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Highly active sites of low spin Fe II N 4 species: The identification and the ORR performance
Nano Research ( IF 9.5 ) Pub Date : 2020-09-21 , DOI: 10.1007/s12274-020-3054-8
Huizhu Cai , Bingbing Chen , Xiao Zhang , Yuchen Deng , Dequan Xiao , Ding Ma , Chuan Shi

Over recent years, catalytic materials of Fe-N-C species have been recognized being active for oxygen reduction reaction (ORR). However, the identification of active site remains challenging as it generally involves a pyrolysis process and mixed components being obtained. Herein Fe3C/C and Fe2N/C samples were synthesized by temperature programmed reduction of Fe precursors in 15% CH4/H2 and pure NH3, respectively. By acid leaching of Fe2N/C sample, only single sites of FeN4 species were presented, providing an ideal model for identification of catalytic functions of the single sites of FeN4 in ORR. A correlation was conducted between the concentration of FeIIN4 in low spin state by Mössbauer spectra and the kinetic current density at 0.8 V in alkaline media, and such a structure-performance correlation assures the catalytic roles of low spin FeIIN4 species as highly active sites for the ORR.



中文翻译:

低自旋Fe II N 4物种的高活性位点:鉴定和ORR性能

近年来,已经认识到Fe-NC物质的催化材料对氧还原反应(ORR)具有活性。然而,活性位点的鉴定仍然具有挑战性,因为它通常涉及热解过程并获得混合组分。在此,通过温度编程分别还原Fe前驱体在15%CH 4 / H 2和纯NH 3中的合成Fe 3 C / C和Fe 2 N / C样品。通过Fe 2 N / C样品的酸浸,仅显示了FeN 4物种的单个位点,为鉴定FeN 4单个位点的催化功能提供了理想的模型在ORR中。通过Mössbauer光谱在低自旋态下的Fe II N 4浓度与碱性介质在0.8 V下的动电流密度之间建立了相关性,这种结构-性能相关性确保了低自旋Fe II N 4物种的催化作用作为ORR高度活跃的网站。

更新日期:2020-11-12
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