The effect of temperature and oxygen partial pressure on the concentration of iron and manganese ions in La1/3Sr2/3Fe1−xMnxO3−δ

Literature Information

Publication Date 2023-12-15
DOI 10.1039/D3CP05421G
Impact Factor 3.676
Authors

Sergey S. Nikitin, Alexander D. Koryakov, Elizaveta A. Antipinskaya, Mikhail V. Patrakeev


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Abstract

The oxygen content was measured in cubic perovskite-type La1/3Sr2/3Fe1−xMnxO3−δ (x = 0.1, 0.17, 0.25, and 1/3) in the range of oxygen partial pressure from 10−22 to 0.5 atm at 750–950 °C with a step of 50 °C by coulometric titration. Gradual removal of oxygen from the oxides during the measurements was carried out until the stability limit was achieved and the reductive decomposition began. An increase in manganese content was shown to lead to a decrease in the stability of La1/3Sr2/3Fe1−xMnxO3−δ under reducing conditions. The obtained data on oxygen content were used for defect chemistry modeling in the oxides. The enthalpy of the Fe3+ to Fe4+ and Mn3+ to Mn4+ oxidation reactions (ΔHox0) was determined to be −103.2 ± 0.3 and −250 ± 2 kJ mol−1, respectively, for the x = 0.1 composition, and increased slightly with increasing manganese content. The large difference in ΔHox0 determines a strong distinction between the behavior of iron and manganese in perovskite-type oxides. An increase in manganese content in La1/3Sr2/3Fe1−xMnxO3−δ was found to lead to a decrease in the concentration of Fe4+ ions, but did not affect the concentration of Fe2+ ions. The impact of La/Sr ratio was evaluated by comparison of the obtained data with that for La0.5Sr0.5Fe1−xMnxO3−δ, and found to be different for iron and manganese. An increase in lanthanum fraction causes a decrease in the concentration of Fe2+ ions and an increase in the concentration of Mn2+ under reducing conditions.

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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
Self-citation Rate: 10.3%
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Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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