Fluorine intercalation in the n = 1 and n = 2 layered manganites Sr2MnO3.5+x and Sr3Mn2O6 |
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| Affiliation: | 1. School of Chemistry, University of Birmingham, Birmingham, UK;2. EMAT, University of Antwerp Groenenborgerlaan 171, B-2020 Antwerp, Belgium;1. Department of Chemistry and Brockhouse Institute of Materials Research, McMaster University, Hamilton, ON, Canada L8S 4M1;2. Department of Chemistry, Michigan State University, East Lansing, MI 48824, USA;3. Canadian Neutron Beam Centre, National Research Council, Chalk River Laboratories, Chalk River, ON, Canada K0J 1J0;1. Christian Doppler Laboratory for Advanced Ferroic Oxides, Sheffield Hallam University, Howard Street, S1 1WB Sheffield, UK;2. Christian Doppler Laboratory for Advanced Ferroic Oxides, Institute for Chemistry and Technology of Materials, Graz University of Technology, Stremayrgasse 9, Graz A-8010, Austria;3. Department of Materials Science and Engineering, The University of Sheffield, Mappin Street, S1 3JD Sheffield, UK;1. Department of Metallurgy and Materials Engineering (MTM), KU Leuven, Kasteelpark Arenberg 44, 3001 Heverlee, Belgium;2. Department of Electrical Engineering (ESAT), KU Leuven, Kasteelpark Arenberg 10, 3001 Heverlee, Belgium;3. Electron Microscopy for Materials Science (EMAT), University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp, Belgium;4. Imec – Partner in Solliance, Kapeldreef 75, 3001 Heverlee, Belgium;5. Imec Division IMOMEC – Partner of Solliance, Wetenschapspark 1, 3590 Diepenbeek, Belgium;6. Institute for Material Research (IMO), Hasselt University, Wetenschapspark 1, 3590 Diepenbeek, Belgium;7. TNO, De Rondom 1, 5612 AP Eindhoven, The Netherlands;8. SIM vzw, Technologiepark 935, 9052 Zwijnaarde, Belgium;1. Division of Nanomaterials and Chemistry, Hefei National Laboratory for Physical Sciences at the Microscale, Department of Chemistry, University of Science and Technology of China, Hefei 230026, PR China;2. Shandong Provincial Key Laboratory of Chemical Energy Storage and Novel Cell Technology, Department of Chemistry and Chemical Engineering, Liaocheng University, Liaocheng 252059, PR China |
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| Abstract: | Fluorine insertion into the oxygen defect superstructure manganite Sr2MnO3.5+x has been shown by transmission electron microscopy (TEM) to result in two levels of fluorination. In the higher fluorine content sections, the fluorine anions displace oxygen anions from their apical positions into the equatorial vacancies, thus destroying the superstructure and reverting to a K2NiF4-type structure (a = 3.8210(1) Å and c = 12.686(1) Å). Conversely, lower fluorine content sections retain the Sr2MnO3.5+x defect superstructure, crystallising in the P21/c space group. Fluorine intercalation into the reduced double-layer manganite Sr3Mn2O6 occurs in a step-wise fashion according to the general formula Sr3Mn2O6Fy with y = 1, 2, and 3. It is proposed that the y = 1 phase (a = 3.815(1) Å, c = 20.29(2) Å) is produced by the filling of all the equatorial oxygen vacancies by fluorine atoms whilst the y = 2 phase (a = 3.8222(2) Å, c = 21.2435(3) Å) has a random distribution of fluorine anions throughout both interstitial rocksalt and equatorial sites. Neutron powder diffraction data suggest that the fully fluorinated y = 3 phase (a = 3.8157(6) Å, c = 23.666(4) Å) corresponds to the complete occupation of all the equatorial oxygen vacancies and the interstitial sites by intercalated fluorine. |
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