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Sonochemical Hydrogen Production Efficiently Catalyzed by Au/TiO2
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文摘
Au/TiO2 was used as a highly efficient sonocatalyst to produce H2 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: (1) 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 of each 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 H2 evolved from methanol/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 H2 evolution, nearly half of the hydrogen atoms were nevertheless derived from water molecules. Control studies of H2 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.

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