Synthesis of biomass combustion fly ash derived zeolites for CO2 adsorption: Optimisation of hydrothermal synthetic pathway

Abstract

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.