Towards a low-emission resource circulation of valuable metals from municipal solid waste incineration fly ash

The incineration fly ash (IFA) resulting from municipal solid waste combustion is laden with heavy metals, necessitating proper treatment not only for environmental management but also to reclaim the metal values. The surge in non-traditional metals like cobalt as emerging contaminant within IFA samples further attracts to address this issue. In response, the hydrometallurgical recycling of a cobalt-bearing IFA has been studied. Thereby, approximately 98 % zinc and 96 % cobalt were leached using a 1.0 mol/L H₂SO₄ solution at 90 °C and 1 h of leaching time. In-depth analysis of the leaching process unveiled metals' dissolution primarily via the ion-exclusion mechanism, as evidenced by lower diffusion coefficients (between 10^-9 and 10^-11 m²/s) and activation energies (9.6-14.9 kJ/mol). Above 99 % separation of zinc from the cobalt-bearing leach liquor was achieved by extraction with 1.0 mol/L D2EHPA at an equilibrium pH below 3.0, followed by stripping with a 2.0 mol/L H₂SO₄ solution. Cobalt, remained in the raffinate was efficiently precipitated by adding a 20 % excess dosage of oxalic acid to the stoichiometric ratio of C₂O₄^2-:Co²⁺, resulting in only 5 mg/L cobalt left in the solution when precipitation occurred at a pH of 2.8. Additionally, the conversion of CoC₂O₄ to high-purity Co₃O₄ was conducted through heat-treatment at 600 °C. The resulting Co₃O₄ was mixed with Li₂CO₃ at a Li/Co molar ratio of 1.1, yielding a LiCoO₂ precursor that exhibited good electrochemical properties with a capacity of 128 mAh/g, thus affirming the high quality of the recycled cobalt. A comprehensive life-cycle assessment of the recycling process revealed that cobalt precipitation alone contributes approximately 50 % of the total global warming potential (GWP = 4.2624 kg CO₂-eq). Notably, this value is remarkably lower than the GWP reported for primary cobalt production, highlighting the environmentally-friendly approach of this recycling endeavor.