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Electrooxidation of formic acid enhanced by surfactant-free palladium nanocubes on surface modified graphene catalyst

机译:无表面活性剂的钯纳米立方体在表面改性石墨烯催化剂上增强甲酸的电氧化

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摘要

Direct Formic Acid Fuel Cells (DFAFCs) have been extensively focused and rapidly growing as one of alternative energy systems for portable devices and automobiles. However, power energy requires the active and selective metal nanocatalysts to perform the highest electrochemical activity. Here, we propose a nanocubic shape of palladium nanoparticles (PdNPs) decorated on functionalized graphene (fG), where surface modification is obtained by surfactant free method. The 11 nm and high dispersion of Pd nanocubes (PdNCs), which are majorly enclosed with (1 0 0) indicated by XRD and HRTEM results, are successfully deposited on functionalized graphene (PdNCs/fG) and used as an enhanced electrocatalysts for formic acid oxidation. Our PdNCs/fG catalyst displays a remarkable mass activity towards formic acid oxidation (494.50 A/g, over 100 times) compared to commercial catalysts of Pd/C, and over 20 times to PdNPs on unmodified graphene or reduced graphene oxide (PdNPs/rGO). Moreover, our catalyst exhibits better stability and higher CO resistance. The PdNCs/fG catalyst also generates the superior specific activity towards formic acid oxidation to 20.37 A/m(2). The study demonstrates the synergistic effect of high selective site enabled by {1 0 0} facet on PdNCs and a great potential from a support of modified graphene to Pd metal catalyst for the development of electrocatalysts in fuel cell applications.
机译:作为用于便携式设备和汽车的替代能源系统之一,直接甲酸燃料电池(DFAFC)已得到广泛关注并迅速发展。然而,电能需要活性和选择性金属纳米催化剂来执行最高的电​​化学活性。在这里,我们提出了装饰在功能化石墨烯(fG)上的纳米立方形状的钯纳米颗粒(PdNPs),其中表面改性是通过无表面活性剂的方法获得的。 XRD和HRTEM结果表明,主要被(1 0 0)包围的11 nm高分散的Pd纳米立方(PdNCs)成功沉积在官能化​​石墨烯(PdNCs / fG)上,并用作甲酸的增强电催化剂氧化。与商用Pd / C催化剂相比,我们的PdNCs / fG催化剂对甲酸氧化表现出显着的质量活性(494.50 A / g,超过100倍),在未改性的石墨烯或还原的氧化石墨烯(PdNPs / rGO)上对PdNPs的活性超过20倍)。此外,我们的催化剂表现出更好的稳定性和更高的抗CO性能。 PdNCs / fG催化剂还对甲酸氧化产生出色的比活性,达到20.37 A / m(2)。该研究证明了{1 0 0}面对PdNC的高选择性位点的协同作用,以及从改性石墨烯到Pd金属催化剂的支持在燃料电池应用中开发电催化剂的巨大潜力。

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