盐度影响下松散沉积物中甲烷水合物生成特征研究

纪云开, 王佳贤, 邱晓倩, 孟庆国, 张永超, 胡高伟, 蔡峰, 刘昌岭. 盐度影响下松散沉积物中甲烷水合物生成特征研究[J]. 海洋地质与第四纪地质, 2024, 44(6): 71-81. doi: 10.16562/j.cnki.0256-1492.2024090901
引用本文: 纪云开, 王佳贤, 邱晓倩, 孟庆国, 张永超, 胡高伟, 蔡峰, 刘昌岭. 盐度影响下松散沉积物中甲烷水合物生成特征研究[J]. 海洋地质与第四纪地质, 2024, 44(6): 71-81. doi: 10.16562/j.cnki.0256-1492.2024090901
JI Yunkai, WANG Jiaxian, QIU Xiaoqian, MENG Qingguo, ZHANG Yongchao, HU Gaowei, CAI Feng, LIU Changling. Effect of salinity on the formation of methane hydrate in unconsolidated sediments[J]. Marine Geology & Quaternary Geology, 2024, 44(6): 71-81. doi: 10.16562/j.cnki.0256-1492.2024090901
Citation: JI Yunkai, WANG Jiaxian, QIU Xiaoqian, MENG Qingguo, ZHANG Yongchao, HU Gaowei, CAI Feng, LIU Changling. Effect of salinity on the formation of methane hydrate in unconsolidated sediments[J]. Marine Geology & Quaternary Geology, 2024, 44(6): 71-81. doi: 10.16562/j.cnki.0256-1492.2024090901

盐度影响下松散沉积物中甲烷水合物生成特征研究

  • 基金项目: 国家自然科学基金“南海北部高富集天然气水合物储层特征与成藏控制机理研究”(U2244224),“南海神狐海域水合物储层气-水-水合物三相共存微观机理研究”(42206233),“海洋沉积物中水合物生成过程的孔隙水转化规律及其控制机理研究”(42176212);泰山学者工程项目(tsqn202312280)
详细信息
    作者简介: 纪云开(1990—),男,博士,副研究员,主要从事多孔介质水合物相变与多相渗流研究,E-mail:jiyunkai@yeah.net
    通讯作者: 刘昌岭(1966—),男,博士,研究员,主要从事天然气水合物模拟实验研究,E-mail:qdliuchangling@163.com
  • 中图分类号: P774.4

Effect of salinity on the formation of methane hydrate in unconsolidated sediments

More Information
  • 深入认识含盐水松散沉积物体系中甲烷水合物生成特征,对精准评价海域天然气水合物资源量有重要意义。本研究利用低场核磁共振原位探测技术研究了盐度对松散砂样中甲烷水合物生成特征的影响。结果表明,松散砂样体系下不同大小孔隙中水合物生成诱导时间存在差异;甲烷水合物更易在小孔隙中生成。随着孔隙水盐度增大,水合物生成诱导时间呈现指数增长。在最初20 min内,随着孔隙水盐度的增大,水合物生成速率先升后降,在盐度为3.0 wt%条件下生成速率最大。在松散砂样体系下的不同位置处,甲烷水合物生成诱导时间的差异性以及孔隙水通过水合物膜的方式转变会引起水合物生成过程中生成速率的变化。沉积物表面影响和水合物的阻隔作用使砂样中部分孔隙水不能转化为水合物,而孔隙水盐度的增加促使这种作用增强,孔隙水最终转化率降低,水合物饱和度减小。

  • 加载中
  • 图 1  水合物专用低场核磁共振测试装置照片

    Figure 1. 

    图 2  水合物专用低场核磁共振测试装置示意图

    Figure 2. 

    图 3  含水量与T2分布信号总强度之间的关系

    Figure 3. 

    图 4  甲烷水合物生成过程中T2分布变化图(实验4)

    Figure 4. 

    图 5  甲烷水合物生成过程中T2minT2max变化(实验4)

    Figure 5. 

    图 6  不同初始孔隙水盐度下砂样中甲烷水合物生成过程中的水合物饱和度变化曲线

    Figure 6. 

    图 7  不同孔隙水初始盐度条件下甲烷水合物生成诱导时间变化图

    Figure 7. 

    图 8  不同孔隙水初始盐度下砂样中甲烷水合物生成过程的水合物生成速率变化曲线

    Figure 8. 

    图 9  不同初始孔隙水盐度条件下孔隙水最终转化率与孔隙水最终盐度变化

    Figure 9. 

    图 10  不同孔隙水初始盐度条件下甲烷水合物生成过程的孔隙水盐度变化曲线

    Figure 10. 

    表 1  砂样的主要参数

    Table 1.  Major parameters of sand samples

    编号 粒径/μm 表观体积/cm3 初始含水量/g 初始含水饱和度/% 孔隙度/% 盐度/wt%
    1 100~200 42.41 9.51 49.88 44.97 0.0
    2 100~200 42.41 9.40 49.40 44.86 1.5
    3 100~200 42.41 9.22 48.62 44.71 3.0
    4 100~200 42.41 9.37 49.23 44.87 4.5
    下载: 导出CSV
  • [1]

    刘昌岭, 张永超, 纪云开, 等. 天然气水合物微观测试技术与应用进展[J]. 海洋地质与第四纪地质, 2024, 44(3):136-148

    LIU Changling, ZHANG Yongchao, JI Yunkai, et al. Advances in microscopic testing techniques and applications for natural gas hydrates[J]. Marine Geology & Quaternary Geology, 2024, 44(3):136-148.]

    [2]

    吴能友, 李彦龙, 刘乐乐, 等. 海洋天然气水合物储层蠕变行为的主控因素与研究展望[J]. 海洋地质与第四纪地质, 2021, 41(5):3-11

    WU Nengyou, LI Yanlong, LIU Lele, et al. Controlling factors and research prospect on creeping behaviors of marine natural gas hydrate-bearing-strata[J]. Marine Geology & Quaternary Geology, 2021, 41(5):3-11.]

    [3]

    Sloan E D Jr. Clathrate Hydrates of Natural Gases[M]. New York: Marcel Dekker, Inc. , 1990.

    [4]

    刘乐乐, 万义钊, 李承峰, 等. 天然气水合物储层有效绝对渗透率现场测试进展[J]. 海洋地质前沿, 2022, 38(11):40-55

    LIU Lele, WAN Yizhao, LI Chengfeng, et al. Advances in field testing of the effective absolute permeability of gas hydrate reservoirs[J]. Marine Geology Frontiers, 2022, 38(11):40-55.]

    [5]

    Zhan L, Wang Y, Li X S. Experimental study on characteristics of methane hydrate formation and dissociation in porous medium with different particle sizes using depressurization[J]. Fuel, 2018, 230:37-44. doi: 10.1016/j.fuel.2018.05.008

    [6]

    卢静生, 熊友明, 李栋梁, 等. 非成岩水合物储层降压开采过程中出砂和沉降实验研究[J]. 海洋地质与第四纪地质, 2019, 39(4):183-195

    LU Jingsheng, XIONG Youming, LI Dongliang, et al. Experimental study on sand production and seabottom subsidence of non-diagenetic hydrate reservoirs in depre-ssurization production[J]. Marine Geology & Quaternary Geology, 2019, 39(4):183-195.]

    [7]

    张永超, 刘昌岭, 刘乐乐, 等. 水合物生成导致沉积物孔隙结构和渗透率变化的低场核磁共振观测[J]. 海洋地质与第四纪地质, 2021, 41(3):193-202

    ZHANG Yongchao, LIU Changling, LIU Lele, et al. Sediment pore-structure and permeability variation induced by hydrate formation: evidence from low field nuclear magnetic resonance observation[J]. Marine Geology & Quaternary Geology, 2021, 41(3):193-202.]

    [8]

    Makogon Y F, Holditch S A, Makogon T Y. Natural gas-hydrates: a potential energy source for the 21st Century[J]. Journal of Petroleum Science and Engineering, 2007, 56(1-3):14-31. doi: 10.1016/j.petrol.2005.10.009

    [9]

    黄伟, 张伟, 梁金强, 等. 尖峰北盆地含气流体运聚疏导组合特征及对水合物成藏的控制作用[J]. 海洋地质与第四纪地质, 2020, 40(4):148-161

    HUANG Wei, ZHANG Wei, LIANG Jinqiang, et al. Characteristics of gas-bearing fluid migration and accumulation system and their control on gas hydrate accumulation in the Jianfengbei Basin of South China Sea[J]. Marine Geology & Quaternary Geology, 2020, 40(4):148-161.]

    [10]

    Zhang X M, Liu Q Q, He J J, et al. Research progress of incremental synthesis and enhancement mechanism of natural gas hydrates: a review[J]. Renewable and Sustainable Energy Reviews, 2024, 202:114695. doi: 10.1016/j.rser.2024.114695

    [11]

    Nguyen N N, Nguyen A V. Recent insights into the anomalous dual nature (both promotion and Inhibition) of chemical additives on gas hydrate formation[J]. Chemical Engineering Journal, 2023, 475:146362. doi: 10.1016/j.cej.2023.146362

    [12]

    Sun R H, Yang M J, Song Y C. Effect of NaCl concentration on depressurization-induced methane hydrate dissociation near ice-freezing point: associated with metastable phases[J]. Journal of Natural Gas Science and Engineering, 2021, 96:104304. doi: 10.1016/j.jngse.2021.104304

    [13]

    王英梅, 刘生浩, 滕亚栋, 等. NaCl浓度对CO2水合物形成与稳定性的影响[J]. 化工进展, 2023, 42(11):6093-6101

    WANG Yingmei, LIU Shenghao, TENG Yadong, et al. Effect of NaCl concentration on the formation and stability of CO2 hydrate[J]. Chemical Industry and Engineering Progress, 2023, 42(11):6093-6101.]

    [14]

    Dholabhai P D, Kalogerakis N, Bishnoi P R. Kinetics of methane hydrate formation in aqueous electrolyte solutions[J]. The Canadian Journal of Chemical Engineering, 1993, 71(1):68-74. doi: 10.1002/cjce.5450710110

    [15]

    Mekala P, Babu P, Sangwai J S, et al. Formation and dissociation kinetics of methane hydrates in seawater and silica sand[J]. Energy & Fuels, 2014, 28(4):2708-2716.

    [16]

    Chong Z R, Chan A H M, Babu P, et al. Effect of NaCl on methane hydrate formation and dissociation in porous media[J]. Journal of Natural Gas Science and Engineering, 2015, 27:178-189. doi: 10.1016/j.jngse.2015.08.055

    [17]

    Wang J L, Sun J S, Wang R, et al. Mechanisms of synergistic inhibition of NaCl and glycine mixtures on methane hydrate formation: experimental and molecular dynamic simulation[J]. Gas Science and Engineering, 2023, 110:204880. doi: 10.1016/j.jgsce.2023.204880

    [18]

    Gao Q, Zhao J Z, Yin Z Y, et al. Experimental study on methane hydrate formation in quartz sand under tri-axial condition[J]. Journal of Natural Gas Science and Engineering, 2021, 85:103707. doi: 10.1016/j.jngse.2020.103707

    [19]

    Mok J, Choi W, Kim S, et al. NaCl-induced enhancement of thermodynamic and kinetic CO2 selectivity in CO2+N2 hydrate formation and its significance for CO2 sequestration[J]. Chemical Engineering Journal, 2023, 451:138633. doi: 10.1016/j.cej.2022.138633

    [20]

    Sun X, Liu D J, Chang D C, et al. Analysis of natural gas hydrate formation in sodium dodecyl sulfate and quartz sand complex system under saline environment[J]. Petroleum Science and Technology, 2018, 36(14):1073-1079. doi: 10.1080/10916466.2018.1460613

    [21]

    张金锋. 甲烷水合物在不同体系中的生成动力学研究[D]. 浙江工业大学硕士学位论文, 2003

    ZHANG Jinfeng. Research on the kinetics of methane hydrate formation in various systems[D]. Master Dissertation of Zhejiang University of Technology, 2003.]

    [22]

    Nguyen N N, Nguyen A V. The dual effect of sodium halides on the formation of methane gas hydrate[J]. Fuel, 2015, 156:87-95. doi: 10.1016/j.fuel.2015.04.022

    [23]

    Xu J F, Du S, Hao Y C, et al. Molecular simulation study of methane hydrate formation mechanism in NaCl solutions with different concentrations[J]. Chemical Physics, 2021, 551:111323. doi: 10.1016/j.chemphys.2021.111323

    [24]

    Ji Y K, Hou J, Cui G D, et al. Experimental study on methane hydrate formation in a partially saturated sandstone using low-field NMR technique[J]. Fuel, 2019, 251:82-90. doi: 10.1016/j.fuel.2019.04.021

    [25]

    展静, 张鹏, 王英梅, 等. 多孔介质水合物中未水合水的核磁共振实验研究[J]. 中南大学学报: 自然科学版, 2022, 53(4):1525-1535

    ZHAN Jing, ZHANG Peng, WANG Yingmei, et al. NMR study of unhydrated water in hydrate of porous media[J]. Journal of Central South University: Science and Technology, 2022, 53(4):1525-1535.]

    [26]

    Wang J X, Ji Y K, Liu C L, et al. Pore water conversion characteristics during methane hydrate formation: insights from low-field nuclear magnetic resonance (NMR) measurements[J]. Journal of Marine Science and Engineering, 2024, 12(4):619. doi: 10.3390/jmse12040619

    [27]

    Ji Y K, Liu C L, Zhang Z, et al. Experimental study on characteristics of pore water conversion during methane hydrates formation in unsaturated sand[J]. China Geology, 2022, 5(2):276-284.

    [28]

    Ren J J, Yin Z Y, Li Q P, et al. Pore-scale investigation of CH4 hydrate kinetics in clayey-silty sediments by low-field NMR[J]. Energy & Fuels, 2022, 36(24):14874-14887.

    [29]

    Ge X M, Liu J Y, Fan Y R, et al. Laboratory investigation into the formation and dissociation process of gas hydrate by low-field NMR technique[J]. Journal of Geophysical Research: Solid Earth, 2018, 123(5):3339-3346. doi: 10.1029/2017JB014705

    [30]

    Liu Z, Chen L T, Wang Z Y, et al. Hydrate phase equilibria in natural sediments: inhibition mechanism and NMR-based prediction method[J]. Chemical Engineering Journal, 2023, 452:139447. doi: 10.1016/j.cej.2022.139447

    [31]

    Zhao Y C, Li M, Dong S, et al. Fractal analysis on CO2 hydrate-bearing sands during formation and dissociation processes with NMR[J]. Science of the Total Environment, 2023, 859:160326. doi: 10.1016/j.scitotenv.2022.160326

    [32]

    Coates G R, Xiao L Z, Prammer M G. NMR Logging: Principles and Applications[M]. Houston: Halliburton Energy Services, 1999.

    [33]

    Kleinberg R L, Flaum C, Griffin D D, et al. Deep sea NMR: methane hydrate growth habit in porous media and its relationship to hydraulic permeability, deposit accumulation, and submarine slope stability[J]. Journal of Geophysical Research: Solid Earth, 2003, 108(B10):2508.

    [34]

    Wu X Z, Guo G Q, Ye H Y, et al. Application of dual horizontal well systems in the Shenhu area of the South China Sea: analysis of productivity improvement[J]. Journal of Marine Science and Engineering, 2023, 11(7):1443. doi: 10.3390/jmse11071443

    [35]

    Wu Z R, Gu Q K, Li G J, et al. Effect of decomposition water content of natural gas hydrate on permeability and gas production of clay sediments based on numerical simulation[J]. Journal of Natural Gas Science and Engineering, 2022, 108:104826. doi: 10.1016/j.jngse.2022.104826

    [36]

    刘庭崧, 刘妮, 陈利涛, 等. CH4水合物生长速率影响因素的分子动力学模拟[J]. 原子与分子物理学报, 2020, 37(5):778-782

    LIU Tingsong, LIU Ni, CHEN Litao, et al. Molecular dynamics simulation of factors affecting the growth rate of CH4 hydrate[J]. Journal of Atomic and Molecular Physics, 2020, 37(5):778-782.]

    [37]

    Liu L H, Liu S Y, Peng H L, et al. Surface charge of mesoporous calcium silicate and its adsorption characteristics for heavy metal ions[J]. Solid State Sciences, 2020, 99:106072. doi: 10.1016/j.solidstatesciences.2019.106072

    [38]

    Gupta R, Deo Pathak D. Surface functionalization of mesoporous silica with maltodextrin for efficient adsorption of selective heavy metal ions from aqueous solution[J]. Colloids and Surfaces A: Physicochemical and Engineering Aspects, 2021, 631:127695. doi: 10.1016/j.colsurfa.2021.127695

    [39]

    Guo Y, Xiao W, Pu W F, et al. CH4 nanobubbles on the hydrophobic solid–water interface serving as the nucleation sites of methane hydrate[J]. Langmuir, 2018, 34(34):10181-10186. doi: 10.1021/acs.langmuir.8b01900

    [40]

    Liu F P, Li A R, Wang C, et al. Kinetic analysis of CO2 hydrate formation in the aqueous solutions of transition metal chlorides[J]. Greenhouse Gases: Science and Technology, 2024, 14(2):284-294. doi: 10.1002/ghg.2264

    [41]

    Liang H Y, Guan D W, Yang L, et al. Multi-scale characterization of shell thickness and effective volume fraction during gas hydrates formation: a kinetic study[J]. Chemical Engineering Journal, 2021, 424:130360. doi: 10.1016/j.cej.2021.130360

    [42]

    Rouquerol J, Rodríguez-Reinoso F, Sing K S W, et al. Characterization of Porous Solids III[M]. Amsterdam: Elsevier, 1994.

    [43]

    Handa Y P, Stupin D Y. Thermodynamic properties and dissociation characteristics of methane and propane hydrates in 70 -Å-radius silica gel pores[J]. The Journal of Physical Chemistry, 1992, 96(21):8599-8603. doi: 10.1021/j100200a071

    [44]

    Moridis G J. Numerical studies of gas production from methane hydrates[J]. SPE Journal, 2003, 8(4):359-370. doi: 10.2118/87330-PA

  • 加载中

(10)

(1)

计量
  • 文章访问数:  465
  • PDF下载数:  81
  • 施引文献:  0
出版历程
收稿日期:  2024-09-09
修回日期:  2024-10-13
刊出日期:  2024-12-28

目录