Xu Xuan, Sun Yaofang, Fan Zihong, Zhao Deqiang, Xiong Shimin, Zhang Bingyao, Zhou Shiyu, Liu Guotao
Key Laboratory of Three Gorges Reservoir Region's Eco-Environment, Ministry of Education, Chongqing University, Chongqing, China.
National Centre for International Research of Low-Carbon and Green Buildings, Chongqing University, Chongqing, China.
Front Chem. 2018 Mar 26;6:64. doi: 10.3389/fchem.2018.00064. eCollection 2018.
Many studies have focused on the use of BiVO as a photocatalyst, but few have investigated the production of free radicals during the photocatalytic process. Following synthesis of flowerlike BiVO and characterization by X-ray diffraction (XRD), Raman spectroscopy, Scanning electron microscopy (SEM) Scanning electron microscopy (EDX), UV-Vis and XPS, we successfully prepared BiVO. Then we used electron spin resonance (ESR) to determine the production and degradation of individual active free radicals, including the superoxide radical (·[Formula: see text]) and the hydroxyl radical (·OH). In the first experiment, we used ESR to detect the signals of free radicals (·[Formula: see text] and ·OH) under varying oxygen conditions. The results shown that in addition to production by ·[Formula: see text], ·OH could also be produced by oxidation of h to OH. In the next experiment, we detected ·OH under varying pH to identify the result of the first experiment, and found that signal intensities increased with increasing pH, indicating the mechanism for ·OH production. Finally, we conducted a trapping experiment to examine free radical degradation mechanisms. We identified ·OH and h as the main active free radicals and showed the complete production about ·OH. These results improve current knowledge of free radical production mechanisms, which can be used to enhance the photocatalytic performance of BiVO.
许多研究都聚焦于将BiVO用作光催化剂,但很少有研究考察光催化过程中自由基的产生情况。在合成花状BiVO并通过X射线衍射(XRD)、拉曼光谱、扫描电子显微镜(SEM)、扫描电子显微镜能谱分析(EDX)、紫外可见光谱和X射线光电子能谱(XPS)进行表征之后,我们成功制备了BiVO。然后我们使用电子自旋共振(ESR)来测定单个活性自由基的产生和降解情况,包括超氧自由基(·[化学式:见原文])和羟基自由基(·OH)。在第一个实验中,我们使用ESR检测不同氧气条件下自由基(·[化学式:见原文]和·OH)的信号。结果表明,除了由·[化学式:见原文]产生外,·OH也可由h氧化为OH产生。在接下来的实验中,我们在不同pH值下检测·OH以验证第一个实验的结果,发现信号强度随pH值升高而增加,这表明了·OH的产生机制。最后,我们进行了一个捕获实验来研究自由基降解机制。我们确定·OH和h为主要活性自由基,并展示了·OH的完整产生过程。这些结果增进了我们对自由基产生机制的现有认识,可用于提高BiVO的光催化性能。