Disintegration or redispersion of supported sintered gold nanoparticles （Au NPs） in the presence of alkyl halide can give catalyst regeneration or redispersion of sintered Au catalysts. The selectivity of alkyl hali...Disintegration or redispersion of supported sintered gold nanoparticles （Au NPs） in the presence of alkyl halide can give catalyst regeneration or redispersion of sintered Au catalysts. The selectivity of alkyl halides, temperature and size distributions were investigated to elucidate the redispersion of Au NPs during halide-induced decomposition. This study proved that the alkyl halide induced the redispersion of sintered Au NPs which depended on the R-X （X = I, Br, CI） bond dissociation energy （BDE） and thus provided a simple descriptor for the regeneration of inactive supported Au cata- lysts. A correlation between the BDE of R-X and dispersion efficiency was established. The tendency for disintegration and redispersion followed the R-X BDE of the alkyl halide. Compared to alkyl chlorides and bromides, iodides were more efficient for redispersing sintered Au NPs. As a descriptor, the BDE of R-I played a crucial role in particle redispersion. These findings provided in- sights into the mechanism of organic halide-induced Au NP disintegration and the effect of the hal- ide type on the redispersion of sintered catalysts.展开更多
Graphdiyne(GDY)has attracted considerable attention as a new two-dimensional(2D)carbon hybrid material because of its good conductivity,adjustable electronic structure,and special electron transfer enhancement propert...Graphdiyne(GDY)has attracted considerable attention as a new two-dimensional(2D)carbon hybrid material because of its good conductivity,adjustable electronic structure,and special electron transfer enhancement properties.GDY has great potential in the field of photocatalytic water splitting for hydrogen evolution,owing to its unique properties.In this study,GDY was successfully prepared by the mechanochemical coupling of precursors C_(6)Br_(6) and CaC_(2) using a ball-milling approach.The prepared GDY,especially its microstructure and composition,was well characterized using different techniques such as X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),Fourier-transform infrared,and Raman characterization techniques.By exploiting the unique two-dimensional(2D)structure and outstanding light absorption properties of GDY,GDY/CdSe 2D/0D heterojunctions were successfully established and applied to photocatalytic hydrogen evolution.The hydrogen evolution activity of GDY/CdSe-20,a type of composite material,reached 6470μmol g^(-1) h^(-1),which is 461 and 40 times higher than that of GDY and CdSe,respectively.Moreover,the fine electrical conductivity of GDY enabled rapid and effective transfer of the photogenerated electrons in CdSe into the hydrogen evolution reaction.The transfer path of the photogenerated electrons was studied through XPS with in situ irradiation,and a reasonable mechanism for the hydrogen evolution reaction was proposed.This study provides a feasible approach for the large-scale preparation of GDY and demonstrates the prospects of GDY in the field of photocatalysis.展开更多
文摘Disintegration or redispersion of supported sintered gold nanoparticles （Au NPs） in the presence of alkyl halide can give catalyst regeneration or redispersion of sintered Au catalysts. The selectivity of alkyl halides, temperature and size distributions were investigated to elucidate the redispersion of Au NPs during halide-induced decomposition. This study proved that the alkyl halide induced the redispersion of sintered Au NPs which depended on the R-X （X = I, Br, CI） bond dissociation energy （BDE） and thus provided a simple descriptor for the regeneration of inactive supported Au cata- lysts. A correlation between the BDE of R-X and dispersion efficiency was established. The tendency for disintegration and redispersion followed the R-X BDE of the alkyl halide. Compared to alkyl chlorides and bromides, iodides were more efficient for redispersing sintered Au NPs. As a descriptor, the BDE of R-I played a crucial role in particle redispersion. These findings provided in- sights into the mechanism of organic halide-induced Au NP disintegration and the effect of the hal- ide type on the redispersion of sintered catalysts.
文摘Graphdiyne(GDY)has attracted considerable attention as a new two-dimensional(2D)carbon hybrid material because of its good conductivity,adjustable electronic structure,and special electron transfer enhancement properties.GDY has great potential in the field of photocatalytic water splitting for hydrogen evolution,owing to its unique properties.In this study,GDY was successfully prepared by the mechanochemical coupling of precursors C_(6)Br_(6) and CaC_(2) using a ball-milling approach.The prepared GDY,especially its microstructure and composition,was well characterized using different techniques such as X-ray diffraction,scanning electron microscopy,transmission electron microscopy,X-ray photoelectron spectroscopy(XPS),Fourier-transform infrared,and Raman characterization techniques.By exploiting the unique two-dimensional(2D)structure and outstanding light absorption properties of GDY,GDY/CdSe 2D/0D heterojunctions were successfully established and applied to photocatalytic hydrogen evolution.The hydrogen evolution activity of GDY/CdSe-20,a type of composite material,reached 6470μmol g^(-1) h^(-1),which is 461 and 40 times higher than that of GDY and CdSe,respectively.Moreover,the fine electrical conductivity of GDY enabled rapid and effective transfer of the photogenerated electrons in CdSe into the hydrogen evolution reaction.The transfer path of the photogenerated electrons was studied through XPS with in situ irradiation,and a reasonable mechanism for the hydrogen evolution reaction was proposed.This study provides a feasible approach for the large-scale preparation of GDY and demonstrates the prospects of GDY in the field of photocatalysis.
