Gold Nanoparticles on Mesoporous Interparticle Networks of Titanium Dioxide Nanocrystals for Enhanced Photonic Efficiencies

被引:174
作者
Ismail, Adel A. [1 ,2 ]
Bahnemann, Detlef W. [1 ,2 ]
Bannat, Inga [2 ,3 ]
Wark, Michael [2 ,3 ]
机构
[1] Leibniz Univ Hannover, Inst Tech Chem, D-30167 Hannover, Germany
[2] Leibniz Univ Hannover, ZFM, D-30167 Hannover, Germany
[3] Leibniz Univ Hannover, Inst Phys Chem & Elektrochem, D-30167 Hannover, Germany
关键词
PHOTOCATALYTIC ACTIVITY; QUANTUM YIELDS; HETEROGENEOUS PHOTOCATALYSIS; FORMALDEHYDE FORMATION; HYDROGEN-PRODUCTION; CHARGE-DISTRIBUTION; TIO2; NANOCOMPOSITES; OXIDATION; SILICA;
D O I
10.1021/jp900766g
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Nanocomposites consisting of Au and TiO2 nanocrystals have been synthesized through simple one-step sol-gel reactions of titanium tetraisopropoxide with hydrogen tetrachloroaurate in the presence of an F127 triblock copolymer as the template to direct the formation of nanostructured photocatalysts. The thus formed Au/TiO2 network gels were calcined at 500 degrees C for 4 h, leading to Au/TiO2 nanocomposites with high interparticle mesoporosity, pore diameters of around 10 nm, and BET surface areas of about 100 m(2)/g. TEM investigations of 0.5 wt % Au/TiO2 reveal that the TiO2 particles are quite uniform in size and shape. The particle sizes of TiO2 and Au are in the range of 5-10 and 20-120 nm, respectively. The photocatalytic methanol oxidation to formaldehyde chosen as the test reaction to examine the photocatalytic activity of the Au/TiO2 was shown to be more effective as compared with pure TiO2 and with Degussa P25, respectively. The increased photocatalytic activity of Au/TiO2 with interparticle mesopores is attributed to a higher intrinsic activity of the Au/TiO2 and improved intrinsic electron diffusion. The latter effect is explained by considering the mesoporous TiO2 network to behave like an antenna system for the photogenerated electrons, enabling them to reach the respective TiO2/Au contacts with high probability. Thus, a few Au particles in electronic contact with the entire TiO2 structure are sufficient to act as efficient electron relays, enabling the charge transfer to the solutes. The sample 0.5 wt % Au/TiO2 nanocrystals with smaller Au nanoparticles is therefore more photoactive than those composed of larger Au particles and hence less semiconductor/metal contacts.
引用
收藏
页码:7429 / 7435
页数:7
相关论文
共 65 条
[61]   Structural and electronic properties of Au on TiO2(110) [J].
Yang, ZX ;
Wu, RQ ;
Goodman, DW .
PHYSICAL REVIEW B, 2000, 61 (20) :14066-14071
[62]   Understanding polymorphic phase transformation behavior during growth of nanocrystalline aggregates:: Insights from TiO2 [J].
Zhang, HZ ;
Banfield, JF .
JOURNAL OF PHYSICAL CHEMISTRY B, 2000, 104 (15) :3481-3487
[63]   Thermodynamic analysis of phase stability of nanocrystalline titania [J].
Zhang, HZ ;
Banfield, JF .
JOURNAL OF MATERIALS CHEMISTRY, 1998, 8 (09) :2073-2076
[64]   Mesoporous structure and phase transition of nanocrystalline TiO2 [J].
Zhang, YH ;
Weidenkaff, A ;
Reller, A .
MATERIALS LETTERS, 2002, 54 (5-6) :375-381
[65]   Synthesis of mesoporous titanium dioxide materials by using a mixture of organic compounds as a non-surfactant template [J].
Zheng, JY ;
Pang, JB ;
Qiu, KY ;
Wei, Y .
JOURNAL OF MATERIALS CHEMISTRY, 2001, 11 (12) :3367-3372