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g-C3N4在可见光下协同PDS降解磺胺二甲嘧啶的机制研究
引用本文:张钱新,陈平,王枫亮,曾泳钦,苏跃涵,吕文英,姚琨,刘海津,刘国光. g-C3N4在可见光下协同PDS降解磺胺二甲嘧啶的机制研究[J]. 环境科学学报, 2017, 37(10): 3772-3779
作者姓名:张钱新  陈平  王枫亮  曾泳钦  苏跃涵  吕文英  姚琨  刘海津  刘国光
作者单位:广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,广东工业大学环境科学与工程学院, 广州 510006,河南师范大学化学与环境科学学院, 新乡 453007,广东工业大学环境科学与工程学院, 广州 510006
基金项目:国家自然科学基金(No. 21377031,21677040);广东省自然科学基金(No.2016A030313697);河南省教育厅项目(No.13A610528)
摘    要:以二聚氰胺为前驱体合成光催化剂石墨相碳化氮(g-C_3N_4),通过透射电子显微镜(TEM)、X射线衍射(XRD)和紫外可见漫反射光谱(UV-vis DRS)等技术对g-C_3N_4材料进行形貌结构和光学性能的表征.实验过程中,以g-C_3N_4光催化降解磺胺二甲嘧啶(SMZ)中,加入过硫酸盐(PDS)联合效果的研究结果表明,PDS加快了g-C_3N_4对SMZ的光催化降解;通过荧光测试,表明了PDS使g-C_3N_4的光生空穴(h~+)与光生电子(e-)能够进行有效地分离,从而加强其光催化性能;实验同时研究了PDS/g-C_3N_4体系对磺胺二甲嘧啶(SMZ)光催化降解的影响机制.研究表明,SMZ的光催化降解反应符合准一级动力学规律;pH在酸性环境下有利于SMZ的降解;使用草酸钠作为光生空穴分子捕获剂,检测到h~+存在于PDS/g-C_3N_4光催化体系中,并计算得出h~+的贡献率为65.9%,表明h~+在降解中起到主要作用;TOC的检测表明,加入PDS有助于SMZ的矿化.

关 键 词:g-C3N4  过硫酸盐PDS  磺胺二甲嘧啶  空穴
收稿时间:2017-03-16
修稿时间:2017-05-14

Photocatalytic degradation mechanism of sulfamethazine using PDS/g-C3N4 under visible light irradiation
ZHANG Qianxin,CHEN Ping,WANG Fengliang,ZENG Yongqin,SU Yuehan,L,#; Wenying,YAO Kun,LIU Haijin and LIU Guoguang. Photocatalytic degradation mechanism of sulfamethazine using PDS/g-C3N4 under visible light irradiation[J]. Acta Scientiae Circumstantiae, 2017, 37(10): 3772-3779
Authors:ZHANG Qianxin,CHEN Ping,WANG Fengliang,ZENG Yongqin,SU Yuehan,L&#   Wenying,YAO Kun,LIU Haijin  LIU Guoguang
Affiliation:School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006,School of Chemistry and Environmental Science, Henan Normal University, Xinxiang 453007 and School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006
Abstract:Graphite phase C3N4 (g-C3N4) was synthesized using dicyandiamide as the precursor. The morphology and optical properties of g-C3N4 were characterized by transmission electron microscopy (TEM), X-ray diffraction (XRD) and UV-visible diffuse reflection (UV-vis DRS). In this study, the effect of the addition of persulfate (PDS) on the degradation of sulfamethazine (SMZ) by g-C3N4 photocatalytic degradation was studied. The results showed that PDS enhanced the photocatalytic degradation of SMZ by g-C3N4. The fluorescence test showed that PDS could effectively separate the photogenerated hole (h+) and photogenerated electron (e-) from g-C3N4 to enhance its photocatalytic performance. The different factors of PDS/g-C3N4 system on the photocatalytic degradation of sulfadimidine (SMZ) was also investigated. The degradation of SMZ followed pseudo-first-order kinetics. Acidic condition is conductive to the degradation of SMZ. Quenching experiment demonstrated that h+ was present in the PDS/g-C3N4 photocatalytic system using sodium oxalate as photogenerated scavenger, and the contribution of h+ was calculated to be 65.9%. This result indicated the major role of h+ in degradation of SMZ. The detection of total organic carbon (TOC) indicated that the addition of PDS enhanced the mineralization of SMZ.
Keywords:g-C3N4  peroxydisumphate (PDS)  sulfamethazine  hole (h+)
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