Immobilizing Extremely Catalytically Active Palladium Nanoparticles to Carbon Nanospheres: A Weakly-Capping Growth Approach
Immobilizing Extremely Catalytically Active Palladium Nanoparticles to Carbon Nanospheres: A Weakly-Capping Growth Approach
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DOI：
10.1021/jacs.5b06707
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发表时间：
2015-09-16
影响因子：
15
通讯作者：
Xu, Qiang
中科院分区：
文献类型：
--
作者：
Zhu, Qi-Long;Tsumori, Nobuko;Xu, Qiang
采用简单的甲醇介导的弱帽化生长方法（WCGA），以无水甲醇作为温和还原剂和弱帽化剂，成功合成了碳纳米球负载的超细钯纳米粒子（Pd NP）。 Pd NP 在环境温度下对甲酸水溶液 (FA) 100% 选择性脱氢表现出极高的 Pd 催化活性。 Pd NPs 的小尺寸和清洁的表面极大地提高了所制备的催化剂的催化性能，提供了高达 43 L H-2 g(pd)(-1) min(-1) 的平均无 CO H-2 生成速率和 60 ℃ 下 7256 h(-1) 的周转频率。这些值远高于迄今为止报道的用于非均相催化脱氢的最活性催化剂所获得的值。 FA。这种非常简便有效的甲醇介导的 WCGA 为具有清洁表面的超细金属纳米粒子提供了强大的入口，以实现增强的性能。此外，催化结果为FA在储氢方面的有效应用开辟了新途径。
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 Pd 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 H-2 generation up to 43 L H-2 g(pd)(-1) min(-1) and a turnover frequency of 7256 h(-1) at 60 degrees 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.