粉煤灰直接湿法矿化封存CO2机制及关键影响因素优化研究

    Study on the mechanism of direct wet mineralization of fly ash for CO2 storage and optimization of key influencing factors

    • 摘要: 为了提升粉煤灰的CO2封存效率,促进粉煤灰在CO2矿化封存与防灭火工程的资源化利用,对粉煤灰矿化反应条件及添加剂配比进行了优化研究。采用直接湿法矿化技术,构建了气−液−固三相反应体系,通过正交试验设计系统考察水灰比、反应时间、气体流量对矿化效率的影响,并通过极差分析与方差分析确定主次因素及最优参数组合,进而评估不同条件对矿化性能的影响程度及主次顺序;引入Na2CO3、NaCl、NaOH、NaHCO3等添加剂(浓度0.5 mol/L),通过单因素试验筛选最优配方;矿化产物的物相组成与微观形貌通过X射线衍射仪(XRD)、扫描电子显微镜(SEM)表征,结合热重分析(TGA)定量评估CO2封存量;灭火性能试验通过模拟煤堆自燃场景,监测温度及CO体积分数变化,验证材料的实际灭火效果。结果表明:矿化条件优化方面,水灰比4∶1、反应时间45 min、气体流量150 mL/min时,CO2封存量达57.75 kg/t,显著优于其他组合;添加剂优选试验中,0.5 mol/L Na2CO3效果最佳,其通过提高液相\mathrmCO_3^2- 浓度并维持碱性环境,促进CaCO3生成;而NaCl因增加CaCO3溶解度抑制沉淀,NaOH因强碱性环境导致方解石晶粒尺寸减小,均降低矿化效率;XRD与SEM表征证实,矿化后粉煤灰中波特兰石(Ca(OH)2)与生石灰(CaO)衍射峰消失,方解石(CaCO3)峰显著增强;微观形貌显示,原样多孔结构表面附着致密球状CaCO3颗粒,验证了CO2矿化路径的可行性;粉煤灰基材料在灭火试验中通过覆盖层阻隔氧气、水分蒸发吸热及渗透降温协同作用,使得煤堆上、中、下部温度在600 s内降至120 ℃以下,CO体积分数在180 s后稳定在30×10−6以下。

       

      Abstract: In order to enhance the CO2 sequestration efficiency of fly ash and promote its resource utilization in CO2 mineralization sequestration and fire prevention and extinguishing projects, an optimization study was conducted on the reaction conditions and additive ratios of the fly ash mineralization process. A direct wet mineralization technique was employed to establish a gas-liquid-solid three-phase reaction system. The effects of water-to-ash ratio, reaction time, and gas flow rate on mineralization efficiency were systematically examined through an orthogonal experimental design. Range analysis and variance analysis were used to determine the primary and secondary influencing factors as well as the optimal parameter combination, thereby evaluating the impact of different conditions on mineralization performance. Additives including Na2CO3, NaCl, NaOH, and NaHCO3 (at a concentration of 0.5 mol/L) were introduced, and a single-factor experiment was conducted to screen for the optimal formulation. The mineralization products were characterized by X-ray diffraction (XRD) and scanning electron microscopy (SEM), while thermo gravimetric analysis (TGA) was used to quantitatively assess the CO2 sequestration capacity. Fire suppression performance was evaluated through simulated coal pile spontaneous combustion experiments by monitoring temperature and CO volume fraction variations to verify the practical fire extinguishing effect. The results indicate that: in terms of mineralization condition optimization, a water-to-ash ratio of 4∶1, reaction time of 45 minutes, and gas flow rate of 150 mL/min yielded a CO2 sequestration capacity of 57.75 kg/t, significantly surpassing other parameter combinations; among the additive selection experiments, 0.5 mol/L Na2CO3 exhibited the best performance by increasing the \mathrmCO_3^2- concentration in the liquid phase and maintaining an alkaline environment to promote CaCO3 formation. Conversely, NaCl reduced mineralization efficiency by enhancing CaCO3 solubility, while NaOH, due to its strong alkalinity, decreased calcite grain size, thereby inhibiting precipitation; XRD and SEM characterization confirmed the disappearance of portlandite (Ca(OH)2) and quicklime (CaO) diffraction peaks in mineralized fly ash, with a significant enhancement of calcite (CaCO3) peaks. The microstructural analysis revealed the transformation of the originally porous surface into a dense layer of spherical CaCO3 particles, verifying the feasibility of the CO2 mineralization pathway; in fire extinguishing experiments, the fly ash-based material effectively reduced coal pile temperatures below 120 ℃ within 600 seconds through oxygen barrier coverage, heat absorption via moisture evaporation, and penetration cooling mechanisms. The CO volume fraction stabilized below 30×10−6 after 180 seconds.

       

    /

    返回文章
    返回