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CH3O·引发的溴酸盐还原机制探究
引用本文:郭少华,蓝梅,兰华春,李曈,张弓.CH3O·引发的溴酸盐还原机制探究[J].环境科学学报,2018,38(9):3630-3635.
作者姓名:郭少华  蓝梅  兰华春  李曈  张弓
作者单位:河北工程大学能源与环境工程学院;清华大学环境学院;中国科学院生态环境研究中心饮用水科学与技术重点实验室
基金项目:国家自然科学基金(No.51722811)
摘    要:针对溴酸盐(BrO-3)污染,本研究以三聚氰胺为前驱体制备石墨相氮化碳(g-C3N4)为自由基诱导催化材料.通过XRD、TEM、UV/Vis-DRS对其物相组成和光催化性能进行表征发现,制备的层状g-C3N4有稳定片层结构及可见光响应的禁带宽度(~2.70 e V).可见光照射下,g-C3N4表面产生的光生载流子不能直接还原溴酸盐.然而,若有有机小分子(如甲醇)存在,光催化还原效率迅速增大.通过原位电子顺磁共振谱(EPR)及对材料表面的光电化学测试分析,我们探索了该体系的光催化还原Br O-3的机制.结果表明,g-C3N4带隙较窄其空穴氧化能力较弱,在光催化过程中空穴只能将甲醇分子转化为CH3O·自由基,因而甲醇分子的存在提升了光生载流子的分离效率,加剧了自由基的累积.该自由基具有较高的还原活性,可迅速将水相中的溴酸根还原至溴离子.

关 键 词:g-C3N4  可见光催化  溴酸盐  反应机制  CH3
收稿时间:2018/2/4 0:00:00
修稿时间:2018/2/27 0:00:00

The bromate reduction induced by CH3
GUO Shaohu,LAN Mei,LAN Huachun,LI Tong and ZHANG Gong.The bromate reduction induced by CH3O·[J].Acta Scientiae Circumstantiae,2018,38(9):3630-3635.
Authors:GUO Shaohu  LAN Mei  LAN Huachun  LI Tong and ZHANG Gong
Institution:1. College of Energy and Environmental Engineering, Hebei University of Engineering, Handan 056038;2. School of Environment, Tsinghua University, Beijing 100084;3. China Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085,College of Energy and Environmental Engineering, Hebei University of Engineering, Handan 056038,School of Environment, Tsinghua University, Beijing 100084,China Key Laboratory of Drinking Water Science and Technology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085 and School of Environment, Tsinghua University, Beijing 100084
Abstract:we herein prepared the graphitic-C3N4 (g-C3N4) materials using melamine as precursors by a pyrolysis approach. Based on characterization XRD, TEM and UV/Vis-DRS, it was found that the layered ha stable laminar structure the gap width of visible light response~2.70 eV. Under visible light, the g-C3N4 photocatalyst exhibited the inferior photocatalytic reduction of bromate (BrO3-), while the reduction efficiency increased rapidly after the addition of organic (methanol). in-situ electron paramagnetic resonance (EPR) and photoelectrochemical analysisThe results demonstrate that the narrow g-C3N4 band gap weaken the hole oxidation ability, thereby only transfer the methanol into methanol free radicals (CH3O·) in the process of photocatalysishus the presence of methanol the separation efficiency of the photogenerated electron-hole pairs, the accumulation of free radicals. In viewing of the superior reduction ability, the in-situ generated CH3O· with high concentration the high BrO3- removal performance.
Keywords:g-C3N4  visible-light photocatalysis  bromate  reaction mechanism  CH3
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