粉煤灰因产量大、价格低廉，具备矿化吸附固定CO₂能力等优势，成为煤炭行业CCUS矿化技术中重要原材料之一。但粉煤灰中钙基活性物质含量较少，表现出较低的CO₂封存能力，且基于固碳粉煤灰的煤矿采空区安全封存技术尚不完善。基于此，本文利用碱性激活剂提升粉煤灰矿化反应活性，增强粉煤灰矿化固碳效率，自主搭建高温高压搅拌反应釜矿化实验平台，研究碱活化粉煤灰矿化固碳性能，并为固碳粉煤灰煤矿采空区安全封存技术提出潜在应用途径，通过COMSOL软件确定固碳粉煤灰采空区安全封存关键技术参数，研究基于固碳粉煤灰的采空区安全封存效果。

借助高温高压搅拌反应釜矿化实验平台及热重分析仪，总结基于压降法与热重分析法的矿化反应CO₂吸收性能表征方式。结果表明，粉煤灰矿化反应过程反应釜内压力在前30min内快速降低后逐渐平稳，即CO₂吸收过程主要集中在矿化反应前期；粉煤灰碱活化处理、矿化反应压力增加、矿化反应温度升高均可提升粉煤灰矿化反应CO₂吸收性能，其中碱活化处理对粉煤灰矿化固碳性能提升效果最优；根据皮尔逊相关系数量化分析，粉煤灰中Ca元素与S元素含量与CO₂吸收量呈现显著的线性相关，直接影响粉煤灰CO₂矿化吸收性能；矿化反应后粉煤灰中吸附水、结晶水与Ca(OH)₂含量减少，Ca(OH)₂参与矿化反应被消耗，同时硅酸盐矿物含量因矿化反应而降低。

通过多方位测试实验，总结了碱活化粉煤灰矿化反应前后结构与组成特征。结果表明，微观尺度下粉煤灰呈规则球状颗粒，碱活化处理后颗粒表面被C-S-H凝胶物质覆盖，且凝胶中Si-O聚合度较高；碱活化剂会促进粉煤灰颗粒表面溶解，内部应力变化造成颗粒微观破裂和细化，导致粉煤灰粒径分布降低；随着碱活化程度提高，粉煤灰中CaO与MgO含量上升，表面Ca元素分布量显著提升，碱活化处理可促进粉煤灰细化，暴露更多活性Ca元素有利于矿化固碳；碱活化粉煤灰矿化反应后，球状颗粒周围形成大量以Ca、C、O为主的非结晶物质，且粒径分布范围提升，证明粉煤灰表面形成新的CaCO₃沉淀。

基于采空区综采架后间断充填技术与煤矿采空区物理化学协同封存方式，形成固碳粉煤灰采空区安全封存工艺体系。利用COMSOL数值模拟优化采空区安全封存工艺参数，在保证采空区封存地质体安全稳定前提下，计算采空区最大碳封存量。数值模拟结果表明，充填封存体间隔距离直接影响采空区结构安全稳定，充填体间隔距离从2m增加至20m时，采空区上覆岩位移显著增加，充填体支撑压力大幅提升。以天池煤矿605工作面采空区为例，采空区充填体间隔距离优化值为4.2m。以碱活化程度为15%的褐煤粉煤灰为矿化原材料，基于固碳粉煤灰的采空区封存技术物理化学协同碳封存总量为2995.3吨。

Fly ash has become one of the essential raw materials in the CCUS mineralization technology within the coal industry due to its significant output, low cost, and ability to mineralize, absorb, and fix CO₂. However, the content of calcium-based active substances in fly ash is low, resulting in a reduced capacity for CO₂ sequestration. Moreover, the safe sequestration technology of coal mine goafs using carbon-fixed fly ash is not yet fully developed. This paper utilizes an alkaline activator to enhance the mineralization reaction activity of fly ash, thereby improving the efficiency of mineralization and carbon fixation. An independent high-temperature, high-pressure stirring reactor mineralization experimental platform was constructed to investigate the carbon fixation performance of alkali-activated fly ash. It also proposes potential application pathways for the technology of safe sequestration in coal mine goafs using carbon-fixed fly ash. Key technical parameters for the safe sequestration of carbon-fixed fly ash in goafs were determined using COMSOL software, exploring the effectiveness of safe sequestration in goafs based on carbon-fixed fly ash.

With the high-temperature and high-pressure stirred reactor mineralization experimental platform and TG analyzer, the CO₂ absorption performance characterization method of mineralization reaction based on the pressure drop and TG analysis method is summarized. The results show that during the fly ash mineralization reaction, the pressure in the reactor decreased rapidly in the first 30 minutes and then gradually stabilized, the CO₂ absorption process was mainly concentrated in the early stage of the mineralization reaction. The alkali activation treatment of fly ash, the increasing in mineralization reaction pressure and temperature can improve the CO₂ absorption performance of mineralization reaction, among which alkali activation treatment has the best effect on improving the mineralization and carbon fixation performance of fly ash. According to the quantitative analysis of Pearson's correlation coefficient, the Ca and S elements in fly ash have a significant linear correlation with the CO₂ absorption, which directly affects the mineralization absorption performance of fly ash. After the mineralization reaction, the contents of adsorbed water, crystal water and Ca(OH)₂ in fly ash are reduced, and Ca(OH)₂ participates in the mineralization reaction and is consumed, while the silicate mineral content is reduced due to the mineralization reaction.

Through multi-faceted testing experiments, the structure and composition characteristics before and after the alkali-activated fly ash mineralization reaction were summarized. The results show that fly ash appears as regular spherical particles at microscopic, after alkali activation treatment, the particles surface is covered with C-S-H gel material, and the Si-O polymerization degree is high. The alkali activator will promote the surface dissolution of fly ash particles, and internal stress changes will cause microscopic cracking of particles, resulting in a reduction in particle size distribution. As the degree of alkali activation increases, the CaO and MgO contents increase, and the surface Ca element distribution increases significantly, which can promote the refinement of fly ash and expose more active Ca elements, which is beneficial to mineralization and carbon fixation. After the mineralization reaction, a large amount of amorphous substances mainly composed of Ca, C, and O were formed around the spherical particles, and the particle size distribution range increased, proving that new CaCO₃ precipitation was formed on the surface of the fly ash.

Based on the intermittent backfilling technology behind the comprehensive mining frame in goaf areas and the physicochemical collaborative sequestration approach in coal mine goafs, a safe sequestration process system for carbon-fixed fly ash in goaf areas has been developed. Utilizing COMSOL for numerical simulations optimizes the process parameters for safe sequestration in goaf areas, calculating the maximum carbon sequestration capacity while ensuring the safety and stability of the geologic bodies in the goaf. The simulation results indicate that the spacing distance between backfill bodies directly impacts the safety and stability of the goaf structure. An increase in the spacing distance from 2m to 20m significantly raises the displacement of the overlying rock in the goaf and substantially increases the support pressure of the backfill body. Taking the goaf of the 605-working face in Tianchi Coal Mine as an example, the optimized spacing distance between the backfill bodies is 4.2m. Using lignite fly ash with an alkali activation degree of 15% as the mineralized raw material, the total amount of physicochemical synergistic carbon sequestration achieved through the goaf's safe sequestration technology based on carbon-fixed fly ash is 2995.3 tons.

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