邓帅;胡高伟;卜庆涛;

• 1:中国地质科学院
• 2:青岛海洋地质研究所自然资源部天然气水合物重点实验室
• 3:海洋国家实验室海洋矿产资源评价与探测技术功能实验室

摘要(Abstract)：

掌握影响天然气水合物(简称水合物)在海底沉积物中形成的因素对其能源和气候环境效应的评估有重要的意义。水合物的含量与沉积物颗粒的粒径紧密相关,水合物多产出于粗砂中。以人工样品为主的实验研究表明,由于孔隙半径产生的毛细管抑制压力,多孔介质的颗粒越细,孔隙越小,一定条件下稳定温度越低(或压力越高)。沉积物颗粒的比表面积与水合物饱和度呈现很高的相关性,比粒径更有优势。利用比表面积可以定量地表示粒径和孔隙大小之间的关系,量化分析孔隙大小对水合物形成的影响。此外,我国南海神狐海域水合物尽管赋存在细粒沉积物中,却具有较高的饱和度,这可能与南海沉积物中富含丰富的有孔虫壳体有关,通过微观层面的观察发现,这些古生物壳体不仅充当了沉积物中的粗砂部分,而且其多孔结构也使沉积孔隙空间增加,从而为水合物富集提供了有利的生长环境和便利的赋存空间。Klauda等的模型假定多孔介质孔径尺寸的概率密度分布函数为正态分布,新的相平衡模型包含了尺寸效应。颜荣涛等把有效孔隙半径和水合物饱和度联系起来,从而将水合物饱和度引入相平衡模型中。分形模型将分形参数与孔隙度建立了关系,但并没有与温压条件等进一步联系起来,对水合物形成和分解的影响还需做进一步的推导和实验。

关键词(KeyWords)： 水合物;粒径;比表面积;有孔虫;孔径分布

Abstract:

Keywords:

基金项目(Foundation): 国家重点研发计划(2017YFC0307600);; 国家自然科学基金项目(41474119);; 中国地质调查局项目(DD20160219)

作者(Author): 邓帅;胡高伟;卜庆涛;

Email:

DOI:

参考文献(References)：

• [1] Wang J S,Gao Y Y,Li Q,et al.Grain size constraint on gas hydrate occurrence:Evidence from sediment size during IODP 311 (in Chinese)[J].Adv.Earth.Sci.,2007,22:659-665.
• [2] Lu H,Kawasaki T,Ukita T,et al.Particle size effect on the saturation of methane hydrate in sediments:Constrained from experimental results[J/OL].Mar.Petrol.Geol.,2011,28:1801-1805.
• [3] Uchida T,Takeya S,Chuvilin E M,et al.Decomposition of methane hydrates in sand,sandstone,clays,and glass beads[J/OL].J.Geophys.Res.,2004,109:B05206.doi:10.102912003 jb002771.
• [4] Bahk J J,Kim D H,Chun J H,et al.Gas hydrate occurrences and their relation to host sediment properties:Results from second Ulleung Basin gas hydrate drilling expedition,East Sea[J].Mar.Petrol.Geol.,2013,47:21-29.
• [5] Lee J Y,Kim G Y,Kang N K,et al.Physical properties of sediments from the Ulleung Basin,East Sea:Results from second Ulleung Basin gas hydrate drilling expedition,East Sea (Korea)[J].Mar.Petrol.Geol.,2013,47:43-55.
• [6] Behseresht J,Bryant S L.Sedimentological control on saturation distribution in Arctic gas-hydrate-bearing sands[J].Earth Planet.Sci.Lett.,2012,341/344:114-127.
• [7] Dallimore S R,Collett T S.Intrapermafrost gas hydrates from a deep core-hole in the Mackenzie delta,northwest-territories[J].Canada.Geology,1995,23:527-530.
• [8] Boswell R,Collett T S,Frye M,et al.Subsurface gas hydrates in the northern gulf of Mexico[J].Mar.Petrol.Geol.,2012,34:4-30.
• [9] 刘昌岭,业渝光,孙始财,等.不同体系下天然气水合物P-T稳定条件及其影响因素的实验研究[J].中国科学:地球科学,2013,43(3):406-413.
• [10] 张辉,卢海龙,梁金强,等.南海北部神狐海域沉积物颗粒对天然气水合物聚集的主要影响[J].中国科学:地球科学,2016,61(3):388-397.
• [11] Wang H B,Yang S X,Wu N Y,et al.Controlling factors for gas hydrate occurrence in Shenhu area on the northern slope of the South China Sea[J].Sci.China:Earth Sci.,2013,56:513-520.
• [12] 陈芳,苏新,周洋,等.南海北部陆坡神狐海域晚中新世以来沉积物中生物组分变化及意义[J].海洋地质与第四纪地质,2009,29(2):1-8.
• [13] 陈芳,苏新,陆红锋,等.南海神狐海域有孔虫与高饱和度水合物的储存关系[J].地球科学:中国地质大学学报,2013,38(5):907-915.
• [14] 李承峰,胡高伟,张巍,等.有孔虫对南海神狐海域细粒沉积层中天然气水合物形成及赋存特征的影响[J].中国科学:地球科学,2016,46(9):1223-1230.
• [15] Trehu A M,Long P E,Torres M E,et al.Three-dimensional distribution of gas hydrate beneath southern hydrate ridge:Constraints from ODP Leg 204[J].Earth.Planet.Sci.Lett.,2004,222:845-862.
• [16] Handa Y P,Stupin D.Thermodynamic properties and dissociation characteristics of methane and propane hydrates in 70-? radius silica gelpores[J].J.Phys.Chem.,1992,96:8599-8603.
• [17] Ye Y G,Liu C L,Liu S Q,et al.Experimental studies on several significant problems related marine gas hydrate[J].High Tech.Lett.,2004,10(Suppl):352-359.
• [18] Smith D H,Wilder J W,Seshadri J,et al.Methane hydrate equilibria in silica gels with broad pore size distributions[J].Aiche Journal,2002,48:393-400.
• [19] Smith D H,Wilder J W,Seshadri K,et al.Thermodynamics of carbon dioxide hydrate formation in media with broad pore-size distributions[J].Environ.Sci .Technol.,2002,36:5192-5198.
• [20] Smith D H,Wilder J W,Seshadri K,et al.Equilibrium pressures and temperatures for equibria involving SI and SⅡ hydrate and free gas inporous media[C]//Proceedings of the fourth international conference on gas hydrates,Yokohama :[s.n.],2002:295-299.
• [21] Lu H L,Matsumoto R.Preliminary experimental results of the stable P-T conditions of methane hydrate in a nannofossil-rich claystonecolumn[J].Geochem.,2002,36:21-30.
• [22] Turner D,Sloan E D.Hydrate phase equilibrium measurements and predictions in sediments[C]//Proceedings of the Fourth International Conference on Gas Hydrates.Yokohama:[s.n.],2002:327-330.
• [23] 李明川,樊栓狮,赵金洲,等.多孔介质对天然气水合物形成的影响[J].石油物探,2007,46(1):13-15.
• [24] Sun R,Duan Z.An accurate model to predict the thermodynamic stability of methane hydrate and methane solubility in marine environments[J].Chem.Geol.,2007,244:248-262.
• [25] Anderson R,Tohidi B,Webber J B W,et al.Gas hydrate growth and dissociation in narrow pore networks:Capillary inhibition and hysteresis phenomena[J].Geol.Soc.London,Spec.Publ.,2009,319:145-159.
• [26] Bahk J J,Um I K,Holland M,et al.Core lithologies and their constraints on gas-hydrate occurrence in the East Sea,offshore Korea:Results from the site UBGH1-9[J].Mar.Petrol.Geol.,2011,28:1943-1952.
• [27] Klauda J B,Stanley I S.modelling gas hydrate equilibria in laboratory and natural porous media[J].Ind.Eng.Chem.Res.,2001,40:4197-4208.
• [28] Klauda J B,Stanley I S.Predictions of gas hydrate phase equilibria and amounts in natural sediment porous media[J].Mar.Petrol.Geol.,2003,20:459-470.
• [29] Dewhurst D N,Aplin A C,Sarda,J P,et al.Influence of clay fraction on pore-scale properties and hydraulic conductivity of experimentally compacted mudstones[J].Geophys.Res.Solid Earth 1999,104:29261.
• [30] 李金平,梁德青,郭开华,等,多孔介质中气体水合物相平衡研究进展[J].石油与天然气化工,2004,33(5):315-319.
• [31] 颜荣涛,魏厚振,吴二林,等.一个考虑沉积物孔径分布特征的水合物相平衡模型[J].物理化学学报,2011,27(2):295-301.
• [32] 颜荣涛,牟春梅,张芹,等,考虑沉积物孔隙毛细效应影响的宏观相平衡模型[J/OL].中国科学:物理学,力学,天文学,2019,9(3):doi:10.3866/PKU.WHXB20110204.
• [33] Sheng Z,Xie S Q,Pan C Y,et al.Probability and mathematical statistics[M].Beijing:Higher Education Press;2001:315-319.
• [34] Seshadri K,Wilder J W,Smith D H,et al.Measurements of equilibrium pressures and temperatures for propane hydrate in silica gel with different pore size distributions[J].Phys.Chem.,2001,105:2627-2631.
• [35] 杨建,陈家军,杨周喜,等.松散砂粒孔隙结构、孔隙分形特征及渗透率研究[J].水文地质工程地质,2008,35(3):93-97.
• [36] Uchida T,Takeya S,Chuvilin E M,et al.Decomposition of methane hydrates in sand,sandstone,clays,and glass beads[J].J.Geophys Res.,2004,109:B05206.doi:10.102912003jb002771.
• [37] Torres M E,Trehu A M,Cespedes N,et al.Methane hydrate formation in turbidite sediments of northern Cascadia,IODP expedition 311[J].Earth Planet.Sci.Lett.,2008,271:170-180.