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Tuning Oxide Properties by Oxygen Vacancy Control During Growth and Annealing
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Understanding the Interplay of Vacancy, Cation, and Charge Ordering in the Tunable Sc2VO5+δ Defect Fluorite System
Dmitry Vrublevskiy, Joey A Lussier, Jenny R Panchuk
1Department of Chemistry, University of Winnipeg, Winnipeg, MB R3B 2E9, Canada.
Inorganic Chemistry
|December 23, 2020
Summary
This study reveals the complex structure of Sc2VO5+δ, detailing vanadium charge ordering and its transformation into a disordered cubic phase at high temperatures. This research aids in designing new oxide ion conductors.
Area of Science:
- Solid-state chemistry
- Materials science
- Inorganic chemistry
Background:
- The Sc2VO5+δ phase was previously misidentified as an oxygen-precise stoichiometric compound.
- Understanding the structural and redox behavior of defect fluorites is crucial for materials design.
Purpose of the Study:
- To synthesize and characterize the cation-ordered tetragonal Sc2VO5+δ phase.
- To elucidate the vanadium disproportionation reactions and structural transformations.
- To investigate the phase competition between ordered tetragonal and disordered cubic Sc2VO5+δ structures.
Main Methods:
- Synthesis in various atmospheric conditions (oxidative, reductive, inert).
- Ex situ and in situ powder X-ray and neutron diffraction.
- DC magnetometry and X-ray absorption near-edge structure (XANES) spectroscopy.
Main Results:
- Demonstrated four synthesis routes for Sc2VO5+δ.
- Identified vanadium charge ordering in the tetragonal phase with V3+, V4+, and V5+ cations occupying specific sites.
- Revealed the transformation of the tetragonal phase to a disordered cubic phase above 600 °C.
- Established a structure-reaction map showing oxygen-dependent phase competition.
Conclusions:
- The cation-ordered tetragonal Sc2VO5+δ phase exhibits unique vanadium charge ordering.
- The material undergoes a reversible structural transition to a disordered cubic phase.
- This work provides insights for designing advanced oxide ion conductors and vacancy structures.
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