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High-pressure sorption isotherms and sorption kinetics of CH_4 and CO_2 on coals

机译：煤上CH_4和CO_2的高压吸附等温线及吸附动力学

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摘要

Using a manometric experimental setup, high-pressure sorption measurements with CH_4 and CO_2 were performed on three Chinese coal samples of different rank (VR_r = 0.53%, 1.20%, and 3.86%). The experiments were conducted at 35,45, and 55 ℃ with pressures up to 25 MPa on the 0.354-1 mm particle fraction in the dry state. The objective of this study was to explore the accuracy and reproducibility of the manometric method in the pressure and temperature range relevant for potential coalbed methane (CBM) and CO_2-enhanced CBM (CO_2-ECBM) activities (P＞8 MPa, T＞35℃). Maximum experimental errors were estimated using the Gauss error propagation theorem, and reproducibility tests of the high-pressure sorption measurements for CH_4 and CO_2 were performed. Further, the experimental data presented here was used to explicitly study the CO_2 sorption behaviour of Chinese coal samples in the elevated pressure range (up to 25 MPa) and the effects of temperature on supercritical CO_2 sorption isotherms.rnThe experiments provided characteristic excess sorption isotherms which, in the case of CO_2 exhibit a maximum around the critical pressure and then decline and level out towards a constant value. The results of these manometric tests are consistent with those of previous gravimetric sorption studies and corroborate a crossover of the 35,45, and 55 ℃ CO_2 excess sorption isotherms in the high-pressure range. The measurement range could be extended, however, to significantly higher pressures. The excess sorption isotherms tend to converge, indicating that the temperature dependence of CO_2 excess sorption on coals at high-pressures (＞20 MPa) becomes marginal. Further, all CO_2 high-pressure isotherms measured in this study were approximated by a three-parameter excess sorption function with special consideration of the density ratio of the "free" phase and the sorbed phase. This function provided a good representation of the experimental data.rnThe maximum excess sorption capacity of the three coal samples for methane ranged from 0.8 to 1.6 mmol/g (dry, ash-free) and increased from medium volatile bituminous to subbituminous to anthracite. The medium volatile bituminous coal also exhibited the lowest overall excess sorption capacity for CO_2. However, the subbituminous coal was found to have the highest CO_2 sorption capacity of the three samples. The mass fraction of adsorbed substance as a function of time recorded during the first pressure step was used to analyze the kinetics of CH_4 and CO_2 sorption on the coal samples. CO_2 sorption proceeds more rapidly than CH_4 sorption on the anthracite and the medium volatile bituminous coal. For the subbituminous coal, methane sorption is initially faster, but during the final stage of the measurement CO_2 sorption approaches the equilibrium value more rapidly than methane.
机译：使用测压实验装置，对三种不同等级的中国煤样品（VR_r = 0.53％，1.20％和3.86％）进行CH_4和CO_2高压吸附测量。实验是在35,45和55℃于干燥状态下以0.354-1 mm的颗粒级分在最高25 MPa的压力下进行的。本研究的目的是探索压力法在与潜在煤层气（CBM）和CO_2增强的CBM（CO_2-ECBM）活性（P＞ 8 MPa，T＞ 35）相关的压力和温度范围内的准确性和可重复性。 ℃）。使用高斯误差传播定理估计最大实验误差，并进行了CH_4和CO_2的高压吸附测量的重现性测试。此外，本文提供的实验数据用于明确研究中国煤样品在高压范围（最高25 MPa）下的CO_2吸附行为以及温度对超临界CO_2吸附等温线的影响。在CO_2的情况下，在临界压力附近表现出最大值，然后下降并趋于恒定值。这些测压试验的结果与以前的重力吸附研究结果一致，并证实了在高压范围内35,45和55℃CO_2过量吸附等温线的交叉。但是，测量范围可以扩展到更高的压力。过量吸附等温线趋于收敛，表明在高压（＞ 20 MPa）下煤上CO_2过量吸附对温度的依赖性很小。此外，在本研究中测得的所有CO_2高压等温线均通过三参数过量吸附函数进行了近似，并特别考虑了“游离”相与被吸附相的密度比。该功能很好地说明了实验数据。三个煤样品对甲烷的最大过剩吸附容量为0.8至1.6 mmol / g（干燥，无灰），并且从中等挥发性的沥青到次烟煤再增加。中等挥发性的烟煤对CO_2的总体过剩吸附能力也最低。但是，发现三个样品中的次烟煤对CO_2的吸附能力最高。在第一压力步骤中记录的吸附物质的质量分数随时间的变化被用于分析煤样品上CH_4和CO_2吸附的动力学。在无烟煤和中等挥发性烟煤上，CO_2的吸附比CH_4的吸附更快。对于次烟煤，甲烷的吸附最初速度更快，但在测量的最后阶段，CO_2的吸附比甲烷更快地达到平衡值。

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  • 来源
    《Fuel》 |2010年第3期|569-580|共12页
  • 作者

    Dongyong Li; Qinfu Liu; Philipp Weniger; Yves Gensterblum; Andreas Busch; Bernhard M. Krooss;

  • 作者单位

    Department of Resources and Earth Science, China University of Mining and Technology, Beijing, PR China Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Aachen, Germany;

    Department of Resources and Earth Science, China University of Mining and Technology, Beijing, PR China;

    Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Aachen, Germany;

    Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Aachen, Germany;

    Shell International Exploration and Production B.V., Rijswijk, The Netherlands;

    Institute of Geology and Geochemistry of Petroleum and Coal, RWTH Aachen University, Aachen, Germany;

  • 收录信息 美国《科学引文索引》(SCI);美国《工程索引》(EI);
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    coalbed methane (CBM); CO_2-ECBM; CO_2 coal seam sequestration; sorption kinetics; supercritical CO_2;

    机译：煤层气（CBM）;CO_2-ECBM;CO_2煤层固存;吸附动力学超临界CO_2;

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