Efficient elimination of organic contaminants via a non-radical pathway involving activation of sulfite by synergistic adsorption-catalysis bifunctional chitosan-modified MOF derivative

Abstract

Usually, Metal-based sulfite activation systems follow a radical generation pathway but are rare in non-radical pathways. Singlet oxygen (1O2) generation-targeted catalyst was synthesized by introducing non-redox metal oxides ZnO into chitosan-modified cobalt-zinc bimetallic oxides (CZ1.0C) via template method. Compared with Co3O4, the catalyst CZ1.0C coupled to the sulfite system (CZ1.0C/SO32-) maintained good adaptability in a common water background and a wide pH range (7–11). In addition, the CZ1.0C/SO32- system showed high efficiency in the degradation of Congo red (kobs = 0.190 min−1) and 100 % sulfite utilization. EPR, probe experiments, and DFT calculations proved the dominant role of 1O2, with a concentration three orders of magnitude higher than that of radicals. The controlled generation of non-radicals was achieved owing to the doping of ZnO and the conversion of lattice oxygen and oxygen vacancies. The catalytic oxidation intermediate HSO5- has also been demonstrated in the system, which achieves non-radical pathway oxidation through electron-mediated interactions. This article aims to develop a new “waste control by waste” strategy, which combines high selective adsorption and catalysis to achieve sulfur resource recovery and water pollutants elimination.