Immobilizing Extremely Catalytically Active Palladium Nanoparticles to Carbon Nanospheres: A Weakly-Capping Growth Approach

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• 作者：Qi-Long Zhu ; Nobuko Tsumori ; Qiang Xu
• 刊名：Journal of the American Chemical Society
• 出版年：2015
• 出版时间：September 16, 2015
• 年：2015
• 卷：137
• 期：36
• 页码：11743-11748
• 全文大小：461K
• ISSN：1520-5126

文摘

Ultrafine palladium nanoparticles (Pd NPs) supported on carbon nanospheres have been successfully synthesized using a facile methanol-mediated weakly-capping growth approach (WCGA) with anhydrous methanol as a mild reductant and a weakly capping agent. The Pd NPs show exceedingly high catalytic activity for 100% selective dehydrogenation of aqueous formic acid (FA) at ambient temperatures. The small size and clean surface of the Pd NPs greatly improve the catalytic properties of the as-prepared catalyst, providing an average rate of CO-free H₂ generation up to 43 L H₂ g_Pd^鈥? min^鈥? and a turnover frequency of 7256 h^鈥? at 60 掳C. These values are much higher than those obtained even with the most active catalyst reported thus far for heterogeneously catalyzed dehydrogenation of FA. This remarkably facile and effective methanol-mediated WCGA provides a powerful entry into ultrafine metal NPs with clean surface to achieve enhanced performance. Moreover, the catalytic results open up new avenues in the effective applications of FA for hydrogen storage.