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氮掺杂石墨烯/TiO 在光助下增强过一硫酸盐对有机污染物降解的活化作用:对 N 掺杂机制的深入了解。

Enhanced activation of peroxymonosulfate by nitrogen-doped graphene/TiO under photo-assistance for organic pollutants degradation: Insight into N doping mechanism.

机构信息

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.

出版信息

Chemosphere. 2020 Apr;244:125526. doi: 10.1016/j.chemosphere.2019.125526. Epub 2019 Dec 3.

Abstract

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.

摘要

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。

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