摘要
本文采用浸渍法制备了石墨相氮化碳改性TiO_(2)纳米管阵列的复合光电极(g-C_(3)N_(4)/TNAs),对复合光电极的晶型结构、形貌和元素价态进行了表征。利用紫外可见漫反射光谱、光致发光光谱和电化学工作站评价了g-C_(3)N_(4)/TNAs的光电化学性能。在施加1.5 V偏压和可见光照射下,评价了g-C_(3)N_(4)/TNAs对间氯硝基苯(m-chloronitrobenzene,m-CNB)的光电催化降解性能。结果表明,g-C_(3)N_(4)的负载拓宽了TNAs的光吸收范围,促进了光生载流子的分离。相较于其它光电极,以浸渍液g-C_(3)N_(4)浓度为300 mg·L^(-1)时制备的g-C_(3)N_(4)-300/TNAs具有较好的光电化学性能和较高的光电催化m-CNB的性能。此外,g-C_(3)N_(4)-300/TNAs在光电催化降解m-CNB过程中具有良好的可重复使用性和稳定性。自由基捕获实验和电子顺磁共振光谱表明·OH、·O^(-)_(2)和h^(+)是g-C_(3)N_(4)/TNAs光电催化降解m-CNB的主要活性物质,g-C_(3)N_(4)和TNAs形成的异质结符合Z型电荷转移机制。
The graphitic carbon nitride modified TiO_(2) nanotube arrays(g-C_(3)N_(4)/TNAs) composite photoelectrode was prepared by impregnation method.The crystal structure,morphology and elemental valence state of as-prepared photoelectrodes were characterized.The photoelectrochemical properties of g-C_(3)N_(4)/TNAs were evaluated by UV-Vis diffuse reflectance spectroscopy,photoluminescence spectroscopy and electrochemical workstation.The photoelectrocatalytic performance of g-C_(3)N_(4)/TNAs for m-chloronitrobenzene(m-CNB) degradation was investigated under bias voltage of 1.5 V and visible light irradiation.The experimental results showed that the load of g-C_(3)N_(4) broadened the light absorption range and promoted photocarriers separation of TNAs.Compared with other photoelectrodes,g-C_(3)N_(4)-300/TNAs photoelectrode prepared at g-C_(3)N_(4) concentration of 300 mg·L^(-1) had better photoelectrochemical properties and higher photoelectrocatalytic performance for m-CNB degradation.Additionally,g-C_(3)N_(4)-300/TNAs had good reusability and stability during the photoelectrocatalytic degradation process of m-CNB.Free radical trapping experiments and electron paramagnetic resonance spectra demonstrated that ·OH,·O^(-)_(2) and h^(+) were the main active species for the photoelectrocatalytic degradation of m-CNB by g-C_(3)N_(4)-300/TNAs.The heterojunction between g-C_(3)N_(4) and TNAs conformed to the Z-type charge transfer mechanism.
作者
张春蕾
信帅帅
王旭
霍思月
马晓明
刘文婕
高孟春
Zhang Chunlei;Xin Shuaishuai;Wang Xu;Huo Siyue;Ma Xiaoming;Liu Wenjie;Gao Mengchun(The Key Laboratory of Marine Environmental Science and Ecology,Ministry of Education,Qingdao 266100,China;Qingdao Sagegroup Environmental PingDu Sewage Treatment Company Limited,Qingdao 266706,China)
出处
《中国海洋大学学报（自然科学版）》
CAS
CSCD
北大核心
2023年第4期54-66,共13页
Periodical of Ocean University of China
基金
国家自然科学基金项目(21878280)资助。
