Z型Cl-PhC_(2)Cu/Bi_(2)WO_(6)异质结的构建及光催化降解四环素的机制研究  

The construction of Z-scheme heterojunction of chlorine-doped copperphenylacetylene/ bismuth tungstate and the mechanism of photocatalyticdegradation of tetracycline

作　　者：张晋帆 吕文英[1] 刘国光[1] 林子力 陈颖怡 张誉丹 张广治 余宗舜 李宇琳 刘德柱 张筱昱 陈雨 ZHANG Jinfan;LÜWenying;LIU Guoguang;LIN Zili;CHEN Yingyi;ZHANG Yudan;ZHANG Guangzhi;YU Zongshun;LI Yulin;LIU Dezhu;ZHANG Xiaoyu;CHEN Yu(Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control,Guangdong-Hong Kong-Macao Joint Laboratory for Contaminants Exposure and Health,School of Environmental Science and Engineering,Guangdong University of Technology,Guangzhou 510006)

机构地区：[1]广东工业大学环境科学与工程学院,粤港澳污染物暴露与健康联合实验室,广东省环境催化与健康风险控制重点实验室,广州510006

出　　处：《环境科学学报》2024年第2期59-70,共12页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.22176042,22076029,21906029)。

摘　　要：通过简易的超声自组装方法制备了氯掺杂苯乙炔铜(PCl)/三维中空球状钨酸铋(BS)直接Z型异质结光催化材料,并通过场发射扫描电镜、傅里叶变换红外光谱、紫外-可见光漫反射光谱、X射线光电子能谱等手段对PCBS的形貌及其化学性能进行表征.结果表明,当BS与PCl的质量比为0.3时,对四环素(TC)展现出了最优异的光催化反应速率(0.3411 min^(-1)),分别是BS和PCl的2.66和4.16倍.环境影响因素(pH、不同离子、实际水体等)及循环实验结果表明,PCBS具有极大的实际应用潜力.通过淬灭实验的结果可知,超氧自由基(·O_(2)^(-))和单线态氧(^(1)O_(2))在PCBS降解TC的过程中起到了重要作用.光电化学等测试的结果表明,PCBS的光生载流子分离效率得到明显改善,能更有效率地生成活性物种,其中,PCBS产生·O_(2)^(-)的速率分别是PCl和BS的1.94和44.74倍.此外,循环伏安曲线证明了光生电子在PCBS中的迁移路径复合Z型异质结载流子迁移机制.本研究对基于苯乙炔铜的新型光催化剂开发及应用提供了理论指导和科学依据.For this work,chlorine-doped phenylacetylene copper(PCl)/three-dimensional hollow sphere bismuth tungstate(BS)direct Z-scheme heterojunction photocatalyst were prepared by simplified ultrasonic stirring technique.The morphology and chemical properties of PCBS were characterized by field emission scanning electron microscopy,Fourier transform infrared spectroscopy,ultraviolet-visible diffuse reflectance spectroscopy,and X-ray photoelectron spectroscopy.When the mass ratio of BS to PCl is 0.3,it exhibits the best photocatalytic reaction rate(0.3411 min^(-1))for tetracycline(TC),which is 2.66 and 4.16 times that of BS and PCl,respectively.In addition,the results of environmental factors(pH,different ions,actual water,etc.)and cycle experiments show that PCBS has great practical application potential.The results of quenching experiments showed that·O_(2)^(-)and singlet oxygen(^(1)O_(2))played an important role in the degradation of TC by PCBS.The results of photoelectrochemical show that the separation efficiency of photogenerated carriers of PCBS is significantly improved,and the active species can be generated more efficiently.Among them,the rate of·O_(2)^(-)production of PCBS is 1.94 and 44.74 times that of PCl and BS,respectively.In addition,the cyclic voltammetry curve proves that the migration path of photogenerated electrons in PCBS is compound with the carrier migration mechanism of Z-scheme heterojunction.This study provides theoretical guidance and scientific basis for the development and application of new photocatalysts based on phenylacetylene copper.

关 键 词：苯乙炔铜 钨酸铋 四环素 Z型异质结 光催化 

分 类 号：X703[环境科学与工程—环境工程]