Effects of Mineral Composition and TOC Content of Coal Gangue on CO2 Adsorption Capacity

Backfilling the industrial solid waste coal gangue into deep coal mine goafs for CO2 geological sequestration is a crucial pathway to achieve the synergistic effect of pollution reduction and carbon mitigation. However, in complex deep geological environments, the chemical evolution of multiple mineral phases of coal gangue under gas–water–rock coupling effects and the carbon-controlling mechanism of residual total organic carbon (TOC) remain unclear. In this study, coal gangue from the goaf of the Xiaobaodang Coal Mine was used as the research object. Relying on a customized high-temperature and high-pressure reaction system to simulate the deep in situ environment (45 °C, 10 MPa), and combined with X-ray diffraction (XRD), total organic carbon determination, and isothermal CO2 adsorption experiments, the geochemical mechanism by which inorganic minerals and organic residual carbon synergistically control the ultimate CO2 adsorption potential was systematically revealed. The results show that the modification of the CO2 adsorption potential of coal gangue by gas–water–rock reactions exhibits strong mineral phase differentiation. Systems rich in active silicates generate a large amount of secondary clay minerals through intense carbonation alteration, achieving a significant increase in micro–nano pores and absolute adsorption capacity. Systems rich in carbonates steadily release deep primary adsorption potential by widening mass transfer channels through mineral dissolution. In contrast, systems rich in primary clay minerals face an irreversible attenuation of adsorption space due to physical clogging of pore throats caused by fluid migration. Furthermore, the initial organic carbon content exerts a significant non-linear regulatory effect on the development of the micropore network. The physical adsorption sites provided by the high relative content of layered clay minerals (>41%), coupled with the interfacial enhancement effect exerted by a moderate organic carbon content (0.12~0.16%), constitute an optimal physicochemical synergistic enhancement network, which is the core geological reason for stimulating the ultimate carbon sequestration capacity of coal gangue. The results of this study not only enrich the multiphase interfacial thermodynamic theory of complex heterogeneous geological bodies but also provide solid theoretical support for the precise optimization of target areas and the long-term evaluation of carbon sinks in goaf CO2 sequestration engineering.