School of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034, China.
School of Light Industry and Chemical Engineering, Dalian Polytechnic University, Dalian, 116034, China.
Chemosphere. 2020 Apr;244:125526. doi: 10.1016/j.chemosphere.2019.125526. Epub 2019 Dec 3.
Production of sulfate radical from peroxymonosulfate (PMS) activation by carbon-based catalysts is a promising strategy to degrade pollutants. However, the electron-transfer ability of carbon catalysts, which is critical in PMS activation, still needs to be improved. In this study, a novel photo-assisted PMS activation system (PPAS) was constructed on a nitrogen-doped graphene/TiO (NG/TiO), in which the photogenerated electrons excited from TiO could be utilized by NG for enhanced PMS activation on it. Moreover, the N content was varied to firstly investigate the role of N doping on PPAS. Under photo-assistance, the NG/TiO displayed significantly enhanced PMS activation for removal of organic pollutants. 100% bisphenol A (BPA) can be removed within 1 h. The results show that the degradation kinetic constant of BPA by the NG/TiO PPAS was 24 times higher than that under PMS alone, and was 1.4 times higher than that of rGO/TiO PPAS. The singlet oxygen (O) and sulfate radical (SO) were the main reactive species in PPAS. The outstanding performance of NG/TiO system was ascribed to the two main reasons: on one hand, the N doping decreased the schottky barrier formed between NG and TiO, which favored the electron transfer from TiO to NG. On the other hand, the N doping enhanced the adsorption and electron-transfer ability of NG towards PMS.
过一硫酸盐(PMS)在碳基催化剂作用下产生硫酸根自由基,是一种很有前途的降解污染物的策略。然而,碳催化剂的电子转移能力在 PMS 活化中至关重要,仍需要进一步提高。在这项研究中,构建了一种新型的氮掺杂石墨烯/TiO(NG/TiO)光辅助过一硫酸盐活化体系(PPAS),其中 TiO 光生电子可被 NG 利用,从而增强 NG 上的 PMS 活化。此外,改变 N 含量,首先研究了 N 掺杂对 PPAS 的作用。在光辅助下,NG/TiO 对去除有机污染物具有显著增强的过一硫酸盐活化作用。100%双酚 A(BPA)可在 1 h 内完全去除。结果表明,NG/TiO PPAS 中 BPA 的降解动力学常数比单独使用 PMS 时高 24 倍,比 rGO/TiO PPAS 高 1.4 倍。单线态氧(O)和硫酸根自由基(SO)是 PPAS 中的主要活性物质。NG/TiO 体系的优异性能归因于两个主要原因:一方面,N 掺杂降低了 NG 和 TiO 之间形成的肖特基势垒,有利于电子从 TiO 转移到 NG。另一方面,N 掺杂增强了 NG 对 PMS 的吸附和电子转移能力。