Arsenic-calcium residue (ACR) is a hazardous solid waste generated by the metallurgical industry, posing a significant environmental risk. However, the stability and transformation behavior of ACR in sulfidic conditions remains unclear. Herein, we have investigated the stability and speciation evolution of arsenic (As), sulfur (S), and trace metals during the exposure of ACR to diverse S(-II) concentrations under anoxic conditions at pH of 6 and 11. Our results indicate that environmentally relevant levels of S(-II) (i.e., 1, 10, and 50 mM) significantly enhance the mobilization of As(III) and Cd from ACR, with greater release at pH 6. The main mechanism for the release of As(III) and trace metals from ACR is the reductive dissolution of Ca-arsenate/arsenite and As-trace metals-gypsum. The reductive dissolution of As-trace metals-gypsum leads to the formation of SO and SO. XRD, FE-SEM, FTIR, XPS, and HRTEM analyses reveal that gypsum serves as the host phase for As fixation at pH 6, while calcium-arsenate/arsenite phases predominate at pH 11. Secondary AsS, CdS, CuS, and symplesite are generated at pH 6, whereas parasymplesite, CdS, and CuS are predominant at pH 11. These results enhance our understanding of the environmental behavior of As, S, and trace metals associated with ACR.
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