合成用于二氧化碳吸附的生物质燃烧粉煤灰衍生沸石:优化水热合成途径

Ben Petrovic, Mikhail Gorbounov, Salman Masoudi Soltani
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摘要

研究人员将工业生物质燃烧飞灰作为沸石的前体,以评估其吸附二氧化碳的潜力。采用田口 L9 阵列,通过实验设计对合成方法进行了优化。确定了三个具有统计意义的变量:结晶温度、结晶时间和液固比。对主效应的分析表明,在 50 °C 时,一组最佳条件下制备的样品具有最高的吸附能力(1.84 mmol g-1)。这是因为在用 NaOH 进行碱熔和水热处理后,原粉煤灰转化成了 A 型(LTA)和 X 型(FAU)沸石。吸附焓估计为 -40.2kJmol-1,并且与表面覆盖率有关;零覆盖率时的等效吸附焓为 -86 kJ mol-1。在模拟变温吸附过程(50 °C/150°C吸附/解吸)中,吸附剂的工作容量在总共 40 个循环后保持在首次吸附量的 85%。通过非线性回归,展示了二氧化碳的平衡吸附等温线和动力学吸附等温线,并建立了模型,以揭示粉煤灰衍生沸石的吸附机理。多相沸石内部存在显著的异质性,呈现出微孔和中孔。所开发的吸附剂为生物质燃烧飞灰的价值化提供了一条可行的途径,在二氧化碳分离方面具有良好的应用潜力。
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Synthesis of biomass combustion fly ash derived zeolites for CO2 adsorption: Optimisation of hydrothermal synthetic pathway

Industrial biomass combustion fly ash has been investigated as a precursor for zeolites with a view to evaluate the potential for adsorption of CO2. The synthesis methodology has been optimised via Design of Experiment by employing a Taguchi L9 array. Three variables were identified as statistically significant, the crystallisation temperature, crystallisation time and the liquid to solid ratio. Analysis of the main effects revealed an optimum set of conditions which produced a sample with the highest adsorption capacity of those prepared, 1.84 mmol g−1 at 50 °C. This was a result of the conversion of the as-received fly ash into type A (LTA) and type X (FAU) zeolites after alkaline fusion with NaOH and hydrothermal treatment. The enthalpy of adsorption was estimated at -40.2kJmol−1 and was shown to be dependent on surface coverage; the isosteric enthalpy of adsorption at zero coverage was -86 kJ mol−1. The working capacity of the adsorbent was maintained at 85 % of the first adsorption uptake after a total of 40 cycles in a simulated temperature swing adsorption process (50 °C/150 °C adsorption/desorption). The equilibrium and kinetic CO2 adsorption isotherms are presented and modelled through non-linear regression to reveal the adsorption mechanisms demonstrated by the fly ash-derived zeolites. Significant heterogeneity exists within the multi-phase zeolite which presents both micro and mesoporosity. The developed adsorbent presents a feasible route to valorisation of biomass combustion fly ash with good potential for application in the separation of CO2.

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