Polychloride and benzene ring synergistically boosting photocatalytic degradation and nitrogen fixation performances of carbon nitride

Abstract

The limited active site exposure, insufficient light absorption and poor charge behavior of carbon nitride (CN) limit its application in environmental remediation and clean energy production. In this study, ultrathin porous CN with enhanced photocatalytic activity was constructed by doping 2,2′,5,5′-Tetrachlorobenzidine (TB) into CN framework. The synergistic effect of polychloride and benzene rings on CN leads to the significant enhancement of range/intensity of visible-light harvest and charge behavior, as well as specific surface area. The optimal sample achieves 100% tetracycline photodegradation efficiency with a rate constant approximately 9 times of pristine CN, and total organic carbon removal efficiency reaches 78.2%. Moreover, photocatalytic ammonia production rate is 7 times of pristine CN. Through active species trapping experiments, ESR, LC-MS, toxicity prediction and DFT calculations, the main active species, degradation pathway, intermediates toxicity and enhanced mechanism of photocatalytic activity are investigated. This work provides a reference for simultaneously regulating the morphology, light absorption and charge behavior of CN-based photocatalyst for addressing environmental and energy concerns.