Mass spectrometric study and modeling of the thermodynamic properties in the Gd2O3-ZrO2-HfO2 system at high temperatures

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Mass spectrometric study and modeling of the thermodynamic properties in the Gd2O3-ZrO2-HfO2 system at high temperatures. / Kablov, Eugene N.; Shilov, Andrey L.; Stolyarova, Valentina L.; Vorozhtcov, Viktor A.; Karachevtsev, Fedor N.; Lopatin, Sergey I.; Shugurov, Sergey M.

In: Rapid Communications in Mass Spectrometry, Vol. 36, No. 13, e9306, 15.07.2022.

Research output: Contribution to journal › Article › peer-review

BibTeX

@article{87c5ee8fd2ee45379653d832285c43ce,

title = "Mass spectrometric study and modeling of the thermodynamic properties in the Gd2O3-ZrO2-HfO2 system at high temperatures",

abstract = "Rationale: Materials based on the Gd2O3-ZrO2-HfO2 system are promising for a wide range of high-temperature technological applications, such as for obtaining thermal barrier coatings in the aviation and space industry, as well as advanced materials in nuclear power applications. Experimental studies of the ceramics based on this system by the Knudsen effusion mass spectrometric method provides such valuable information as the vapor composition over the samples and enables derivation of the thermodynamic functions. Methods: Samples of ceramics in the Gd2O3-ZrO2-HfO2 system were synthesized and analyzed by X-ray fluorescence and diffraction techniques. The vaporization processes and partial pressures of the vapor species over the samples were obtained by the high-temperature mass spectrometric method using the ion current comparison method. The derived thermodynamic functions were optimized within the Generalized Lattice Theory of Associated Solutions (GLTAS) approach. Results: At the temperature of 2600 K, the GdO, ZrO, ZrO2, HfO, and O vapor species were found over the samples, but only for the GdO and ZrO species were accurate experimental data on the partial pressures obtained. In all the ceramic samples, the Gd2O3 activity was determined. On this experimental basis, modeling within the GLTAS approach was performed. It allowed the evaluation of the Gd2O3, ZrO2, and HfO2 activities in the system under study and a rough approximation of the excess Gibbs energy as a function of composition to be obtained. Conclusions: At 2600 K the Gd2O3-ZrO2-HfO2 system is characterized by negative deviations of its thermodynamic properties from the ideal behavior. Consistency of the obtained modeling results indicate reasonable uniformity of the energy parameters of the lattice model derived in calculations of the hafnia-containing oxide systems, which may be used in further modeling of multicomponent systems.",

author = "Kablov, {Eugene N.} and Shilov, {Andrey L.} and Stolyarova, {Valentina L.} and Vorozhtcov, {Viktor A.} and Karachevtsev, {Fedor N.} and Lopatin, {Sergey I.} and Shugurov, {Sergey M.}",

note = "Publisher Copyright: {\textcopyright} 2022 John Wiley & Sons Ltd.",

year = "2022",

month = jul,

day = "15",

doi = "10.1002/rcm.9306",

language = "English",

volume = "36",

journal = "Rapid Communications in Mass Spectrometry",

issn = "0951-4198",

publisher = "Wiley-Blackwell",

number = "13",

}

RIS

TY - JOUR

T1 - Mass spectrometric study and modeling of the thermodynamic properties in the Gd2O3-ZrO2-HfO2 system at high temperatures

AU - Kablov, Eugene N.

AU - Shilov, Andrey L.

AU - Stolyarova, Valentina L.

AU - Vorozhtcov, Viktor A.

AU - Karachevtsev, Fedor N.

AU - Lopatin, Sergey I.

AU - Shugurov, Sergey M.

PY - 2022/7/15

Y1 - 2022/7/15

N2 - Rationale: Materials based on the Gd2O3-ZrO2-HfO2 system are promising for a wide range of high-temperature technological applications, such as for obtaining thermal barrier coatings in the aviation and space industry, as well as advanced materials in nuclear power applications. Experimental studies of the ceramics based on this system by the Knudsen effusion mass spectrometric method provides such valuable information as the vapor composition over the samples and enables derivation of the thermodynamic functions. Methods: Samples of ceramics in the Gd2O3-ZrO2-HfO2 system were synthesized and analyzed by X-ray fluorescence and diffraction techniques. The vaporization processes and partial pressures of the vapor species over the samples were obtained by the high-temperature mass spectrometric method using the ion current comparison method. The derived thermodynamic functions were optimized within the Generalized Lattice Theory of Associated Solutions (GLTAS) approach. Results: At the temperature of 2600 K, the GdO, ZrO, ZrO2, HfO, and O vapor species were found over the samples, but only for the GdO and ZrO species were accurate experimental data on the partial pressures obtained. In all the ceramic samples, the Gd2O3 activity was determined. On this experimental basis, modeling within the GLTAS approach was performed. It allowed the evaluation of the Gd2O3, ZrO2, and HfO2 activities in the system under study and a rough approximation of the excess Gibbs energy as a function of composition to be obtained. Conclusions: At 2600 K the Gd2O3-ZrO2-HfO2 system is characterized by negative deviations of its thermodynamic properties from the ideal behavior. Consistency of the obtained modeling results indicate reasonable uniformity of the energy parameters of the lattice model derived in calculations of the hafnia-containing oxide systems, which may be used in further modeling of multicomponent systems.

AB - Rationale: Materials based on the Gd2O3-ZrO2-HfO2 system are promising for a wide range of high-temperature technological applications, such as for obtaining thermal barrier coatings in the aviation and space industry, as well as advanced materials in nuclear power applications. Experimental studies of the ceramics based on this system by the Knudsen effusion mass spectrometric method provides such valuable information as the vapor composition over the samples and enables derivation of the thermodynamic functions. Methods: Samples of ceramics in the Gd2O3-ZrO2-HfO2 system were synthesized and analyzed by X-ray fluorescence and diffraction techniques. The vaporization processes and partial pressures of the vapor species over the samples were obtained by the high-temperature mass spectrometric method using the ion current comparison method. The derived thermodynamic functions were optimized within the Generalized Lattice Theory of Associated Solutions (GLTAS) approach. Results: At the temperature of 2600 K, the GdO, ZrO, ZrO2, HfO, and O vapor species were found over the samples, but only for the GdO and ZrO species were accurate experimental data on the partial pressures obtained. In all the ceramic samples, the Gd2O3 activity was determined. On this experimental basis, modeling within the GLTAS approach was performed. It allowed the evaluation of the Gd2O3, ZrO2, and HfO2 activities in the system under study and a rough approximation of the excess Gibbs energy as a function of composition to be obtained. Conclusions: At 2600 K the Gd2O3-ZrO2-HfO2 system is characterized by negative deviations of its thermodynamic properties from the ideal behavior. Consistency of the obtained modeling results indicate reasonable uniformity of the energy parameters of the lattice model derived in calculations of the hafnia-containing oxide systems, which may be used in further modeling of multicomponent systems.

UR - http://www.scopus.com/inward/record.url?scp=85131319429&partnerID=8YFLogxK

UR - https://www.mendeley.com/catalogue/0fbe6ab1-bf7d-37e2-867f-ca0bb90f2c0e/

U2 - 10.1002/rcm.9306

DO - 10.1002/rcm.9306

M3 - Article

AN - SCOPUS:85131319429

VL - 36

JO - Rapid Communications in Mass Spectrometry

JF - Rapid Communications in Mass Spectrometry

SN - 0951-4198

IS - 13

M1 - e9306

ER -

ID: 93805506