Detoxification and Recovery of Spent Carbon Cathodes via NaOH–Na 2 CO 3 Binary Molten Salt Roasting–Water Leaching: Toward a Circular Economy for Hazardous Solid Waste from Aluminum Electrolysis

The conversion of solid waste into secondary resources has become a prerequisite for the sustainable development of the industry. This study focused on the development of the detoxification process for spent carbon cathode (SCC) without environmental pollution risks and the exploration of the recycling direction of recovered carbonaceous materials. First, the mechanism of thermodynamic conversion and decomposition of toxic substances was explored. Parameters of NaOH–Na 2 CO 3 binary molten salt roasting were optimized through an orthogonal design and a single-factor experiment, and gas release behavior during detoxification treatment was investigated. Results showed that most of the fluoride and cyanide were dissociated and decomposed, and the leaching concentration of fluoride and cyanide was as low as 7.58 and 0.12 mg/L after detoxification treatment, respectively. Then, a multistage recovery process of fluorine from fluorine-containing leachate was designed, and the comprehensive utilization of exhaust gas and the recycling of the reaction reagent were realized simultaneously. The possibility of recovering graphitized carbon blending to prepare carbon anodes was discussed in detail, and the catalytic mechanism of main impurity elements on the O 2 /CO 2 reactivity of carbon anodes was investigated via density-functional-based tight binding (DFTB). The results showed that the Boudouard reaction and carbon–O 2 reaction were affected because of the presence of Ca or Na, and the recovered graphitized carbon with a low blending ratio was more suitable for the preparation of carbon anodes. Finally, an economic benefit analysis was conducted to evaluate the industrial application potential of the proposed detoxification treatment. Compared with landfills, the proposed process reduced the disposal cost while eliminating environmental pollution risks and realized the on-site recovery and reuse of valuable components, showing considerable environmental and economic benefits.