g-C_(3)N_(4)/TiO_(2)纳米管阵列光阳极的制备及其光电催化降解邻氯硝基苯  

Preparation of g-C_(3)N_(4)/TiO_(2) nanotube arrays photoanode for photoelectrocatalytic degradation of o-chloronitrobenzene

作　　者：马晓明 信帅帅 张春蕾 马丙瑞 刘文婕 高孟春[1,2] MA Xiaoming;XIN Shuaishuai;ZHANG Chunlei;MA Bingrui;LIU Wenjie;GAO Mengchun(The Key Laboratory of Marine Environmental Science and Ecology,Ministry of Education,Ocean University of China,Qingdao 266100;College of Environmental Science and Engineering,Ocean University of China,Qingdao 266100)

机构地区：[1]中国海洋大学海洋环境与生态教育部重点实验室,青岛266100 [2]中国海洋大学环境科学与工程学院,青岛266100

出　　处：《环境科学学报》2022年第8期166-178,共13页Acta Scientiae Circumstantiae

基　　金：国家自然科学基金(No.21878280)。

摘　　要：采用阳极氧化-涂覆煅烧法成功制备了g-C_(3)N_(4)/TiO_(2)纳米管阵列(g-C_(3)N_(4)/TNAs)光阳极,并通过扫描电镜、X射线衍射仪、X射线光电子能谱仪、紫外可见漫反射光谱仪、光致发光光谱仪和电化学工作站等表征分析了g-C_(3)N_(4)/TNAs光阳极的形貌、晶形结构、光学特性和光电化学性能.表征结果证实,g-C_(3)N_(4)的引入通过缩小禁带宽度扩宽了TNAs的可见光响应范围,提高了光电流密度和光生电子寿命,促进了光生电子和空穴的分离.g-C_(3)N_(4)/TNAs光阳极在光电催化体系内对邻氯硝基苯(o-CNB)的降解效率高于其在光催化和电催化体系中对o-CNB的降解效率,且具有良好的稳定性和可重复性.活性物质捕获实验、电子自旋共振测试和能带结构分析表明,g-C_(3)N_(4)/TNAs光阳极中TNAs和g-C_(3)N_(4)之间存在Z型异质结相互作用机制.在光电催化体系内降解o-CNB的主要活性物质是•O_(2)^(-)、•OH和光生空穴,而光生电子是次要的活性物质.The g-C_(3)N_(4)/TiO_(2) nanotube arrays(g-C_(3)N_(4)/TNAs)photoanode was successfully prepared by the anodic oxidation and coating calcination method.The morphology,crystal structure,optical property and photoelectrochemical performance of g-C_(3)N_(4)/TNAs photoanode were analyzed through scanning electron microscopy,X-ray diffractometer,X-ray photoelectron spectrometer,ultraviolet visible diffuse reflectance spectrometer,photoluminescence spectrometer and electrochemical workstation.The characterization results proved that the introduction of g-C_(3)N_(4) broadened the visible-light response range of TNAs by narrowing the band gap width and increased the photocurrent density and photogenerated electron lifetime,which could promote the separation of photogenerated electrons and holes.The o-chloronitrobenzene(o-CNB)degradation efficiency by g-C_(3)N_(4)/TNAs photoanode in the photoelectrocatalytic system was higher than that in the photocatalytic and electrocatalytic systems.The g-C_(3)N_(4)/TNAs photoanode has good stability and repeatability.The active species capture experiment,electron spin resonance test and energy band structure analysis demonstrated the existence of Z-scheme heterojunction interaction mechanism between TNAs and g-C_(3)N_(4) in the g-C_(3)N_(4)/TNAs photoanode.The main active species for o-CNB photoelectrocatalytic degradation were•O_(2)^(-),•OH and photogenerated holes,while the photogenerated electrons were auxiliary active species.

关 键 词：邻氯硝基苯(o-CNB) 石墨相氮化碳 TiO_(2)纳米管阵列 光电催化降解 Z型异质结 

分 类 号：X703[环境科学与工程—环境工程]