We address the composition-controlled synthesis of monodispersed AgPd alloy nanoparticles （NPs）, their assembly for the first time on mesoporous graphitic carbon nitride （mpg-C3N4）, and the unprecedented catalysis...We address the composition-controlled synthesis of monodispersed AgPd alloy nanoparticles （NPs）, their assembly for the first time on mesoporous graphitic carbon nitride （mpg-C3N4）, and the unprecedented catalysis of mpg-CgN4@AgPd in the hydrolytic dehydrogenation of ammonia borane （AB） at room temperature. Monodispersed AgPd alloy NPs were synthesized using a high-temperature organic-phase surfactant-assisted protocol comprising the co-reduction of silver（I） acetate and palladium（II） acetylacetonate in the presence of oleylamine, oleic acid, and 1-0ctadecene. This protocol allowed the synthesis of four different compositions of AgPd alloy NPs. The AgPd alloy NPs were then assembled on mpg-C3N4, reduced graphene oxide, and Ketjenblack using a liquid-phase self-assembly method. Among the three supports tested, the mpg-CBN4@AgPd catalysts provided the best activity because of the Mott-Schottky effect, which was driven by the favorable work function difference between mpg-CBN4 and the metal NPs. Moreover, the activity of the mpg-CBN4@AgPd catalyst was further enhanced by an acetic acid treatment （AAt）, and a record initial turnover frequency of 94.1 mOl（hydrogen）＇mOl（catalyst）-l-min-1 was obtained. Furthermore, the mpg-CBN4@Ag42Pdss-AAt catalyst also showed moderate durability for the hydrolysis of AB. This study also includes a wealth of kinetic data for the mpg-CBN4@AgPd-catalyzed hydrolysis of AB.展开更多
文摘We address the composition-controlled synthesis of monodispersed AgPd alloy nanoparticles （NPs）, their assembly for the first time on mesoporous graphitic carbon nitride （mpg-C3N4）, and the unprecedented catalysis of mpg-CgN4@AgPd in the hydrolytic dehydrogenation of ammonia borane （AB） at room temperature. Monodispersed AgPd alloy NPs were synthesized using a high-temperature organic-phase surfactant-assisted protocol comprising the co-reduction of silver（I） acetate and palladium（II） acetylacetonate in the presence of oleylamine, oleic acid, and 1-0ctadecene. This protocol allowed the synthesis of four different compositions of AgPd alloy NPs. The AgPd alloy NPs were then assembled on mpg-C3N4, reduced graphene oxide, and Ketjenblack using a liquid-phase self-assembly method. Among the three supports tested, the mpg-CBN4@AgPd catalysts provided the best activity because of the Mott-Schottky effect, which was driven by the favorable work function difference between mpg-CBN4 and the metal NPs. Moreover, the activity of the mpg-CBN4@AgPd catalyst was further enhanced by an acetic acid treatment （AAt）, and a record initial turnover frequency of 94.1 mOl（hydrogen）＇mOl（catalyst）-l-min-1 was obtained. Furthermore, the mpg-CBN4@Ag42Pdss-AAt catalyst also showed moderate durability for the hydrolysis of AB. This study also includes a wealth of kinetic data for the mpg-CBN4@AgPd-catalyzed hydrolysis of AB.
