerating the formation of hydrate-sand deposition layers. The research findings contribute to ensuring the safety and stability of multiphase flow in the exploitation and production system for combustible ice development.

Key words: methane hydrate, induction time, deposition, flow assurance, combustible ice

中图分类号:

TE 832

刘礼豪, 黄婷, 雍宇, 罗昕浩, 赵泽明, 宋尚飞, 史博会, 陈光进, 宫敬. 含粉砂盐水体系甲烷水合物生成与固相沉积规律研究[J]. 化工学报, DOI: 10.11949/0438-1157.20231297.

Lihao LIU, Ting HUANG, Yu YONG, Xinhao LUO, Zeming ZHAO, Shangfei SONG, Bohui SHI, Guangjin CHEN, Jing GONG. Study on CH₄-hydrate formation and solid-phase deposition in salt-sand coexisting flow systems[J]. CIESC Journal, DOI: 10.11949/0438-1157.20231297.

图/表 18

图 1 高压水合物实验环道示意图[34]

Fig.1 Schematic diagram of the high-pressure flow loop apparatus

图 2 微米级模拟砂粒的扫描电镜图（a-c）以及接触角测量结果（d）[34]

Fig.2 SEM images (a-c) and contact angle (d) measurement of the micron-sized simulated sand particles

表 1 实验条件汇总

Table 1 Summary of Experimental Conditions

实验编号	流量/kg/h	粉砂浓度/wt%	盐浓度/wt%	压力/MPa
SY1	1160	0	0	5.15
SY2	1160	0.1	3	5.15
SY 3	1160	0.5	3	5.15
SY 4	1160	1.5	3	5.15
SY 5	1160	0.1	3	6.45
SY 6	1160	0.5	3	6.45
SY 7	1160	1.5	3	6.45
SY 8	1600	0	0	5.15
SY 9	1600	0.1	0	5.15
SY 10	1600	0	3	5.15
SY 11	1600	0.1	3	5.15
SY 12	1600	0.5	3	5.15
SY 13	1600	1.5	3	5.15

图 3 水合物浆液流动沉积规律

Fig.3 Hydrate slurry flow to deposition process

图 4 阶段I中管内流动情况注:(a) 00:00:31时刻图像;(b) 01:00:05时刻图像

Fig.4 Flow in stage I(a) 00:00:31 moment image; (b) 01:00:05 moment image

图 5 阶段II中管内流动情况注:(a) 01:07:00时刻图像;(b) 01:48:25时刻图像;(c) 02:15:45时刻图像;(d) 02:44:48时刻图像

Fig.5 Flow in stage II(a) 01:07:00 moment image; (b) 01:48:25 moment image; (c) 02:15:45 moment image; (d) image at 02:44:48

图 6 阶段III中管内流动情况注:(a) 02:49:47时刻图像;(b) 03:45:27时刻图像;(c) 04:08:11时刻图像;(d) 04:46:27

Fig. 6 Flow in stage III(a) image at 02:49:47; (b) image at 03:45:27; (c) image at 04:08:11; (d) image at 04:46:27

图 7 阶段IV中管内流动情况注:(a) 05:08:49时刻图像;(b) 05:25:34时刻图像;(c) 05:47:25时刻图像

Fig. 7 Flow in stage IV(a) 05:08:49 moment image; (b) 05:25:34 moment image; (c) 05:47:25 moment image

表 2 相同初始压力与流量下不同体系水合物诱导期结果

Table 2 Average values of hydrate induction time in the flow systems with different conditions

实验编号	体系	诱导期/min
SY8-1	纯水	10.8
SY8-2		17.4
SY8-3		18.6
平均诱导期		15.4±3.2
SY9-1	0.1 wt%粉砂	21.00
SY9-2		21.60
SY9-3		22.80
平均诱导期		21.8±0.67
SY10-1	3 wt% NaCl	31.8
SY10-2		19.8
SY10-3		25.2
平均诱导期		25.6±4.13
SY11-1	3 wt% NaCl+0.1 wt % 粉砂	67.2
SY11-2		39
SY11-3		46.8
平均诱导期		51±10.8

图 8 纯砂/NaCl-砂体系与水分子作用机理

Fig.8 Mechanism of Interaction between pure sand/NaCl-sand system and water molecules

图 9 不同体系中水合物生成温度、压力点

Fig.9 Hydrate formation temperature and pressure point in different systems

图 10 5.15MPa,-2℃条件下不同体系诱导期

Fig.10 Hydrate induction time of different systems at 5.15MPa,-2°C(1600kg/h)

图 11 低流量条件下含粉砂浓度对于水合物诱导期的影响（1160 kg/h，实验SY2-SY7）

Fig.11 Effect of sand concentration on hydrate induction time under low flow conditions(1160 kg/h, SY2-SY7)

图 12 不同含粉砂浓度条件水合物诱导期

Fig.12 Hydrate induction time for different sand concentration conditions

图 13 不同流量条件下不同含粉砂浓度对于诱导期的影响

Fig.13 Effect of different sand concentrations on induction time under different flow conditions

图 14 各体系流动沉积过程阶段对比（流量1160 kg/h）

Fig. 14 Comparison of flow deposition process of each system

图 15 盐-砂体系中水合物颗粒吸附聚并过程

Fig. 15 Schematic diagram of inter-particle adsorption and aggregation

图 16 颗粒间吸附聚并示意图

Fig. 16 Adsorption and aggregation of hydrate particles in the salt-sand system.

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含粉砂盐水体系甲烷水合物生成与固相沉积规律研究

Study on CH₄-hydrate formation and solid-phase deposition in salt-sand coexisting flow systems

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含粉砂盐水体系甲烷水合物生成与固相沉积规律研究

Study on CH4-hydrate formation and solid-phase deposition in salt-sand coexisting flow systems

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Study on CH₄-hydrate formation and solid-phase deposition in salt-sand coexisting flow systems