收稿日期: 2015-04-07
修回日期: 2015-05-22
网络出版日期: 2015-08-10
基金资助
国家重点基础研究发展计划("973”)项目课题(编号：2012CB214705)；国家自然科学基金项目(编号：41372163；41172145)；2014年度山西省煤基重点科技攻关项目(编号：MQ2014-01；MQ2014-12)；山西省煤层气联合研究基金资助项目(编号：2014012001)；湖北省自然科学基金面上项目(编号：2014CFB169)联合资助.
Experimental Analysis of Methane Adsorption-diffusion Property in High-maturity Organic-rich Shale and High-Rank Coal
Received date: 2015-04-07
Revised date: 2015-05-22
Online published: 2015-08-10
煤/页岩中甲烷的吸附—扩散性能是煤层气/页岩气资源评价的关键参数之一。通过对晋城矿区寺河井田二叠系山西组3号煤层样和华南古生界下志留统龙马溪组页岩样进行低温液氮和甲烷等温吸附实验，剖析了高演化富有机质页岩和高煤阶煤中甲烷的吸附—扩散性能，建立了煤/页岩中甲烷的吸附—扩散性模型，对比分析了煤/页岩中甲烷的吸附—扩散性能的差异性和控制机理。结果表明，高演化富有机质页岩样和高煤阶煤样的孔容均主要由介孔和大孔贡献，比表面积主要由微孔和介孔贡献，且高演化富有机质页岩样纳米孔隙更发育，比表面积和孔容要大于煤样。高演化富有机质页岩和高煤阶煤中甲烷的吸附和扩散规律服从Langmuir方程，高演化富有机质页岩中甲烷吸附性能明显低于高煤阶煤，且随着高演化富有机质页岩TOC含量的增加而增高；但其对甲烷扩散性能要高于高煤阶煤一个数量级。高演化富有机质页岩样中孔隙多为开放型，而高阶煤基质孔隙多为半封闭型。对于半封闭型孔隙，强吸附质的溶入会改变吸附剂的大分子结构，其吸附与解吸过程不是可逆的，存在解吸滞后现象，导致高演化富有机质页岩与高煤阶煤中甲烷解吸—扩散过程与扩散—吸附过程中的扩散性能差异性。
孟召平，刘金融，李国庆 . 高演化富有机质页岩和高煤阶煤中甲烷吸附—扩散性能的实验分析[J]. 天然气地球科学, 2015 , 26(8) : 1499 -1506 . DOI: 10.11764/j.issn.1672-1926.2015.08.1499
Methane adsorption-diffusion property in coalbed/shale is one of the key factors for coalbed methane/shale gas resource evaluation.With No.3 coal seam of Permian Shanxi Formation in Sihe coalfield Jincheng mine area and shale of Longmaxi Formation in Lower Silurian of Paleozoic in south China as study objects,the nano-pore system determination using low temperature liquid nitrogen adsorption method and methane adsorption-diffusion experiments of manometer method was conducted,methane adsorption-diffusion properties of high-maturity organic-rich shale samples and high-rank coal sample were elucidated,and then a mathematical model of methane adsorption-diffusion in coal/shale was established,finally the difference of methane adsorption-diffusion in coal and shale and its controlling mechanism were analyzed.It turns out that,meso-pores and macro-pores contribute in a major way to the pore volume of high-maturity organic-rich shale and coal samples and micro-pores and meso-pores contribute in a major way to the specific surface area;the nano-pore system is more developed in shale samples than that in coal sample and the specific surface area and pore volume in shale samples are bigger than that in coal samples;the methane adsorption-diffusion in coal and shale samples can be governed by Langmuir Equation,high-maturity organic-rich shale has a much lower methane adsorption capacity than high-rank coal and the methane adsorption capacity of shale increases with the increase of total organic carbon;open pores dominate in high-maturity organic-rich shale samples while semi-sealed pores dominate in high-rank coal sample;for semi-sealed pores,the dissolution of strong adsorbate into adsorbent will alter the macromolecular structure of adsorbent and result in the irreversibility of adsorption and desorption,that is,desorption hysteresis;therefore the diffusion properties during methane desorption-diffusion are different from that during methane diffusion-adsorption in high-maturity organic-rich shale and coal.
Key words： Organic-rich shale rock; High rank coal; Adsorption; Diffusion
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