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Comprehensive Study of Oxygen Storage in YbFe2O4+x (x ≤ 0.5): Unprecedented Coexistence of FeOn Polyhedra in One Single Phase
Journal of the American Chemical Society ( IF 15.0 ) Pub Date : 2017-11-16 00:00:00 , DOI: 10.1021/jacs.7b06409
Sarah Nicoud 1 , Marielle Huvé 1 , Olivier Hernandez 2 , Alain Pautrat 3 , Mathieu Duttine 4 , Alain Wattiaux 4 , Claire Colin 5 , Houria Kabbour 1 , Olivier Mentré 1
Affiliation  

The multiferroic LuFe2.5+2O4 was recently proposed as a promising material for oxygen storage due to its easy reversible oxidation into LuFe3+2O4.5. We have investigated the similar scenario in YbFe2O4+x, leading to a slightly greater oxygen storage (OSC) capacity of 1434 μmol O/g. For the first time, the structural model of LnFe2O4.5 was fully understood by high-resolution microscopy images, and synchrotron and neutron diffraction experiments, as well as maximum entropy method. The oxygen uptake promotes a reconstructive shearing of the [YbO2] sub-units controlled by the adaptive Ln/Fe oxygen coordination and the Fe2/3+ redox. After oxidation, the rearrangement of the Fe coordination polyhedra is unique such that all available FeOn units (n = 6, 5, 4 in octahedra, square pyramids, trigonal bipyramids, tetrahedra) were identified in modulated rows growing in plane. This complex pseudo-ordering gives rise to short-range antiferromagnetic correlation within an insulating state.

中文翻译:

储氧的YbFe综合研究2 Ø 4+ XX前所未有的FeO共存:≤0.5)ñ多面体在一组单相

最近,人们提出将多铁性LuFe 2.5+ 2 O 4用作有希望的储氧材料,因为它易于可逆地氧化成LuFe 3+ 2 O 4.5。我们已经研究了YbFe 2 O 4+ x中的类似情况,导致储氧量(OSC)略高,为1434μmolO / g。高分辨率显微镜图像,同步加速器和中子衍射实验以及最大熵方法首次完全理解了LnFe 2 O 4.5的结构模型。吸氧促进了[YbO 2的重建剪切]子单元由自适应Ln / Fe氧配位和Fe 2/3 +氧化还原控制。氧化后,Fe配位多面体的重排是独特的,从而可以在平面中生长的已调制行中识别出所有可用的FeO n单元(八面体,方形金字塔,三棱锥,四面体中的n = 6、5、4)。这种复杂的伪排序在绝缘状态下产生了短程反铁磁相关性。
更新日期:2017-11-17
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