Guest Molecule Insertion-Optimized d-Band Center Position in MoS2 with Improved Sulfite Activation Ability Inspired by Sulfite Oxidase.

Abstract

As a prospective member in the family of advanced oxidation processes (AOPs), heterogeneous sulfite activation shows low cost and high safety for poisonous organic pollutants' degradation. To obtain an efficient sulfite activator, sulfite oxidase (SuOx), a molybdenum-based enzyme that can prompt oxidation and activation of sulfite, inspired us greatly. Based on the structure of SuOx, MoS2/BPE (BPE = 1, 2-bis-(4-pyridyl)-ethylene) is synthesized successfully. In MoS2/BPE, the BPE molecule is inserted between the MoS2 layers as a pillar and the N atom links with Mo4+ directly. MoS2/BPE shows excellent SuOx mimic activity. Theoretical calculation implies that BPE insertion optimizes the d-band center position of MoS2/BPE, which regulates the interaction between MoS2 and *SO42-. This prompts •SO4- generation and organic pollutants' degradation. At pH 7.0, its tetracycline degradation efficiency achieved is 93.9% in 30 min. Furthermore, its sulfite activation ability also endows MoS2/BPE with excellent antibiofouling performance because •SO4- can kill the microorganisms in water effectively. This work develops a new sulfite activator based on SuOx. The connection between structure and SuOx mimic activity and sulfite activation ability is clarified in detail.