Insight into the mechanisms for hexavalent chromium reduction and sulfisoxazole degradation catalyzed by graphitic carbon nitride: The Yin and Yang in the photo-assisted processes

摘要

As robust polymeric catalysts, graphitic carbon nitride (g-C3N4) has been known to have great application potential in environmental remediation. However, the mechanisms in the photo-assisted catalytic processes during the reduction or oxidation of pollutants are still difficult to discern and therefore not well studied. In this work, visible-assisted catalytic reduction of hexavalent chromium (Cr(VI)) or oxidation of sulfisoxazole (SIZ) by g-C3N4 with the addition of formic acid (FA) or potassium peroxydisulfate (PS) were systematically investigated. Effects of operation parameters such as g-C3N4 dosage, FA concentration, Cr(VI) concentration, solution pH, PS concentration were studied. The results showed g-C3N4 can be effective and robust catalyst for both the reduction (Yin) and oxidation (Yang) reactions in the environmental remediation. Mechanisms were studied by using electron spin resonance (ESR) spectroscopy. The results revealed the CO2 is the predominant radical for Cr(VI) reduction in the g-C3N4/FA/Vis system and the SO4.- and (OH)-O-. are all the main radicals for the oxidation of SIZ in the g-C3N4/PS/Vis system. The photo-generated carriers by g-C3N4, act as radical initiator, were responsible for the production of the reactive radical species in aqueous solution. This work not only shed a new light on the application of semiconductor polymers for the removal of micropollutants and also will expand the applicability of the polymeric photocatalysts for environmental remediation. (C) 2019 Elsevier Ltd. All rights reserved.