Gasification is an effective technology for the thermal disposal of municipal solid waste (MSW) with lower dioxin emission compared to the prevailing incineration process. Nevertheless, the mechanism of dioxin formation in the reducing atmosphere during the gasification process was seldomly explored. Herein, the effects of the atmosphere, temperature, and chlorine source were systematically investigated in terms of dioxin distribution. With CO2 and H2O as gasification agents, a reducing reaction atmosphere was formed with abundant H2 which effectively suppressed the generation of C–Cl, contributing to a substantial decrease of dioxin concentration by ∼80% compared to the incineration process. The formation of dioxin was favored at temperatures below 700 °C with its peak concentration achieved at 500 °C. It was unveiled that inorganic chlorine played a dominant role in the reducing atmosphere, with a lower proportion of C–O–C/O–CO on residual slag compared to an oxidizing atmosphere. Additionally, the generated H2 reduced the concentration of dioxins by attacking C–Cl and inhibiting the crucial Deacon reaction for dioxin formation, validated by density functional theory calculation. Eventually, the formation route paradigm and the reaction mechanism of dioxin formation from MSW gasification were revealed, facilitating and rationally guiding the control of dioxin emission.
The calorific value of household refuse (HR) is greatly improved after classification, which includes the implementation of sufficient pyrolysis conditions. Therefore, a better pyrolysis effect can be achieved by co-pyrolysis with industrial solid waste (ISW) with high calorific value. In this work, HR and ISW were used as raw materials for co-pyrolysis experiments. The influence on the distribution of three-phase products after co-pyrolysis, the concentration of heavy metals and dioxins in the flue gas, and the distribution of PCDD/Fs isomers were studied. The results showed that, at a temperature of 600 °C and H/C = 1.3, of the formed material, the quantity of pyrolysis gas was approximately 27 wt.%, and the quantity of pyrolysis oil was approximately 40.75 wt.%, which mainly contained alkanes, olefins, and aromatic hydrocarbons. When S/C = 0.008, pyrolysis gas accounted for 25.95 wt.% of the formed material, and pyrolysis oil for 41.95 wt.% of the formed material. The ignition loss rate of pyrolysis coke was approximately 20%, and the maximal calorific value was 14,217 KJ/kg. According to the thermogravimetric experiment, the co-pyrolysis of HR and ISW can promote the positive reaction of pyrolysis, and the weight loss reached 62% at 550 °C. The emission of gaseous heavy metals was relatively stable, and the concentration of heavy metals slightly decreased. The main heavy metals in the ash were Cu, Fe, and Zn. The emission of dioxins could be effectively reduced by the pyrolysis of HR with ISW, and the produced dioxins were mainly synthesized from de novo synthesis. After pyrolysis, the toxic equivalent of dioxins in the flue gas was reduced from 0.69 to 0.29 ng I-TEQ/Nm3, and the distribution of dioxin isomers in the flue gas had little influence. The experimental results provide a theoretical basis for the application of co-pyrolysis technology with HR and ISW.
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