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Title: Structural, magnetic, and oxygen storage properties of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ}

Abstract

Single-phase polycrystalline samples of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ} were synthesized over the full solubility range under reducing oxygen partial pressure conditions. Rietveld refinements using neutron powder diffraction data (NPD) confirmed the persistence of the parent hexagonal P6{sub 3}cm (Space group #185) structure for all the stoichiometric (δ=0) samples. The (Mn–O) bond lengths derived from NPD data were found to be consistent with non-degenerate Mn{sup +3} high-spin state e“{sup 2}e′{sup 2} in trigonal–bipyramidal coordination. Detailed thermogravimetric measurements show large reversible oxygen storage/release capabilities (within the range of oxygen content 3.0–3.3) at unusually low temperatures of 200–400 °C in air or oxygen atmospheres. A phase transition to a new hexagonal phase (Hex1) was observed to take place around δ∼0.29 for the oxygen-loaded Dy-rich samples (x<0.5). Analysis of x-ray and neutron diffraction data using Rietveld refinements demonstrate that the superstructure is formed by tripling the c-axis of the original P6{sub 3}cm unit cell. Modeling of the Hex1 superstructure converged to a structural symmetry consistent with the noncentrosymmetric space group R3c (#161). In magnetization measurements, a ferrimagnetic order for DyMnO{sub 3.0} was observed below 8 K. The dilution of Dy magnetism with nonmagnetic yttrium results in reducing both the transition temperature and themore » effective paramagnetic moment. - Graphical abstract: Superstructure of the (R3c) Dy{sub 0.7}Y{sub 0.3}MnO{sub 3.29} in the lattice range c=0.27611–0.42829 (left panel) along with its low-temperature oxygen absorption/desorption capability in pure O{sub 2} (right panel). - Highlights: • Polycrystalline samples of Dy{sub 1−x}Y{sub x}MnO{sub 3+δ} were synthesized in the hexagonal phase. • They exhibit large oxygen storage/release capabilities at low oxidation temperatures. • A phase transition to the R3c superstructure was observed around δ=0.29. • Both the Tc and effective paramagnetic moment were reduced with the Dy substitution.« less

Authors:
 [1];  [1];  [2];  [3]; ;  [1];  [1];  [2]
  1. Department of Physics, Northern Illinois University, DeKalb, IL 60115 (United States)
  2. (United States)
  3. Australian Nuclear Science and Technology Organization, ANSTO, Sydney, NSW (Australia)
Publication Date:
OSTI Identifier:
22443395
Resource Type:
Journal Article
Journal Name:
Journal of Solid State Chemistry
Additional Journal Information:
Journal Volume: 217; Other Information: Copyright (c) 2014 Elsevier Science B.V., Amsterdam, The Netherlands, All rights reserved.; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0022-4596
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; ABSORPTION; BOND LENGTHS; DESORPTION; HEXAGONAL LATTICES; HIGH SPIN STATES; MAGNETIC PROPERTIES; MAGNETIZATION; NEUTRON DIFFRACTION; OXIDATION; OXYGEN; PARAMAGNETISM; PARTIAL PRESSURE; PHASE TRANSFORMATIONS; POLYCRYSTALS; SPACE GROUPS; THERMAL GRAVIMETRIC ANALYSIS; TRANSITION TEMPERATURE; TRIGONAL LATTICES; X-RAY DIFFRACTION; YTTRIUM

Citation Formats

Abughayada, C., E-mail: castro.gha@gmail.com, Dabrowski, B., Materials Science Division, Argonne National Laboratory, Argonne, IL 60439, Avdeev, M., Kolesnik, S., Remsen, S., Chmaissem, O., and Materials Science Division, Argonne National Laboratory, Argonne, IL 60439. Structural, magnetic, and oxygen storage properties of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ}. United States: N. p., 2014. Web. doi:10.1016/J.JSSC.2014.05.017.
Abughayada, C., E-mail: castro.gha@gmail.com, Dabrowski, B., Materials Science Division, Argonne National Laboratory, Argonne, IL 60439, Avdeev, M., Kolesnik, S., Remsen, S., Chmaissem, O., & Materials Science Division, Argonne National Laboratory, Argonne, IL 60439. Structural, magnetic, and oxygen storage properties of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ}. United States. doi:10.1016/J.JSSC.2014.05.017.
Abughayada, C., E-mail: castro.gha@gmail.com, Dabrowski, B., Materials Science Division, Argonne National Laboratory, Argonne, IL 60439, Avdeev, M., Kolesnik, S., Remsen, S., Chmaissem, O., and Materials Science Division, Argonne National Laboratory, Argonne, IL 60439. Mon . "Structural, magnetic, and oxygen storage properties of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ}". United States. doi:10.1016/J.JSSC.2014.05.017.
@article{osti_22443395,
title = {Structural, magnetic, and oxygen storage properties of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ}},
author = {Abughayada, C., E-mail: castro.gha@gmail.com and Dabrowski, B. and Materials Science Division, Argonne National Laboratory, Argonne, IL 60439 and Avdeev, M. and Kolesnik, S. and Remsen, S. and Chmaissem, O. and Materials Science Division, Argonne National Laboratory, Argonne, IL 60439},
abstractNote = {Single-phase polycrystalline samples of hexagonal Dy{sub 1−x}Y{sub x}MnO{sub 3+δ} were synthesized over the full solubility range under reducing oxygen partial pressure conditions. Rietveld refinements using neutron powder diffraction data (NPD) confirmed the persistence of the parent hexagonal P6{sub 3}cm (Space group #185) structure for all the stoichiometric (δ=0) samples. The (Mn–O) bond lengths derived from NPD data were found to be consistent with non-degenerate Mn{sup +3} high-spin state e“{sup 2}e′{sup 2} in trigonal–bipyramidal coordination. Detailed thermogravimetric measurements show large reversible oxygen storage/release capabilities (within the range of oxygen content 3.0–3.3) at unusually low temperatures of 200–400 °C in air or oxygen atmospheres. A phase transition to a new hexagonal phase (Hex1) was observed to take place around δ∼0.29 for the oxygen-loaded Dy-rich samples (x<0.5). Analysis of x-ray and neutron diffraction data using Rietveld refinements demonstrate that the superstructure is formed by tripling the c-axis of the original P6{sub 3}cm unit cell. Modeling of the Hex1 superstructure converged to a structural symmetry consistent with the noncentrosymmetric space group R3c (#161). In magnetization measurements, a ferrimagnetic order for DyMnO{sub 3.0} was observed below 8 K. The dilution of Dy magnetism with nonmagnetic yttrium results in reducing both the transition temperature and the effective paramagnetic moment. - Graphical abstract: Superstructure of the (R3c) Dy{sub 0.7}Y{sub 0.3}MnO{sub 3.29} in the lattice range c=0.27611–0.42829 (left panel) along with its low-temperature oxygen absorption/desorption capability in pure O{sub 2} (right panel). - Highlights: • Polycrystalline samples of Dy{sub 1−x}Y{sub x}MnO{sub 3+δ} were synthesized in the hexagonal phase. • They exhibit large oxygen storage/release capabilities at low oxidation temperatures. • A phase transition to the R3c superstructure was observed around δ=0.29. • Both the Tc and effective paramagnetic moment were reduced with the Dy substitution.},
doi = {10.1016/J.JSSC.2014.05.017},
journal = {Journal of Solid State Chemistry},
issn = {0022-4596},
number = ,
volume = 217,
place = {United States},
year = {2014},
month = {9}
}