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Facile synthesis based on novel carbon-supported cyanogel of structurally ordered Pd3Fe/C as electrocatalyst for formic acid oxidation
Nano Research ( IF 9.5 ) Pub Date : 2018-04-04 , DOI: 10.1007/s12274-018-2051-7
Zhenyuan Liu , Gengtao Fu , Jiahui Li , Zhenqi Liu , Lin Xu , Dongmei Sun , Yawen Tang

A novel carbon-supported cyanogel (C@cyanogel)-derived strategy is used to synthesize an intermetallic Pd3Fe/C compound of the desired ordered Pd3Fe phase with a small particle size. The novelty of this work lies in using carbon-supported K2PdIICl4/K4FeII(CN)6 cyanogel as a reaction precursor, generated through the substitution of two chloride ligands by the nitrogen ends of the cyanide ligands on the metal center. The inherent nature of cyanogels can effectively suppress the movement of Pd0 and Fe0 nuclei in the crystal, benefiting the formation of the intermetallic, which is otherwise challenging via traditional synthesis techniques. The ordered Pd3Fe/C catalyst exhibits excellent catalytic activity and good cycle stability for the formic acid oxidation (FAO) reaction relative to the properties of disordered Pd3Fe/C and commercial Pd/C catalysts, demonstrating that the ordered Pd3Fe/C is a promising replacement for commercial Pd-based catalysts. The outstanding performance can be ascribed to the full isolation of active sites in the ordered Pd3Fe structure and the modified electronic structure of the active components. This work provides an effective and novel route to obtain Pd-based intermetallic compounds with potential applications in a wide range of electrocatalysis.

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中文翻译:

基于新型碳载氰基结构规整的氰基凝胶的简便合成3Fe / C作为甲酸氧化的电催化剂

一种新颖的碳载氰基凝胶(C @ cyanogel)衍生的策略用于合成具有小粒径的所需有序Pd 3 Fe相的金属间Pd 3 Fe / C化合物。这项工作的新颖性在于使用碳负载的K 2 Pd II Cl 4 / K 4 Fe II(CN)6氰基凝胶作为反应前体,它是通过两个氯化物配体被氰化物配体上的氰基配体的氮端取代而产生的。金属中心。cyanogels的固有性质可以有效地抑制Pd 0和Fe 0的运动晶体中的原子核,有利于金属间化合物的形成,否则通过传统合成技术将面临挑战。相对于无序Pd 3 Fe / C和商用Pd / C催化剂的性能,有序Pd 3 Fe / C催化剂对甲酸氧化(FAO)反应显示出优异的催化活性和良好的循环稳定性,这表明有序Pd 3 Fe / C是商业化的基于Pd的催化剂的有希望的替代品。出色的性能可归因于有序Pd 3中活动位点的完全隔离铁结构和活性成分的改性电子结构。这项工作提供了一种有效且新颖的途径来获得具有广泛应用的Pd基金属间化合物,在电催化领域具有潜在的应用。

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更新日期:2018-04-04
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