Size and structure-dependent photocatalytic activity of jingle-bell-shaped silica-coated cadmium sulfide nanoparticles for methanol dehydrogenation

被引:48
作者
Pal, B
Torimoto, T
Iwasaki, K
Shibayama, T
Takahashi, H
Ohtani, B [1 ]
机构
[1] Hokkaido Univ, Catalysis Res Ctr, Sapporo, Hokkaido 0010021, Japan
[2] Hokkaido Univ, Grad Sch Environm Earth Sci, Sapporo, Hokkaido 0600811, Japan
[3] Hokkaido Univ, Ctr Adv Res Energy Technol, Sapporo, Hokkaido 0608628, Japan
关键词
D O I
10.1021/jp046445h
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
Silica-coated cadmium sulfide nanoparticles (SiO2/CdS) having a jingle-bell structure were prepared via size-selective photoetching and were used as photocatalysts for dehydrogenation of methanol. Irradiation Of SiO2/ CdS suspended in an aqueous solution containing methanol induced the liberation of hydrogen (1-12), the amount of which increased linearly with increase in the time of irradiation. The observed stable photocatalytic activity was attributed to the prevention of coalescence between CdS core particles by the surrounding SiO2 shells during the photocatalytic reaction. The rate of H, liberation increased with decrease in the wavelength of irradiation light for the size-selective photoetching, that is, the smaller the size of the CdS core, the higher the rate of H-2 liberation, probably because of increased reduction and oxidation abilities of CdS as a result of decrease in their particle size, that is, size quantization effect. Rhodium photodeposited on SiO2/CdS worked as a cocatalyst for the enhancement of dehydrogenation. The photocatalytic activity was reduced by increase in shell thickness because of a decrease in the rate of penetration of chemical species or the transfer of electrons and holes through the SiO2 layer. Also, the close contact between the core and shell retarded the photocatalytic reaction, indicating that the surface of the CdS core for methanol dehydrogenation was covered with a SiO2 shell layer. The results indicate that the jingle-bell-shaped SiO2/CdS nanoparticles can be an efficient and stable photocatalyst with a flexibly tunable structure, in contrast to s urface- modified CdS particles prepared by a conventional technique.
引用
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页码:18670 / 18674
页数:5
相关论文
共 26 条
[1]  
[Anonymous], 2004, NANOPARTICLES
[2]   ULTRAVIOLET VISIBLE ABSORPTION-SPECTRA OF THE COLLOIDAL METALLIC ELEMENTS [J].
CREIGHTON, JA ;
EADON, DG .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1991, 87 (24) :3881-3891
[3]   PHOTOCATALYTIC PRODUCTION OF H2O2 AND ORGANIC PEROXIDES ON QUANTUM-SIZED SEMICONDUCTOR COLLOIDS [J].
HOFFMAN, AJ ;
CARRAWAY, ER ;
HOFFMANN, MR .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 1994, 28 (05) :776-785
[4]   ENVIRONMENTAL APPLICATIONS OF SEMICONDUCTOR PHOTOCATALYSIS [J].
HOFFMANN, MR ;
MARTIN, ST ;
CHOI, WY ;
BAHNEMANN, DW .
CHEMICAL REVIEWS, 1995, 95 (01) :69-96
[5]   EFFECTS OF SIZE QUANTIZATION OF ZINC-SULFIDE MICROCRYSTALLITES ON PHOTOCATALYTIC REDUCTION OF CARBON-DIOXIDE [J].
INOUE, H ;
TORIMOTO, T ;
SAKATA, T ;
MORI, H ;
YONEYAMA, H .
CHEMISTRY LETTERS, 1990, (09) :1483-1486
[6]   Preparation and characterization of water-soluble jingle-bell-shaped silica-coated cadmium sulfide nanoparticles [J].
Iwasaki, K ;
Torimoto, T ;
Shibayama, T ;
Takahashi, H ;
Ohtani, B .
JOURNAL OF PHYSICAL CHEMISTRY B, 2004, 108 (32) :11946-11952
[7]   Nanoparticles in advanced oxidation processes [J].
Kamat, PV ;
Meisel, D .
CURRENT OPINION IN COLLOID & INTERFACE SCIENCE, 2002, 7 (5-6) :282-287
[8]   Quantum confinement effects enable photocatalyzed nitrate reduction at neutral pH using CdS nanocrystals [J].
Korgel, BA ;
Monbouquette, HG .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (25) :5010-5017
[9]   PHOTOINDUCED REDUCTION OF VIOLOGENS ON SIZE-SEPARATED CDS NANOCRYSTALS [J].
MATSUMOTO, H ;
UCHIDA, H ;
MATSUNAGA, T ;
TANAKA, K ;
SAKATA, T ;
MORI, H ;
YONEYAMA, H .
JOURNAL OF PHYSICAL CHEMISTRY, 1994, 98 (44) :11549-11556
[10]   An overview of semiconductor photocatalysis [J].
Mills, A ;
LeHunte, S .
JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY, 1997, 108 (01) :1-35