Enhanced Heterogeneous Activation of Peroxymonosulfate by Nitrogen–Sulfur Co-Doped Mofs-Derived Carbon

Abstract

It is important to further enhance the performance of green and efficient non-homogeneous catalysts for advanced oxidation process of Peroxymonosulfate (PMS-AOP) for green treatment of industrial wastewater. In this paper, nitrogen–sulfur co-doped MOFs-derived carbon material (CoSN@C) was prepared by one-pot synthesis followed by carbonization, and its morphological structure was characterized by XRD and SEM. After pyrolysis, the CoSN@C still maintained the dodecahedral morphology and structure of ZIF-67. The synergistic effects of S and N significantly elevated the activation of PMS. The results show that the CoSN@C + PMS system can effectively activate PMS to degrade Rhodamine B (RhB), with a rate constant (1.85 min−1) four times higher than that of the CoN@C + PMS system (0.44 min−1). The optimal catalytic process parameters of material dosage, PMS concentration, temperature, pH, and other parameters were also investigated for the activation of PMS to remove Rhodamine B. The cyclic experiment shows that the CoSN@C has excellent recyclability and the degradation rate of RhB still reached 88.9% after four cycles. Radical capture experiments and EPR tests showed that the CoSN@C + PMS system generated a large amount of SO4·− and ·OH radicals adsorbed on the catalyst surface and a certain amount of singlet oxygen, and the free radical pathway and non-radical pathway worked together to degrade RhB efficiently and rapidly. While non-radical pathway with singlet oxygen as main reactive oxygen species played a key role in the CoN@C + PMS system. This work provides a new idea for the rational design of non-homogeneous catalysts for PMS-AOP system.