Han Sijie, Zhou Xiaozhi, Zhang Jinchao, Xiang Wenxin, Xu Ang
Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, Xuzhou 221008, China.
Carbon Neutrality Institute, China University of Mining and Technology, Xuzhou 221008, China.
ACS Omega. 2022 Feb 24;7(9):8091-8102. doi: 10.1021/acsomega.1c07402. eCollection 2022 Mar 8.
Coal is characterized by a complex pore-fracture network and functional groups, which are derived from various geological origins and which further affect methane adsorption. To explore the relationship between the geological origins of pore-fractures and methane adsorption behaviors, we conducted pore structure tests and adsorption isotherms on six Qinshui high-rank coals. The pores and fractures were observed using an optical microscope (OM), a field emission scanning electron microscope (FESEM), and a high-resolution transmission electron microscope (HRTEM), and the pore structure parameters were determined using mercury intrusion and low-pressure N and CO adsorption. High-pressure CH adsorption isotherms were obtained at 30 °C using the manometric method. Results show that the Qinshui high-rank coals develop five stages of pore size distribution, consisting of the smaller micropore stage (0.3-1 nm), the larger micropore and smaller mesopore stage (1-10 nm), the mesopore and smaller macropore stage (10-110 nm), the microfracture stage (0.11-40 μm), and the larger macropore stage (>40 μm). The micropores dominate the total pore volume (PV) and specific surface area (SSA). Pores and fractures of various morphologies and sizes have different geological origins, which are related to coalification and stress field evolution. Methane adsorption on coals mainly occurs in the micropores as a form of volume filling. The maximum pore size for complete gas filling (MPSCGF) ranges from 0.60 to 0.88 nm in Qinshui high-rank coals. The coal-forming geological processes, such as coalification and stress field evolution, contribute to various pores and fractures, which show different pore sizes and functional groups. The geological origins of pores and fractures control the methane adsorption behaviors in coals by way of the pore size and functional groups. Surface coverage-related methane adsorption behavior occurs in fractures, primary pores, and large-scale secondary pores, while micropore filling is the methane adsorption behavior in macromolecular pores and small-scale secondary pores. The aim of this study is to provide a new insight into the methane adsorption on coals from the geological process of the formation and modification of pores and fractures.
煤具有复杂的孔隙 - 裂隙网络和官能团,这些源自各种地质成因,并进一步影响甲烷吸附。为了探究孔隙 - 裂隙的地质成因与甲烷吸附行为之间的关系,我们对六种沁水高阶煤进行了孔隙结构测试和吸附等温线测定。使用光学显微镜(OM)、场发射扫描电子显微镜(FESEM)和高分辨率透射电子显微镜(HRTEM)观察孔隙和裂隙,并使用压汞法以及低压氮气和二氧化碳吸附法测定孔隙结构参数。采用压力法在30℃下获得高压甲烷吸附等温线。结果表明,沁水高阶煤呈现出五个孔径分布阶段,包括较小微孔阶段(0.3 - 1纳米)、较大微孔和较小中孔阶段(1 - 10纳米)、中孔和较小大孔阶段(10 - 110纳米)、微裂隙阶段(0.11 - 40微米)以及较大大孔阶段(>40微米)。微孔在总孔体积(PV)和比表面积(SSA)中占主导地位。各种形态和尺寸的孔隙和裂隙具有不同的地质成因,这与煤化作用和应力场演化有关。煤对甲烷的吸附主要以体积填充的形式发生在微孔中。沁水高阶煤中完全气体填充的最大孔径(MPSCGF)范围为0.60至0.88纳米。煤化作用和应力场演化等成煤地质过程造就了各种孔隙和裂隙,它们呈现出不同的孔径和官能团。孔隙和裂隙的地质成因通过孔径和官能团控制煤中的甲烷吸附行为。与表面覆盖相关的甲烷吸附行为发生在裂隙、原生孔隙和大规模次生孔隙中,而微孔填充是大分子孔隙和小规模次生孔隙中的甲烷吸附行为。本研究的目的是从孔隙和裂隙形成与改造的地质过程方面,为煤对甲烷的吸附提供新的见解。