| Summary: | Traditional pyrometallurgical recovery of spent lead-acid batteries (LABs) requires a temperature higher than 1000 °C, with accompanying hard-to-collect wastes such as lead dust and sulfur oxides. Against this background, sodium carbonate (Na2CO3) was proposed as a low-cost, safe, and non-toxic reagent for recycling the high-risk environmental elements lead (Pb) and sulfur (S), in spent LAB lead paste, enabling the one-step conservation of multi-component Pb species, including lead sulfate (PbSO4), metallic lead (Pb), and lead dioxide (PbO2), to lead oxide (PbO) and sodium sulfate (Na2SO4). The possible reaction pathways of Pb and S species in vacuum roasting was confirmed by Gibbs free energy reaction with an estimated average activation energy of 272.5 kJ/mol. The insoluble PbO in the reaction product (PbO/Na2SO4/Na2CO3) can be recycled by vacuum filtration, while Na2CO3 and Na2SO4 were separated using a carbonation method. Life cycle assessment revealed that for recycling 1.0 t of spent LABs, the vacuum roasting can reduce the carbon footprint −2.1 × 103 kg CO2 eq, promoting global decarbonization. The designed route is highlighted with waste-free production and is outlined by the twelve principles of green chemistry, showing its great engineering application potential for spent LAB recycling.
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