Cai Tiejun, Liao Yuchao, Peng Zhenshan, Long Yunfei, Wei Zongyuan, Deng Qian
College of Chemistry & Chemical Engineering, Hunan University of Science & Technology, Xiangtan 411201, China.
J Environ Sci (China). 2009;21(7):997-1004. doi: 10.1016/s1001-0742(08)62374-8.
The binary composite photo-catalysts CeO2/TiO2, ZrO2/TiO2 and the ternary composite photo-catalysts H3PW12O40-CeO2/TiO2, H3PW12O40-ZrO2/TiO2 were prepared by sol-gel method. The catalysts were characterized by thermogravimetric-differential thermal analysis (TG-DTA), scanning electron microscopy (SEM) and X-ray diffraction (XRD). The photocatalytic elimination of methanol was used as model reaction to evaluate the photocatalytic activity of the composite catalysts under ultraviolet light irradiation. The effects of doped content, activation temperature, time, initial concentration of methanol and gas flow rate on the catalytic activity were investigated. The results showed that after doping a certain amount of CeO2 and ZrO2, crystallization process of TiO2 was restrained, particles of catalysts are smaller and more uniform. Doping ZrO2 not only significantly improved the catalytic activity, but also increased thermal stability. Doping H3PW12O40 also enhanced the catalytic activity. The catalytic activities of binary and ternary composite photocatalysts were significantly higher than un-doped TiO2. The dynamics law of photocatalytic reaction over the binary CeO2/TiO2 and ZrO2/TiO2 catalysts has been studied. The activation energy 15.627 and 15.631 kJ/mol and pre-exponential factors 0.5176 and 0.9899 s(-1) over each corresponding catalyst were obtained. This reaction accords to the first order dynamics law.
采用溶胶-凝胶法制备了二元复合光催化剂CeO2/TiO2、ZrO2/TiO2以及三元复合光催化剂H3PW12O40-CeO2/TiO2、H3PW12O40-ZrO2/TiO2。通过热重-差热分析(TG-DTA)、扫描电子显微镜(SEM)和X射线衍射(XRD)对催化剂进行了表征。以光催化消除甲醇作为模型反应,评价复合催化剂在紫外光照射下的光催化活性。考察了掺杂量、活化温度、时间、甲醇初始浓度和气体流速对催化活性的影响。结果表明,掺杂一定量的CeO2和ZrO2后,TiO2的结晶过程受到抑制,催化剂颗粒更小且更均匀。掺杂ZrO2不仅显著提高了催化活性,还提高了热稳定性。掺杂H3PW12O40也增强了催化活性。二元和三元复合光催化剂的催化活性明显高于未掺杂的TiO2。研究了二元CeO2/TiO2和ZrO2/TiO2催化剂上光催化反应的动力学规律。得到了各相应催化剂上的活化能15.627和15.631 kJ/mol以及指前因子0.5176和0.9899 s(-1)。该反应符合一级动力学规律。