Surface Chemical Regulation of Coal Gangue–Rice Husk Biochar for Concurrent Promotion of Hg²⁺ Adsorption and Inhibition of Hg⁰ Production

Mercury (Hg) is a global pollutant that poses a serious threat to ecosystems and human health. Biochar has shown great potential for mercury removal due to its porous structure and abundant surface functional groups. However, redox-active moieties on biochar can reduce adsorbed Hg²⁺ to volatile Hg⁰, leading to secondary mercury dispersion. To suppress this reduction, this study proposes a strategy of co-pyrolyzing coal gangue with rice husk to prepare composite biochars (RHB/CG), leveraging the abundant metal oxides in coal gangue to tailor the surface chemistry of biochar. The materials were characterized by FTIR, Raman, and XRD; static adsorption, mercury speciation analysis, and kinetic experiments were conducted. The results show that coal gangue incorporation significantly enhances the Hg²⁺ adsorption capacity of biochar, with the equilibrium adsorption capacity calculated by the pseudo-second-order kinetic model, increasing from 20.6 mg/g for pristine RHB to 38.7 mg/g for RHB/CG-1:1. More importantly, RHB/CG composites effectively suppress the reduction of Hg²⁺ to Hg⁰, and the amount of Hg⁰ accumulated in the system is 57.1% lower than that of pristine RHB. Mechanistic studies reveal that coal-gangue-derived basic functional groups (e.g., C–O–C, Si–O–M) inhibit reduction via sequestering Hg²⁺ through coordination and disruption of electron transfer pathways. PHREEQC simulations (pe = 6.0) confirm the decreased tendency of Hg²⁺ reduction to Hg⁰ with increasing pH, in good agreement with the experimental results showing reduced Hg²⁺ reduction. The corresponding results provide a green and sustainable solution for mercury-contaminated water and soil remediation.