Novel AgPd hollow spheres anchored on graphene as an efficient catalyst for dehydrogenation of formic acid at room temperature
Novel AgPd hollow spheres anchored on graphene as an efficient catalyst for dehydrogenation of formic acid at room temperature
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锚定在石墨烯上的新型AgPd空心球作为室温甲酸脱氢的有效催化剂
DOI：
10.1039/c5ta09159d
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发表时间：
2016-01-01
影响因子：
11.9
通讯作者：
Chen, Lixin
中科院分区：
文献类型：
--
作者：
Jiang, Yiqun;Fan, Xiulin;Chen, Lixin
首次通过简单的一锅水热法成功合成了锚定在石墨烯上的高度分散的AgPd空心球（表示为AgPd- hs /G）。该工艺以l -抗坏血酸（L-AA）为还原剂，柠檬酸三钠为稳定剂，无需添加种子、表面活性剂、有机溶剂、模板剂、稳定剂和复杂的设备。合成的AgPd-Hs/G催化剂呈球形中空结构，平均直径约为18 nm，壁薄约为5 nm。石墨烯具有薄壁的中空结构和优异的分散性，确保了大部分原子位于表面或亚表面，为甲酸脱氢提供了活性催化位点。因此，与Pd/G、AgPd/C等其他催化剂相比，具有更优异的催化效果。合成的AgPd-Hs/G在室温（25℃）条件下对甲酸的分解具有高达333 mol H2 mol−1催化剂h−1的初始周转频率（TOF）。目前制备的AgPd-Hs/G在室温条件下对甲酸脱氢无CO生成，具有高效的催化作用，可以为实际的液氢储存系统铺平道路，从而促进甲酸在燃料电池系统中的应用。
Highly dispersed AgPd hollow spheres anchored on graphene (denoted as AgPd-Hs/G) were successfully synthesized through a facile one-pot hydrothermal route for the first time. The fabrication strategy was efficient and green by using L-ascorbic acid (L-AA) as the reductant and trisodium citrate dihydrate as the stabilizer, without employing any seed, surfactant, organic solvent, template, stabilizing agent, or complicated apparatus. The as-synthesized AgPd-Hs/G catalyst exhibits a sphere-shaped hollow structure with an average diameter of about 18 nm and a thin wall of about 5 nm. The hollow architecture with a thin wall and excellent dispersion on the graphene ensure that most of the atoms are located on the surface or sub-surface, which provides reactive catalytic sites for the dehydrogenation of formic acid. Therefore, a superior catalytic effect was achieved compared with other catalysts such as Pd/G and AgPd/C. The as-synthesized AgPd-Hs/G exhibits a catalytic activity with an initial turnover frequency (TOF) value as high as 333 mol H2 mol−1 catalyst h−1 even at room temperature (25 °C) toward the decomposition of formic acid. The present AgPd-Hs/G with efficient catalysis on the dehydrogenation of formic acid without any CO generation at room temperature can pave the way for a practical liquid hydrogen storage system and therefore promote the application of formic acid in fuel cell systems.