期刊
CHEMISTRY OF MATERIALS
卷 34, 期 5, 页码 2361-2375出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.1c04360
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资金
- French Agence Nationale de la Recherche
- German Deutsche Forschungsgemeinschaft [ANR-18-CE92- 0014-02-ANR]
The investigation explored the substitution of calcium for strontium in the composite spin chain structure of Sr11/8(Mn5/8Co3/8)O3+delta oxide. It demonstrated that the structural nature of the chains and the content of cationic vacancies can be directly designed from the Ca/Sr ratio, which also significantly influences the magnetism of the oxides.
The investigation of the substitution of calcium for strontium in the composite spin chain structure of the oxide Sr11/8(Mn5/8Co3/8)O3+delta has been performed combining powder/single crystal X-ray diffraction and 3D electron diffraction. A large family of composite commensurate/ incommensurate spin chain structures A1+y[(Mn5/8Co3/8)1-z???z]O3, built up of face sharing MnO6/CoO6 octahedra and a CoO6 trigonal prism and containing cationic vacancies (???) on the prismatic sites, has been synthesized, varying the alkaline earth ion content on the A site according to the nominal composition Sr11-nCanMn5Co3O24. It is shown that the structural nature of the chains and content of cationic vacancies can be directly designed from the Ca/Sr ratio, based on the larger oxidation power of strontium compared to calcium during synthesis in air. In this way, the cationic vacancy content z can be significantly decreased from 1/33 to 0.002 by increasing the Ca content from n = 0 to n = 6.8. Correlatively, the proportion of dimeric units (1 octahedron/1 trigonal prism) with respect to trimeric units (2 octahedra/1 trigonal prism) increases continuously from 0 to 1/3 as the Ca content increases from n = 0 to n = 6.8. It is also shown that the influence of the proportion of these dimeric/trimeric units on the magnetism of these oxides is remarkable, suggesting that, besides the size effect of calcium, it plays a role in the appearance of long-range ordering in this system.
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