The integrated system of gas-phase advanced oxidation process combined with sulfite-based wet absorption process is a desirable method for simultaneous removal of SO2, NO, and Hg0, but due to the enrichment of nitrite and Hg2+, resourcing harmless wastewater is still a challenge. To tackle this problem, this study fabricated a bifunctional β-FeOOH@MXene heterogeneous Fenton material, of which the crystalline phase, morphology, structure, and composition were revealed by using X-ray diffraction, Fourier-transform infrared spectroscopy, scanning electron microscopy-energy dispersive x-ray spectroscopy, and transmission electron microscopy. It exhibits excellent performance on nitrite oxidation (99.5%) and Hg2+ removal (99.7%) and can maintain stable outstanding ability after 13 cycles, with superior Hg2+ adsorption capacity (395 mg/g) and ultralow Fe leaching loss (<0.018 wt %). The synergism between MXene and β-FeOOH appears as follows: (i) MXene, as an inductive agent, directionally converted Fe2O3 into β-FeOOH in the hydrothermal method and greatly reduced its monomer size; (ii) the introduced ≡Ti(III)/≡Ti(II) accelerated the regeneration of ≡Fe(II) via rapid electron transfer, thereby improving the heterogeneous Fenton reaction; and (iii) MXene strongly immobilized β-FeOOH to greatly inhibit Fe-leaching. HO•, •O2--, and 1O2 were the main radicals identified by electron spin resonance. Radical quenching tests showed their contributions to NO2- oxidation in the descending order HO• > 1O2 > •O2-. Quantum chemical calculations revealed that •OH-induced oxidation of NO2- or HNO2 was the primary reaction path. Density functional theory calculations combined with X-ray photoelectron spectroscopy and Raman characterizations displayed the Hg2+ removal mechanism, with Hg2Cl2, HgCl2, and HgO as the main byproducts. This novel material provides a new strategy for resourcing harmless wastewater containing nitrite and Hg2+.
Keywords: Ti3C2-based MXene; heterogeneous Fenton; mercury; nitrite; β-FeOOH.