Sonochemical Hydrogen Production Efficiently Catalyzed by Au/TiO2

被引:65
作者
Wang, Yifeng [1 ]
Zhao, Dan [1 ]
Ji, Hongwei [1 ]
Liu, Guilin [1 ]
Chen, Chuncheng [1 ]
Ma, Wanhong [1 ]
Zhu, Huaiyong [2 ]
Zhao, Jincai [1 ]
机构
[1] Chinese Acad Sci, Inst Chem, Beijing Natl Lab Mol Sci, Key Lab Photochem, Beijing 100080, Peoples R China
[2] Queensland Univ Technol, Sch Phys & Chem Sci, Inorgan Mat Res Program, Brisbane, Qld 4001, Australia
关键词
ENVIRONMENTAL REMEDIATION; SONOCATALYTIC DEGRADATION; ORGANIC CONTAMINANTS; OXIDATION PROCESSES; HYDROXYL RADICALS; AQUEOUS-SOLUTIONS; ISOTOPE EXCHANGE; WATER MIXTURES; GOLD; METHANOL;
D O I
10.1021/jp105691v
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
Au/TiO2 was used as a highly ellicient sonocatalyst to produce H-2 from water or aqueous solutions. Au/TiO2 significantly increased the yields of H' and 'OH radicals in the sonolysis of water. Product analysis and isotope evidence indicated that hydrogen molecules derived from methanol/water solutions were formed by three pathways: (I) recombination of two H* atoms from the cleavage of water molecules, (2) H-abstraction from methanol by H' generated by water cleavage. and (3) thermal reforming of methanol. The relative importance leach pathway was assessed by carefully analyzing the hydrogen-isotope composition of the evolved hydrogen gas using a modified gas chromatograph. The source of hydrogen in the H-2 evolved from meethanol/water solutions during sonolysis was also addressed. Data showed that, although the addition of methanol in the presence of Au/TiO2 resulted in a 12-fold increase in the rate of H-2 evolution, nearly half of the hydrogen atoms were nevertheless derived from water molecules. Control studies of H-2 formation in the presence of bare TiO2 and in the absence of a catalyst were also performed. In both cases. the compositions of evolved hydrogen gas were similar to that of the Au/TiO2 system, although hydrogen evolution was much slower. These findings reveal that Au nanoparticles on the TiO2 surface effectively catalyze water cleavage and methanol reforming.
引用
收藏
页码:17728 / 17733
页数:6
相关论文
共 40 条
[1]   Sonochemistry in environmental remediation. 1. Combinative and hybrid sonophotochemical oxidation processes for the treatment of pollutants in water [J].
Adewuyi, YG .
ENVIRONMENTAL SCIENCE & TECHNOLOGY, 2005, 39 (10) :3409-3420
[2]   Experimental solar water thermolysis [J].
Baykara, SZ .
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY, 2004, 29 (14) :1459-1469
[3]   Sonolytic, photocatalytic and sonophotocatalytic degradation of malachite green in aqueous solutions [J].
Berberidou, C. ;
Poulios, I. ;
Xekoukoulotakis, N. P. ;
Mantzavinos, D. .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2007, 74 (1-2) :63-72
[4]   Photocatalysis by Au nanoparticles: Reforming of [J].
Bowker, M ;
Millard, L ;
Greaves, J ;
James, D ;
Soares, J .
GOLD BULLETIN, 2004, 37 (3-4) :170-173
[5]  
BUTTNER J, 1991, J PHYS CHEM-US, V95, P1528
[6]   CRITICAL-REVIEW OF RATE CONSTANTS FOR REACTIONS OF HYDRATED ELECTRONS, HYDROGEN-ATOMS AND HYDROXYL RADICALS (.OH/.O-) IN AQUEOUS-SOLUTION [J].
BUXTON, GV ;
GREENSTOCK, CL ;
HELMAN, WP ;
ROSS, AB .
JOURNAL OF PHYSICAL AND CHEMICAL REFERENCE DATA, 1988, 17 (02) :513-886
[7]   SrSnO3 nanostructures:: Synthesis, characterization, and photocatalytic properties [J].
Chen, Di ;
Ye, Jinhua .
CHEMISTRY OF MATERIALS, 2007, 19 (18) :4585-4591
[8]   Visible-light-driven oxidation of organic contaminants in air with gold nanoparticle catalysts on oxide supports [J].
Chen, Xi ;
Zhu, Huai-Yong ;
Zhao, Jin-Cai ;
Zheng, Zhan-Feng ;
Gao, Xue-Ping .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2008, 47 (29) :5353-5356
[9]   Gold nanoparticles: Assembly, supramolecular chemistry, quantum-size-related properties, and applications toward biology, catalysis, and nanotechnology [J].
Daniel, MC ;
Astruc, D .
CHEMICAL REVIEWS, 2004, 104 (01) :293-346
[10]   Sonophotocatalytic destruction of organic contaminants in aqueous systems on TiO2 powders [J].
Davydov, L ;
Reddy, EP ;
France, P ;
Smirniotis, PG .
APPLIED CATALYSIS B-ENVIRONMENTAL, 2001, 32 (1-2) :95-105