化学学报 ›› 2010, Vol. 68 ›› Issue (03): 211-216. 上一篇    下一篇

研究论文

Ce掺杂K2La2Ti3O10催化剂的可见光高效催化制氢的研究

刘利1,崔文权*,1,梁英华1,邱发礼2   

  1. (1河北理工大学化工与生物技术学院 唐山 063009)
    (2中国科学院成都有机化学研究所 成都 610041)
  • 投稿日期:2009-08-08 修回日期:2009-10-17 发布日期:2010-02-20
  • 通讯作者: 崔文权 E-mail:wkcui@163.com
  • 基金资助:

    唐山市海洋重点实验室(No. 08360204A-3)

Efficiently Photocatalytic Hydrogen Evolution over Ce-doped K2La2Ti3O10 under Visible Light Irradiation

Liu Li1 Cui Wenquan*,1 Liang Yinghua1 Qiu Fali2   

  1. (1 College of Chemical Engineering and Biological Technology, Hebei Polytechnic University, Tangshan 063009)
    (2 Chengdu Institute of Organic Chemistry, Chinese Academy of Sciences, Chengdu 610041)
  • Received:2009-08-08 Revised:2009-10-17 Published:2010-02-20
  • Contact: CUI Wen-Quan E-mail:wkcui@163.com

采用高温固相法合成了铈掺杂的K2La2Ti3O10催化剂, 利用X射线衍射(XRD)、紫外-可见漫反射(UV-vis DRS)、透射电镜(TEM)和X射线光电子能谱(XPS)对催化剂进行了表征. 考察了催化剂的可见光催化分解甲醇水溶液制氢的活性, 并对可见光催化机理进行了分析. 研究表明, 铈的掺杂没有改变K2La2Ti3O10的微晶结构, 并使催化剂粒径有所减小. 紫外可见漫反射分析表明禁带宽度为2.3 eV左右, 对可见光具有较高吸收. XPS表明La和Ti为+3和+4价, 而Ce则是+3和+4的混合价态. 担载2 wt% Pt后, 在可见光下光催化活性大大提高, 当铈的掺杂量为0.5 mol%(即Ce取代La的摩尔百分量)时, 光催化活性达到最大, 产氢速率为0.05 mmol/h; 光照5 h后产氢量为0.22 mmol, 而纯K2La2Ti3O10的产氢量只有0.037 mmol.

关键词: 光催化, Ce掺杂, K2La2Ti3O10, 可见光, 制氢

Ce-doped K2La2Ti3O10 was prepared by a high temperature solid state reaction, and characterized by XRD, UV-Vis DRS, TEM and XPS. The photocatalytic activities of the Ce-doped K2La2Ti3O10 and pure K2La2Ti3O10 catalysts for hydrogen evolution were examined under visible light irradiation. The results showed that the Ce ion entered the crystal lattice of K2La2Ti3O10, and Ce doping resulted in the small size of particle. The Ce-doped K2La2Ti3O10 powder shifted the UV absorption band of K2La2Ti3O10 toward visible light region. According to the investigation of XPS, La and Ti exist mainly in the forms of +3 and +4 valences, respectively. The Ce 3d XPS basically denotes the mixture of Ce4+/3+ oxidation states giving rise to a myriad of peaks. The Ce-doped K2La2Ti3O10 shows a higher activity than K2La2Ti3O10 under visible light irradiation after they were loaded with 2 wt% Pt as co-catalysts. The highest activity was obtained with 0.05 mmol/h when K2La2Ti3O10 doped at 0.5 mol% of Ce ion to La; and after 5 h illumination, the amount of hydrogen production was got to 0.22 mmol, while that value of pure K2La2Ti3O10 was only 0.037 mmol.

Key words: photocatalysis, Ce doping, K2La2Ti3O10, visible light, hydrogen production