A mechanistic study of 4-aminoantipyrine and iron derived non-platinum group metal catalyst on the oxygen reduction reaction

A mechanistic study of 4-aminoantipyrine and iron derived non-platinum group metal catalyst on the oxygen reduction reaction
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DOI:
10.1016/j.electacta.2012.11.025
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发表时间:
2013-02-15
影响因子:
6.6
通讯作者:
Atanassov, Plamen
Atanassov, Plamen
中科院分区:
材料科学2区
文献类型:
--
作者:
Robson, Michael H.;Serov, Alexey;Atanassov, Plamen

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使用牺牲载体法(SSM)合成衍生自铁和4-氨基安替比林前体的高活性非铂族金属(非PGM)催化剂以获得高度多孔的开放框架结构。铁与4-氨基安替比林的比例先前已被优化以在酸性和碱性介质中催化氧的还原。在这项研究中,在这两种介质中的氧的还原机制进行了研究,发现它遵循2 × 2途径。从表面上看,电化学分析似乎表明,由于过氧化物产率低,直接4电子转移途径是有利的,但更仔细的检查表明,遵循2 × 2途径,其中快速步骤是部分还原为过氧化物,随后还原为水的步骤也相当迅速。(C)2012爱思唯尔有限公司保留所有权利。
A highly active non-platinum group metal (non-PGM) catalyst derived from iron and 4-aminoantipyrine precursors was synthesized using a sacrificial support method (SSM) to obtain a highly porous, open framed structure. The ratio of iron to 4-aminoantipyrine had been previously optimized to catalyze the reduction of oxygen in both acid and alkaline media. In this study, the mechanism of the reduction of oxygen in both media was investigated, and it was found to follow the 2 x 2 pathway. On its face, electrochemical analysis seems to suggest that the direct 4 electron transfer pathway is favored due to the low peroxide yield, but a closer examination reveals that the 2 x 2 pathway is followed, where the fast step is the partial reduction to peroxide, and the ensuing reduction step to water is also fairly rapid. (C) 2012 Elsevier Ltd. All rights reserved.