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为了研究锌卟啉/TiO2复合光催化剂的光催化效率及电子转移问题, 本文采用溶胶凝胶法制备了锌卟啉/TiO2的混合光催化材料, 并利用紫外可见光谱、电子顺磁共振谱对锌卟啉/TiO2复合光催化剂进行了表征与分析. 采用溶胶凝胶法制备了锌卟啉-TiO2的混合光催化材料, 通过比较纯P25型TiO2和掺入质量比分别为0.2%, 0.5%, 0.9%锌卟啉敏化剂的锌卟啉/TiO2混合光催化材料的紫外可见光谱图可知, 加入适量锌卟啉敏化剂可提高TiO2对甲基橙溶液的降解效率, 过多的掺入锌卟啉敏化剂会导致TiO2表面被敏化剂覆盖, 从而影响了其对光子的吸收, 降低TiO2的光催化效率, 降低TiO2的光降解率, 甚至低于纯TiO2的光降解率. 应用电子顺磁共振技术对锌卟啉敏化TiO2光催化剂的光催化机理进行了合理的解释, 当使用紫外可见光源对粉末样品进行辐照时, 锌卟啉受光辐照产生的激发态电子促进具有强氧化性的Ti3+和超氧根自由基的生成, 从而有效的促进了光生空穴-电子对的分离, 提高了TiO2的光催化性能.We have investigated the photocatalysis efficiency and electron transfer of the znic prophyrin/TiO2 composite photocatalyst, a sensitised hybrid porphyrin material, and prepared it successfully by sol-gel method. The UV-visible spectroscopy and electron paramagnetic resonance spectra are used to analyze and characterize the znic prophyrin/TiO2 composite photocatalyst. The proportions 0%, 0.2%, 0.5% and 0.9% (mass ratio) of zinc porphyrin, and the photocatalytic mechanism of TiO2 sensitized by zinc porphyrin are reasonably explained by ultraviolet visible spectroscopy and electron paramagnetic resonance spectroscopy (EPR). Different samples' UV-visible spectra show that the degradation efficiency of methyl orange solution by TiO2 may be improved via adding appropriate amount of zinc porphyrin sensitizer. Prohibitive incorporation of the sensitizer would cause excess of particles in the mixed catalyst, leading to the TiO2 surface covered by the sensitizer, thus affecting the absorption of photons, and the light degradation rate of TiO2 may be lowered, even lower than the pure TiO2. EPR spectra show the excited state of electrons in zinc prophyrin generated by irradiation of light can promote the generation of Ti3+ with strong oxidizing and superoxide radicals when using UV-visible light to irradiate the powder samples, thus effectively enhancing the separation of photogenerated electron-hole pairs, and improving the photocatalytic performance of TiO2.
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Keywords:
- ZnTPP /
- UV-visible spectrum /
- electronic paramagnetic resonance /
- photocatalysis
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[1] Yang K S, Dai Y, Huang B B 2007 J. Phys. Chem. C 111 12086
[2] Yang K S, Dai Y, Huang B B 2007 Phys. Rev. B 76 195201
[3] Yang K S, Dai Y, Huang B B 2009 Chem. Phys. Chem. 10 2327
[4] Cai D Y, Qiao D Y 2011 Chemistry and Adhesion 33 442 (in Chinese) [蔡冬英, 乔庆东 2011 化学与黏合 33 442]
[5] Li J Q 2006 Spectroscopy and Spectral Analysis 26 2061 (in Chinese) [李景泉 2006 光谱学与光谱分析 26 2061]
[6] Yu X Y, Liang W, Du Y J, Cheng J J 2000 Material Review 14 38 (in Chinese) [于向阳, 梁文, 杜永娟, 程继健 2000 材料导报 14 38]
[7] Zhao Z Y, Liu Q J, Zhu Z Q, Zhang J 2008 Acta Phys. Sin. 57 3760 (in Chinese) [赵宗彦, 柳淸菊, 朱忠其, 张瑾 2008 物理学报 57 3760]
[8] Fujishima A, Honda K 1972 Nature 238 37
[9] Asahi R, Morikawa T, Ohwaki T, Taga Y 2001 Science 293 269
[10] Li J Q 2006 M.S. Dissertation (Fuzhou: Fuzhou University) (in Chinese) [李景泉 2006 硕士学位论文(福州: 福州大学)]
[11] Wan Z Q, Zheng S N, Jia C Y, Yan W 2009 Acta Chim. Sin. 67 403 (in Chinese) [万中全, 郑树楠, 贾春阳, 延卫 2009 化学学报 67 403]
[12] Niu J F, Yao B H, Yu X J, Peng C, Lu L L 2013 Journal of Functional Materials 8 1132 (in Chinese) [钮金芬, 姚秉华, 余晓皎, 彭超, 鲁蕾蕾 2013 功能材料 8 1132]
[13] Yin C H, Li P X, Hou L T, Xu Z K, Wu C P, Li S B 2014 Acta Phys. Sin. 63 097201 (in Chinese) [殷春浩, 李佩欣, 侯磊田, 徐振坤, 吴彩平, 李少波 2014 物理学报 63 097201]
[14] Wu C P, Yin C H, Xu Z K, Lu L, Li P X, Li S B 2014 Journal of Synthetic Crystals 43 937 (in Chinese) [吴彩平, 殷春浩, 徐振坤, 路璐, 李佩欣, 李少波 2014 人工晶体学报 43 937]
[15] Yin C H, Li S B, Wu C P, Xu Z K, Shen G, Li P X 2014 Journal of Synthetic Crystals 43 2062 (in Chinese) [殷春浩, 李少波, 吴彩平, 徐振坤, 神干, 李佩欣 2014 人工晶体学报 43 2062]
[16] Liu S X, Sun C L 2004 Acta. Phys. Chim. Sin. 20 355 (in Chinese) [刘守新, 孙承林 2004 物理化学学报 20 355]
[17] Shen G 2012 M.S. Dissertation (Xuzhou: China University of Mining and Technology) (in Chinese) [神干 2012 士学位论文 (徐州:中国矿业大学)]
[18] Chong S V, Xia J, Suresh N, Yamaki K, Kadowaki K 2008 Solid State Commun. 148 345
[19] Song X Y, Miao J P, Li L P, Su W H 2000 Chinese Journal of High Pressure Physics 14 37 (in Chinese) [宋小羽, 苗继鹏, 李莉萍, 苏文辉 2000 高压物理学报 14 37]
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