铽负载介孔二氧化钛的制备、表征和协同效应

doi:10.3724/SP.J.1095.2014.30576

摘要/Abstract

摘要： 以嵌段共聚物P123为模板剂，采用蒸发诱导自组装法制备了铽负载介孔TiO2光催化剂，并利用XRD、N2吸附解吸和UV-Vis吸收光谱等技术手段对样品进行了表征。制备的样品为锐钛矿和金红石混合晶相，以罗丹明B为模拟有机降解物，样品显示了良好的可见光催化活性。研究发现0.7%的铽负载和380 ℃的煅烧温度是较佳的制备条件。介孔结构所具有的高的比表面积、小的晶粒尺寸、铽负载诱导的电荷分离和可见光吸收增强协同提高了光催化活性。同时，提出了铽负载二氧化钛诱导增强光催化作用的机理。

关键词: 介孔二氧化钛, 铽负载, 协同效应

Abstract: Using block copolymer P123 as the template, Tb(terbium)-loaded mesoporous TiO2 photocatalysts were prepared by the evaporation induced self-assembly method and characterized by X-ray diffraction(XRD), N2 adsorption-desorption and ultraviolet-visible(UV-Vis) absorbance spectroscopy. Tb-loaded mesoporous TiO2 with a mixture of anatase and rutile phases exhibits a high photocatalytic activity for degradation of rhodamine B(RhB) under the irradiation of visible light. It is found that 0.7% loading of Tb and 380 ℃ calcination temperature are the most appropriate preparation conditions for achieving high photocatalytic performance. The synergistic effect of high specific surface area, small crystallite size of mesoporous TiO2, Tb-induced charge-eparation and increase of visible light absorption has improved the photocatalytic activity. The mechanism of enhancement of photocatalysis in Tb loaded TiO2 is proposed.

Key words: mesoporous titanium dioxide, Tb-loaded, synergistic effect

中图分类号:

陈琪, 费霞, 何琴琴, 武其亮, 何兵, 刘雪霆. 铽负载介孔二氧化钛的制备、表征和协同效应[J]. 应用化学, DOI: 10.3724/SP.J.1095.2014.30576.

CHEN Qi, FEI Xia, HE Qinqin, WU Qiliang, HE Bing, LIU Xueting*. Synthesis, Characterization and Synergistic Effect of Tb-loaded Mesoporous Titanium Dioxide[J]. Chinese Journal of Applied Chemistry, DOI: 10.3724/SP.J.1095.2014.30576.

参考文献

[1] WANG Dianping,LIU Shouxin. Preparation of Mesoporous TiO2 Spheres via Sol-gel Assisted Hydrothermal Method Using Double Templates[J]. Chinese J Catal,2012,33(10):1681-1688.

王殿平,刘守新. 溶胶-凝胶辅助水热双模板法制备球形介孔TiO2[J]. 催化学报,2012,33(10):1681-1688.

[2] HAN Yidan,WANG Kai,XU Zhijian,et al. Preparation of Mesoporous TiO2 by Ionic Liquid Modified Sol-gel Method[J]. J Chinese Ceram Soc,2012,40(9):1289-1293.

韩一丹,王凯,徐志坚,等. 离子液体修饰溶胶-凝胶法制备介孔二氧化钛[J]. 硅酸盐学报,2012,40(9):1289-1293.

[3] ZHOU Huafeng,LIU Yuping,ZHANG Liqing,et al. Preparation and Catalytic Activity of H4SiW12O40/TiO2[J]. Chinese J Process Eng,2012,12(3):522-526(in Chinese).

周华锋,刘玉萍,张丽清，等. 介孔二氧化钛负载硅钨杂多酸的制备及其催化性能[J]. 过程工程学报,2012,12(3):522-526.

[4] TANG Shouqiang,HE Jingping,ZHANG Zhao. Synthesis and Photocatalytic Activity of Fe-doped Mesoporous TiO2 Powder[J]. J Chinese Ceram Soc,2012,40(7):950-956(in Chinese).

唐守强,何菁萍,张昭. 铁负载介孔二氧化钛的制备及其光催化性能[J]. 硅酸盐学报,2012,40(7):950-956.

[5] JIANG Chengzhi,LU Xudong. Effect of Tb3+ and Sm3+ Co-Doped on the Photocatalytic Degradation of Methylene Blue by TiO2[J]. Acta Energ Solar Sin,2011,32(12):1851-1856(in Chinese).

姜承志,卢旭东. Tb3+和Sm3+ 共负载对TiO2 降解亚甲基蓝的影响[J]. 太阳能学报,2011,32(12):1851-1856.

[6] TANG Yuchao,HUANG Xianhuai,TANG Lihua,et al. Mechanisms Research on Visible Irradiation Degradation of Organics by Nitrogen Doped TiO2 Photocatalysts[J]. Chinese J Environ Eng,2012,6(5):1585-1590(in Chinese).

唐玉朝,黄显怀,汤利华,等. N负载TiO2可见光催化降解有机物机理研究[J]. 环境工程学报,2012,6(5):1585-1590.

[7] ZOU Xing,LU Huimin,FANG Keming. Effect of Changeable Valence Rare Earth Oxides on Catalyst Properties[J]. Chinese Rare Earths,2000,21(2): 16-18(in Chinese).

邹兴,卢惠民,方克明. 变价稀土氧化物对催化剂性能的影响[J]. 稀土,2000,21(2):16-18.

[8] Turchi C S,Ollis D F. Photocatalytic Degradation of Organic Water Contaminants:Mechanisms Involving Hydroxyl Radical Attack[J]. J Catal,1990,122(1):178-192.

[9] Ismail A A,Bahnemann D W. Mesoporous Titania Photocatalysts: Preparation, Characterization and Reaction Mechanisms[J]. J Mater Chem,2011,21:11686-11707.

[10] Li F B,Li X Z,Ao C H,et al. Enhanced Photocatalytic Degradation of VOCs using Ln3+-TiO2 Catalysts for Indoor Air Purification[J]. Chemosphere,2005,59(6):787-800.

[11] Jing L,Sun X,Xin B,et al. The Preparation and Characterization of La Doped TiO2 Nanoparticles and Their Photocatalytic Activity[J]. J Solid State Chem,2004,177(10):3375-3382.

[12] Lin J,Yu J C. An Investigation on Photocatalytic Activities of Mixed TiO2-rare Earth Oxides for the Oxidation of Acetone in Air [J]. J Photochem Photobiol A:Chem,1998,116(1):63-67.

[13] Peng T,Zhao D,Dai K,et al. Synthesis of Titanium Dioxide Nanoparticles with Mesoporous Anatase Wall and High Photocatalytic Activity[J]. J Phys Chem B,2005,109(11):4947-4952.

[14] Xu A,Gao Y,Liu H. The Preparation, Characterization, and Their Photocatalytic Activities of Rare-earth-doped TiO2 Nanoparticles[J]. J Catal,2002,207(2):151-157.

[15] ZHANG Xiaoyong,CHAO Mingju,LIANG Erjun,et al. Microstructure and Photo-absorption Property of V-doped Nano-TiO2 Thin Films[J]. J Inorg Mater,2009,24(1):34-38(in Chinese).

张晓勇,晁明举,梁二军,等. 钒负载纳米TiO2薄膜的结构和光吸收性能 [J]. 无机材料学报,2009,24(1):34-38.

[16] ZHOU Huajun,WANG Dazhi,LIU Jinhua. The Photo-absorbency Effect of Size and Doping SnO2 in Nano TiO2[J]. Chinese J Chem Phys,2002,15(1):61-64(in Chinese).

周华军,王大志,刘金华. 纳米二氧化钛的量子尺寸效应及负载氧化锡对其光吸收的影响[J]. 化学物理学报,2002,15(1):61-64.

[17] Wagner C D. Handbook of X-Ray Photoelectron Spectroscopy[M]. Ed G E Muilenberg Perkin-Elmer 1979:138-139.

[18] Takizawa T,Watanabe T,Honda K. Photocatalysis Through Excitation of Adsorbates.2.A Comparative Study of Rhodamine B and Methylene Blue on Cadmium Sulfide[J]. J Phys Chem,1978,82(12):1391-1396.