二氧化碳捕集、利用及封存技术（CCUS）是降低CO₂排放、实现碳中和目标的重要技术路线，在近年来得到了迅速发展。在各类CO₂利用技术中，研发CO₂矿化煤基固废充填材料（CMWB）是实现煤炭工业低碳发展的有效途径之一。CO₂矿化养护煤基固废技术可作为采空区充填材料，具有加速材料早期强度形成、防止采空区中有害气体逸散、降低养护能耗、消耗工业固废等优势。此技术不仅可以实现CO₂封存利用，还能生产高附加值的建材产品，具有广阔的工业化应用前景。现有研究缺乏对CO₂矿化养护煤基固废混凝土，尤其是煤矸石混凝土机械性能、矿化机理及其作为采空区充填材封存CO₂安全性的相关论述。本文选取煤矸石这种常见煤基固废作为混凝土的粗骨料，选取普通硅酸盐水泥、粉煤灰作为凝胶材料，对不同CO₂矿化养护工艺下的煤矸石混凝土机械性能、矿化机理和其作为充填材料在采空区中封存的CO₂安全性进行了相关研究。

本文首先研究了CO₂矿化养护工艺（矿化养护时间、粉煤灰掺量、养护温度）对煤矸石混凝土宏观物理性能和微观结构的影响。结果表明：矿化养护时间增加可促进煤矸石混凝土内部整体性，砂浆区及界面过渡区孔隙率减小，导致煤矸石混凝土力学强度增强。适量掺入粉煤灰（粉煤灰掺量0%~30%）可促进煤矸石混凝土内部水化，表现为自身力学性能增强；过量掺入粉煤灰（粉煤灰掺量≥30%），此时粉煤灰颗粒包裹水泥颗粒，导致混凝土内部矿化反应受阻，表现为煤矸石混凝土力学性能下降。适度增加养护温度（20~40℃），CO₂在混凝土中扩散速率增加，表现为煤矸石混凝土力学性能增加；养护温度过高（≥40℃）时，CO₂在混凝土孔隙水中溶解度降低，混凝土内部矿化反应受阻，表现为煤矸石混凝土力学性能下降。

其次，本文进一步研究了CO₂矿化煤矸石混凝土反应机理，并通过FT-IR、XRD、TG-DTG等方法刻画了煤矸石混凝土在不同矿化养护工艺下化学分子结构及官能团、物相组成及含Ca基物质的变化规律，进一步解释了矿化反应机理与混凝土固碳率变化。结果表明：矿化养护时间增加，使得煤矸石混凝土内部CH物质逐渐减少，CaCO₃含量逐渐增加。随粉煤灰掺量与养护温度增加，煤矸石混凝土内部CH物质变化率呈先减少后增加的趋势，CaCO₃物质变化率呈先增加后减少的趋势。同时，CaCO₃物质变化率代表煤矸石混凝土固碳能力演化，故可以得出混凝土固碳率与矿化养护时间呈正相关，与粉煤灰掺量、养护温度呈开口向下的二次增函数关系。

最后，为获得不同养护工艺参数交互影响下的最优养护工况与其作为充填材料在采空区中的CO₂封存安全性，本文基于多目标优化的响应曲面法构建了煤矸石混凝土抗压强度和固碳率与矿化养护时间、粉煤灰掺量、养护温度的数值模型，得出了最优工艺参数。基于最优工艺参数，利用COMSOL软件实现煤矸石混凝土采空区充填碳封存技术工程实践验证。结果表明：性能预测模型得出，当矿化养护时间为9d，粉煤灰掺量为13.84%、养护温度为50.58℃时，煤矸石混凝土具有最高的抗压强度和较高的固碳率，分别为30.68MPa和21.39%。数值模拟结果表明，煤矸石混凝土力学强度越高，内部CO₂储存量越大。当采空区壁面达到预设最大抗压强度（30.68MPa）时，其对应CO₂储存量为1.4×10⁴kg，达到最大储量时其最大安全注气天数为82d。

Carbon Capture, Utilization, and Storage (CCUS) technology is an important pathway for reducing CO₂ emissions and achieving carbon neutrality goals, and has rapidly developed in recent years. Among various CO₂ utilization technologies, developing CO₂ mineralized coal-based solid waste filling materials (CMWB) is one of the effective approaches to achieve low-carbon development in the coal industry. The technology of CO₂ mineralization curing of coal-based solid waste can be used as a filling material for mined-out areas, offering advantages such as accelerating the early strength formation of materials, preventing the escape of harmful gases in mined-out areas, reducing curing energy consumption, and utilizing industrial solid waste. This technology not only enables the utilization and storage of CO₂ but also produces high-value-added building material products, presenting broad prospects for industrial application. Existing research lacks discussions on the mechanical properties, mineralization mechanisms of CO₂ mineralized coal-based solid waste concrete, particularly coal gangue concrete, and its safety in CO₂ sequestration as a filling material in mined-out areas. This paper selects coal gangue, a common type of coal-based solid waste, as coarse aggregate for concrete, and uses ordinary Portland cement and fly ash as gel materials to study the mechanical properties, mineralization mechanisms of coal gangue concrete under different CO₂ mineralization curing processes, and its safety in CO₂ sequestration as a filling material in mined-out areas.

This article first studies the effects of CO₂ mineralization curing processes (mineralization curing time, fly ash content, curing temperature) on the macroscopic physical properties and microstructure of coal gangue concrete. The results show that an increase in mineralization curing time promotes the overall integrity of the coal gangue concrete, reducing the porosity in the mortar area and the interfacial transition zone, which leads to enhanced mechanical strength of the coal gangue concrete. A moderate addition of fly ash (fly ash content from 0% to 30%) promotes the hydration within the coal gangue concrete, resulting in enhanced mechanical properties; however, excessive addition of fly ash (fly ash content ≥ 30%) leads to fly ash particles enveloping cement particles, hindering the mineralization reactions inside the concrete and resulting in decreased mechanical properties of the coal gangue concrete. Moderately increasing the curing temperature (20 to 40°C) increases the diffusion rate of CO₂ within the concrete, leading to an increase in mechanical properties of the coal gangue concrete; however, excessively high curing temperatures (≥ 40°C) decrease the solubility of CO₂ in the pore water of the concrete, obstructing the internal mineralization reactions and leading to decreased mechanical properties of the coal gangue concrete.

Subsequently, this article further investigates the reaction mechanism of CO₂ mineralized coal gangue concrete and characterizes the changes in chemical molecular structure, functional groups, phase composition, and Ca-based substances of coal gangue concrete under different mineralization curing processes using FT-IR, XRD, and TG-DTG methods. This further elucidates the correlation between the mineralization reaction mechanism and changes in the concrete's carbon fixation rate. The results show that as the mineralization curing time increases, the amount of CH substances inside the coal gangue concrete gradually decreases while the content of CaCO₃ gradually increases. With the increase in fly ash content and curing temperature, the rate of change of CH substances in the coal gangue concrete shows a trend of initially decreasing and then increasing, whereas the rate of change of CaCO₃ substances shows a trend of initially increasing and then decreasing. Simultaneously, the rate of change of CaCO₃ substances represents the evolution of the carbon fixation capacity of the coal gangue concrete. Therefore, it can be concluded that the carbon fixation rate of the concrete is positively correlated with the mineralization curing time and follows a downward-opening quadratic function relationship with the fly ash content and curing temperature.

Finally, to obtain the optimal curing conditions under the interactive effects of different curing process parameters and to assess the safety of CO₂ sequestration as a filling material in closed mined-out areas, this paper constructs a numerical model of the compressive strength and carbon fixation rate of coal gangue concrete in relation to mineralization curing time, fly ash content, and curing temperature, using the response surface method based on multi-objective optimization. The optimal process parameters were determined. Based on these optimal parameters, the COMSOL software was used to implement and validate the engineering practice of carbon sequestration technology for filling mined-out areas with coal gangue concrete. The results show that the performance prediction model indicates that when the mineralization curing time is 9 days, the fly ash content is 13.84%, and the curing temperature is 50.58°C, the coal gangue concrete has the highest compressive strength and a relatively high carbon fixation rate, at 30.68 MPa and 21.39% respectively. Numerical simulation results suggest that the higher the mechanical strength of the coal gangue concrete, the greater the internal CO₂ storage. When the walls of the mined-out area reach the preset maximum compressive strength (30.68 MPa), the corresponding CO₂ storage is 1.4×10⁴ kg, and the maximum safe injection duration at maximum storage is 82 days.

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