Mingwei Yang, Maoguo Tan, Denghong Zhao, Hang Liu, Hongji Chen, Tao Liao, Jia Zeng, Yanke Jiang, Lixia Guo, Bin Sun, Heyan Jiang
Microwave pyrolysis combined with a doping strategy was adopted to precisely regulate the electronic state of carbon materials, thus constructing N-doped porous carbon material CN2 and porous O-doped carbon material CO2, which respectively realized efficient adsorption of TC and TC degradation via PMS activation. This study aims at endowing materials with differentiated functions through doping-induced electron localization/delocalization characteristics. CN2, with its large specific surface area and abundant pyrrolic N active sites formed by N doping, enhanced the π-π interaction with TC via the N-C electron localization effect. The maximum adsorption capacity reached 439 mg/g within 30 min, and kinetic and thermodynamic analyses showed that the adsorption process was dominated by chemical adsorption mediated by π-π interaction. CO2 was rich in C=O groups, and its conjugate system promoted electron delocalization, making C=O sites efficient centers for PMS adsorption and activation. The CO2/PMS system achieved 100% TC removal in 30 min, with a degradation rate constant of 0.148 min-1. DFT calculations clarified the intrinsic mechanism by which electron localization/delocalization regulated the adsorption/degradation performance of the materials. Combined with quenching experiments and EPR tests, it was verified that degradation of TC by CO2 followed a 1O2 non-radical pathway dominated by C=O sites.