Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state

Electron Probe X-ray Microanalysis (EPMA) is a key method for studying phase equilibria in oxide materials, offering an effective balance of precision, accuracy, cost, speed and spatial resolution. It provides valuable compositional data for single phase and multiphase materials, particularly those...

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Main Authors: Roman Starykh, Svetlana Sineva, Denis Shishin, Evgueni Jak
Format: Article
Language:English
Published: Elsevier 2025-07-01
Series:Materials & Design
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Online Access:http://www.sciencedirect.com/science/article/pii/S0264127525006008
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author Roman Starykh
Svetlana Sineva
Denis Shishin
Evgueni Jak
author_facet Roman Starykh
Svetlana Sineva
Denis Shishin
Evgueni Jak
author_sort Roman Starykh
collection DOAJ
description Electron Probe X-ray Microanalysis (EPMA) is a key method for studying phase equilibria in oxide materials, offering an effective balance of precision, accuracy, cost, speed and spatial resolution. It provides valuable compositional data for single phase and multiphase materials, particularly those with complex microstructures. Historically, high absorption of characteristic X-rays has limited the accuracy of oxygen quantification, leading to reliance on metal cation measurements and assumed oxidation states, often resulting in inaccuracies. This study highlights recent advancements in EPMA sample preparation and measurement techniques that significantly enhance oxygen quantification. To validate the method, Fe-O system samples were synthesized at 1300 °C (1573 K) under controlled oxygen partial pressures. A wide range of P(O2) was employed to cover the Fe3+/(Fe2+ + Fe3+) ratios from 0.1 to 1.0 in wüstite, spinel, and hematite phases. The results were compared with existing thermodynamic models and experimental data, demonstrating excellent agreement. The enhanced EPMA methodology offers potential for direct quantitative measurement of oxygen, which in turn, opens an opportunity to estimate Fe3+/(Fe2+ + Fe3+) ratios in complex chemical systems, including quenched slags. The approach is applicable to other metals with variable oxidation states, provided a single element primarily drives oxidation state changes.
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spelling doaj-art-d16d72783e4e4911948badf8860523bc2025-08-20T03:22:04ZengElsevierMaterials & Design0264-12752025-07-0125511418010.1016/j.matdes.2025.114180Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation stateRoman Starykh0Svetlana Sineva1Denis Shishin2Evgueni Jak3Corresponding author.; PYROSEARCH, The University of Queensland, Brisbane, QLD 4072, AustraliaPYROSEARCH, The University of Queensland, Brisbane, QLD 4072, AustraliaPYROSEARCH, The University of Queensland, Brisbane, QLD 4072, AustraliaPYROSEARCH, The University of Queensland, Brisbane, QLD 4072, AustraliaElectron Probe X-ray Microanalysis (EPMA) is a key method for studying phase equilibria in oxide materials, offering an effective balance of precision, accuracy, cost, speed and spatial resolution. It provides valuable compositional data for single phase and multiphase materials, particularly those with complex microstructures. Historically, high absorption of characteristic X-rays has limited the accuracy of oxygen quantification, leading to reliance on metal cation measurements and assumed oxidation states, often resulting in inaccuracies. This study highlights recent advancements in EPMA sample preparation and measurement techniques that significantly enhance oxygen quantification. To validate the method, Fe-O system samples were synthesized at 1300 °C (1573 K) under controlled oxygen partial pressures. A wide range of P(O2) was employed to cover the Fe3+/(Fe2+ + Fe3+) ratios from 0.1 to 1.0 in wüstite, spinel, and hematite phases. The results were compared with existing thermodynamic models and experimental data, demonstrating excellent agreement. The enhanced EPMA methodology offers potential for direct quantitative measurement of oxygen, which in turn, opens an opportunity to estimate Fe3+/(Fe2+ + Fe3+) ratios in complex chemical systems, including quenched slags. The approach is applicable to other metals with variable oxidation states, provided a single element primarily drives oxidation state changes.http://www.sciencedirect.com/science/article/pii/S0264127525006008Fe-O systemFerric to ferrous ratioOxygen measurementEPMA
spellingShingle Roman Starykh
Svetlana Sineva
Denis Shishin
Evgueni Jak
Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
Materials & Design
Fe-O system
Ferric to ferrous ratio
Oxygen measurement
EPMA
title Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
title_full Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
title_fullStr Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
title_full_unstemmed Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
title_short Quantitative measurement of oxygen by Electron Probe X-ray Microanalysis for estimation of iron oxidation state
title_sort quantitative measurement of oxygen by electron probe x ray microanalysis for estimation of iron oxidation state
topic Fe-O system
Ferric to ferrous ratio
Oxygen measurement
EPMA
url http://www.sciencedirect.com/science/article/pii/S0264127525006008
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AT denisshishin quantitativemeasurementofoxygenbyelectronprobexraymicroanalysisforestimationofironoxidationstate
AT evguenijak quantitativemeasurementofoxygenbyelectronprobexraymicroanalysisforestimationofironoxidationstate