盐浸作用下粉煤灰矿化CO2增效机制及抑制煤自燃特性

Enhancement mechanism of CO2 mineralization in fly ash under salt leaching and its inhibition characteristics of coal spontaneous combustion

  • 摘要: 粉煤灰矿化固碳协同防控采空区煤自燃是实现低碳防灭火的重要途径。为解决粉煤灰浆液Ca2+浸出速率慢、矿化CO2效率低,以及传统物理强化方法能耗高等问题,提出盐浸处理强化粉煤灰矿化CO2效能的思路,研究乙酸钠和乙酸铵2种典型盐试剂对粉煤灰矿化效能的强化机制。采用激光粒度仪、低温N2吸附法、红外光谱仪等手段分析盐浸作用对粉煤灰物化结构的改性效果,利用离子色谱仪分析盐浸条件下粉煤灰浆液Ca2+的浸出特性,借助CO2矿化反应系统结合伪二级动力学模型,探究盐浸处理对粉煤灰矿化反应过程的强化规律。试验结果表明:乙酸铵处理使粉煤灰的比表面积和孔容分别提升了62.63%和300.00%,D50较原始样品下降了31.80%,颗粒细化效果显著;乙酸钠处理则在一定程度上起到解聚粉煤灰结构的作用,改性效果相对较弱。在离子浸出方面,乙酸铵处理后粉煤灰浆液中Ca2+质量浓度在浸出30 min时达到4 478 mg/L,较对照组增加了375.37%,乙酸钠处理使Ca2+质量浓度增长了68.57%,表明盐浸处理有效提升了粉煤灰浆液Ca2+浸出质量浓度与速率。矿化反应动力学分析显示,盐浸处理后粉煤灰矿化CO2初始反应速率及固碳量显著提高,乙酸铵处理样品的CO2封存量达到36.18 g/kg,较未处理样品提升了46.30%,乙酸钠处理样品则达到27.98 g/kg。煤自燃抑制试验表明,乙酸铵处理粉煤灰矿化样品与煤样混合后,氧化放热量较原煤样下降了17.48%,较原始粉煤灰和煤样的混合样品降低了9.20%,表现出更优异的煤自燃抑制特性。盐浸作用尤其是乙酸铵处理,可通过物理扩孔—离子交换—化学活化的协同作用显著提升粉煤灰的矿化固碳能力,为粉煤灰碳封存与煤自燃灾害防控的一体化应用提供理论依据。

     

    Abstract: Using fly ash for CO2 mineralization and sequestration, and applying its products to prevent and control spontaneous combustion of coal in goafs, is an important approach to achieve the synergistic governance of pollution reduction, carbon emission reduction, and disaster control. To address the problems of slow leaching rate of Ca2+, low mineralization efficiency in fly ash, as well as high energy consumption of traditional physical modification methods, this study proposes the idea of enhancing the CO2 mineralization efficiency of fly ash through salt leaching treatment, with a focus on investigating the strengthening mechanisms of two typical salt reagents (sodium acetate and ammonium acetate) on the mineralization efficiency of fly ash. Laser particle size analyzer, low-temperature N2 adsorption method, Fourier Transform Infrared Spectrometer (FTIR) and other techniques were used to analyze the modification effect of salt leaching on the physicochemical structure of fly ash; ion chromatograph was employed to study the Ca2+ leaching characteristics in fly ash slurry under salt leaching conditions; and a CO2 mineralization reaction system combined with a pseudo-second-order kinetic model was utilized to explore the strengthening law of salt leaching treatment on the fly ash mineralization process. The experimental results show that ammonium acetate treatment increased the specific surface area and pore volume of fly ash by 62.63% and 300.00% respectively, and the D50 decreased by 31.80% compared with the original sample, exhibiting a significant particle refinement effect. Sodium acetate treatment plays a role in depolymerizing the structure of fly ash to a certain extent, with a relatively weak modification effect. In terms of ion leaching, the mass concentration of Ca2+ in the fly ash slurry reached 4 478 mg/L after 30 minutes of ammonium acetate treatment, which was 375.37% higher than that of the control group; sodium acetate treatment increased the mass concentration of Ca2+ by 68.57%, indicating that salt leaching treatment effectively improved the leaching mass concentration and rate of Ca2+. Kinetic analysis of the mineralization reaction showed that after salt leaching treatment, the initial CO2 mineralization reaction rate and carbon sequestration capacity of fly ash was significantly improved. The CO2 sequestration capacity of fly ash samples treated with ammonium acetate reached 36.18 g/kg, which was 46.30% higher than that of the untreated samples, while the sequestration capacity of samples treated with sodium acetate reached 27.98 g/kg. In terms of inhibiting coal spontaneous combustion, when the mineralized products of ammonium acetate-treated fly ash were mixed with coal samples, the heat release during oxidation decreased by 17.48% compared with the original coal samples and by 9.20% compared with the coal samples treated with original fly ash, demonstrating more excellent inhibition characteristics. Salt leaching treatment, especially ammonium acetate treatment, can significantly enhance the mineralization and carbon sequestration capacity of fly ash through the synergistic effect of physical pore expansion, ion exchange, and chemical activation, providing a theoretical basis for the integrated application of fly ash carbon sequestration and coal spontaneous combustion disaster control.

     

/

返回文章
返回