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多聚烯丙胺功能化钯二十面体:一锅水相合成及其在碱性介质中优越的电催化活性和乙醇耐受性。

Polyallylamine functionalized palladium icosahedra: one-pot water-based synthesis and their superior electrocatalytic activity and ethanol tolerant ability in alkaline media.

机构信息

Jiangsu Key Laboratory of Power Batteries, Laboratory of Electrochemistry, School of Chemistry and Materials Science, Nanjing Normal University, Nanjing 210023, P R China.

出版信息

Langmuir. 2013 Apr 2;29(13):4413-20. doi: 10.1021/la304881m. Epub 2013 Mar 20.

DOI:10.1021/la304881m
PMID:23480348
Abstract

Polyallylamine (PAH) functionalized Pd icosahedra are synthesized through a simple, one-pot, seedless and hydrothermal growth method. Herein, PAH is used efficiently as a complex-forming agent, capping agent, and facet-selective agent. The strong interaction between PAH and Pd atom sharply changes the electronic structure of Pd atom in the Pd icosahedra. The protective function of PAH layers and enhanced antietching capability of Pd atom are responsible for the formation of the Pd icosahedra. Very importantly, the as-prepared PAH functionalized Pd icosahedra exhibit superior electrocatalytic activity and ethanol tolerant ability toward the oxygen reduction reaction (ORR) compared to the commercially available Pt black in alkaline media. At 0.95 V (vs RHE), the ORR specific kinetic current density at the Pd icosahedra is 4.48 times higher than that at commercial Pt black. The fact demonstrates the appropriate surface modification of the Pd nanoparticles by nonmetallic molecules can be regarded as an effective way to enhance the electrocatalytic activity toward the ORR.

摘要

聚烯丙胺(PAH)功能化的钯二十面体通过一种简单的、一锅法、无种子和水热生长方法合成。在这里,PAH 被有效地用作络合剂、封端剂和晶面选择性试剂。PAH 与钯原子之间的强相互作用显著改变了钯二十面体中钯原子的电子结构。PAH 层的保护作用和增强的钯原子抗蚀刻能力是形成钯二十面体的原因。非常重要的是,与商业上可用的 Pt 黑相比,所制备的 PAH 功能化钯二十面体在碱性介质中对氧还原反应(ORR)表现出优异的电催化活性和乙醇耐受性。在 0.95 V(相对于 RHE)下,Pd 二十面体的 ORR 比商业 Pt 黑的比动力学电流密度高 4.48 倍。这一事实证明,通过非金属分子对钯纳米粒子进行适当的表面修饰可以被视为提高 ORR 电催化活性的有效方法。

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