Coupled microwave hydrothermal dechlorination and geopolymer preparation for the solidification/stabilization of heavy metals and chlorine in municipal solid waste incineration fly ash

Abstract

To improve the degradation efficiency of persistent organic pollutants (POPs) in municipal solid waste incineration fly ash (MSWIFA), as well as to overcome the difficulties of subsequent hydrothermal liquid and hydrothermal slag treatment, a two-step treatment strategy of microwave hydrothermal degradation coupled with geopolymer immobilization was proposed. Results showed that the optimal process parameters for microwave hydrothermal dechlorination were a temperature of 220 °C, a time of 1 h, and NaOH addition of 10 wt%. Microwaves accelerated the OH− mediated hydrolysis reactions and promoted the breaking of CCl bonds, leading to dechlorination. The compressive strength of the 20 % MSWIFA-based geopolymers reached 75.79 MPa, and the immobilization rate of the heavy metals (HMs) and Cl− surpassed 90 %. Alkaline environment provided by microwave hydrothermal promoted the formation of Ca(OH)2, which subsequently formed Friedel's salt (3CaO•Al2O3•CaCl2•10H2O) with Cl− in the geopolymer. The charge density difference and density of states (DOS) of Friedel's salt were analyzed by first-principles calculations, confirming that the existence of strong interactions between Ca-s, Al-p, O-p, and Cl-p states was the chemical mechanism of Cl− immobilization. The Friedel's salt and HMs were encapsulated by geopolymers with dense silica-alumina tetrahedral frameworks, achieving the solidification/stabilization (S/S) of HMs and Cl−. This work provided a new approach for the environmentally sound and resourceful treatment of MSWIFA.