Solid–state synthesis of multicomponent equiatomic rare–earth oxides

Pianassola, Matheus; Loveday, Madeline; McMurray, Jake W.; Koschan, Merry; Melcher, Charles L.; Zhuravleva, Mariya

doi:10.1111/jace.16971

Attention

Certain functionality on DOE PAGES may be limited from July 10th, 8 PM EDT through July 13th, 6 AM EDT. We apologize for any inconvenience.

Title: Solid–state synthesis of multicomponent equiatomic rare–earth oxides

Journal Article · 22 December 2019 · Journal of the American Ceramic Society

DOI: https://doi.org/10.1111/jace.16971 · OSTI ID:1606694

^[1]; Loveday, Madeline ^[1];

^[2]; Koschan, Merry ^[1]; Melcher, Charles L. ^[1]; Zhuravleva, Mariya ^[1]

Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Phase formation in multicomponent rare–earth oxides is determined by a combination of composition, sintering atmosphere, and cooling rate. Polycrystalline ceramics comprising various combinations of Ce, Gd, La, Nd, Pr, Sm, and Y oxides in equiatomic proportions were synthesized using solid–state sintering. The effects of composition, sintering atmosphere, and cooling rate on phase formation were investigated. Single cubic or monoclinic structures were obtained with a slow cooling of 3.3°C/min, confirming that rare–earth oxides follow a different structure stabilization process than transition metal high–entropy oxides. In an oxidizing atmosphere, both Ce and Pr induce a cubic structure, while only Ce plays that role in an inert or reducing atmosphere. Samples without Ce or Pr develop a single monoclinic structure. The structures formed at initial synthesis may be converted to a different one, when the ceramics are annealed in an additional atmosphere. Phase evolution of a five–cation composition was also studied as a function of sintering temperature. In conclusion, the binary oxides used as raw materials completely dissolve into a single cubic structure at 1450°C in air.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: National Science Foundation; USDOE

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1606694

Journal Information:: Journal of the American Ceramic Society, Journal Name: Journal of the American Ceramic Society Journal Issue: 4 Vol. 103; ISSN 0002-7820

Publisher:: American Ceramic SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (48)

Nanostructured High-Entropy Alloys with Multiple Principal Elements: Novel Alloy Design Concepts and Outcomes Yeh, J.-W.; Chen, S.-K.; Lin, S.-J. Advanced Engineering Materials, Vol. 6, Issue 5, p. 299-303 https://doi.org/10.1002/adem.200300567	journal	May 2004
Charge-Induced Disorder Controls the Thermal Conductivity of Entropy-Stabilized Oxides Braun, Jeffrey L.; Rost, Christina M.; Lim, Mina Advanced Materials, Vol. 30, Issue 51 https://doi.org/10.1002/adma.201805004	journal	October 2018
Colossal dielectric constant in high entropy oxides Bérardan, David; Franger, Sylvain; Dragoe, Diana physica status solidi (RRL) - Rapid Research Letters, Vol. 10, Issue 4 https://doi.org/10.1002/pssr.201600043	journal	March 2016
Valencies of the lanthanides Johnson, David A.; Nelson, Peter G. Foundations of Chemistry, Vol. 20, Issue 1 https://doi.org/10.1007/s10698-017-9291-6	journal	August 2017
Formation and Stability of Equiatomic and Nonequiatomic Nanocrystalline CuNiCoZnAlTi High-Entropy Alloys by Mechanical Alloying Varalakshmi, S.; Kamaraj, M.; Murty, B. S. Metallurgical and Materials Transactions A, Vol. 41, Issue 10 https://doi.org/10.1007/s11661-010-0344-x	journal	July 2010
Mechanochemical Synthesis of (Co,Cu,Mg,Ni,Zn)O High-Entropy Oxide and Its Physicochemical Properties Balcerzak, Mateusz; Kawamura, Kenichi; Bobrowski, Rafał Journal of Electronic Materials, Vol. 48, Issue 11 https://doi.org/10.1007/s11664-019-07512-z	journal	August 2019
A critical review of high entropy alloys and related concepts Miracle, D. B.; Senkov, O. N. Acta Materialia, Vol. 122 https://doi.org/10.1016/j.actamat.2016.08.081	journal	January 2017
Mechanical alloying and spark plasma sintering of CoCrFeNiMnAl high-entropy alloy Wang, Chao; Ji, Wei; Fu, Zhengyi Advanced Powder Technology, Vol. 25, Issue 4 https://doi.org/10.1016/j.apt.2014.03.014	journal	July 2014
High-entropy oxide phases with magnetoplumbite structure Vinnik, D. A.; Trofimov, E. A.; Zhivulin, V. E. Ceramics International, Vol. 45, Issue 10 https://doi.org/10.1016/j.ceramint.2019.03.221	journal	July 2019
A high-entropy metal oxide as chemical anchor of polysulfide for lithium-sulfur batteries Zheng, Yuenan; Yi, Yikun; Fan, Meihong Energy Storage Materials, Vol. 23 https://doi.org/10.1016/j.ensm.2019.02.030	journal	December 2019
Tensile properties of high- and medium-entropy alloys Gali, A.; George, E. P. Intermetallics, Vol. 39 https://doi.org/10.1016/j.intermet.2013.03.018	journal	August 2013
Structure and magnetic properties of a multi-principal element Ni–Fe–Cr–Co–Zn–Mn alloy Zaddach, A. J.; Niu, C.; Oni, A. A. Intermetallics, Vol. 68 https://doi.org/10.1016/j.intermet.2015.09.009	journal	January 2016
Effect of temperature on mechanical properties of Al0.5CoCrCuFeNi wrought alloy Tsai, Che-Wei; Tsai, Ming-Hung; Yeh, Jien-Wei Journal of Alloys and Compounds, Vol. 490, Issue 1-2 https://doi.org/10.1016/j.jallcom.2009.10.088	journal	February 2010
Electrical, magnetic, and Hall properties of AlxCoCrFeNi high-entropy alloys Kao, Yih-Farn; Chen, Swe-Kai; Chen, Ting-Jie Journal of Alloys and Compounds, Vol. 509, Issue 5 https://doi.org/10.1016/j.jallcom.2010.10.210	journal	February 2011
Superconductivity in thermally annealed Ta-Nb-Hf-Zr-Ti high-entropy alloys Vrtnik, S.; Koželj, P.; Meden, A. Journal of Alloys and Compounds, Vol. 695 https://doi.org/10.1016/j.jallcom.2016.11.417	journal	February 2017
High-entropy fluorite oxides Gild, Joshua; Samiee, Mojtaba; Braun, Jeffrey L. Journal of the European Ceramic Society, Vol. 38, Issue 10 https://doi.org/10.1016/j.jeurceramsoc.2018.04.010	journal	August 2018
A five-component entropy-stabilized fluorite oxide Chen, Kepi; Pei, Xintong; Tang, Lei Journal of the European Ceramic Society, Vol. 38, Issue 11 https://doi.org/10.1016/j.jeurceramsoc.2018.04.063	journal	September 2018
Defect structure and transport properties in (Co,Cu,Mg,Ni,Zn)O high entropy oxide Grzesik, Z.; Smoła, G.; Stygar, M. Journal of the European Ceramic Society, Vol. 39, Issue 14 https://doi.org/10.1016/j.jeurceramsoc.2019.06.018	journal	November 2019
Synthesis and microstructure of the (Co,Cr,Fe,Mn,Ni) 3 O 4 high entropy oxide characterized by spinel structure Dąbrowa, Juliusz; Stygar, Mirosław; Mikuła, Andrzej Materials Letters, Vol. 216 https://doi.org/10.1016/j.matlet.2017.12.148	journal	April 2018
Microstructural development in equiatomic multicomponent alloys Cantor, B.; Chang, I. T. H.; Knight, P. Materials Science and Engineering: A, Vol. 375-377 https://doi.org/10.1016/j.msea.2003.10.257	journal	July 2004
Processing, microstructure and properties of Al0.6CoNiFeTi0.4 high entropy alloy with nanoscale twins Chen, Weiping; Fu, Zhiqiang; Fang, Sicong Materials Science and Engineering: A, Vol. 565 https://doi.org/10.1016/j.msea.2012.12.072	journal	March 2013
Microstructure, thermophysical and electrical properties in AlxCoCrFeNi (0≤x≤2) high-entropy alloys Chou, Hsuan-Ping; Chang, Yee-Shyi; Chen, Swe-Kai Materials Science and Engineering: B, Vol. 163, Issue 3 https://doi.org/10.1016/j.mseb.2009.05.024	journal	July 2009
A new class of high-entropy perovskite oxides Jiang, Sicong; Hu, Tao; Gild, Joshua Scripta Materialia, Vol. 142 https://doi.org/10.1016/j.scriptamat.2017.08.040	journal	January 2018
Nebulized spray pyrolysis of Al-doped Li7La3Zr2O12 solid electrolyte for battery applications Djenadic, Ruzica; Botros, Miriam; Benel, Cahit Solid State Ionics, Vol. 263 https://doi.org/10.1016/j.ssi.2014.05.007	journal	October 2014
Is Li-doped MgAl2O4 a potential solid electrolyte for an all-spinel Li-ion battery? Djenadic, Ruzica; Botros, Miriam; Hahn, Horst Solid State Ionics, Vol. 287 https://doi.org/10.1016/j.ssi.2016.02.008	journal	April 2016
Mechanical and tribological properties of multi-element (AlCrTaTiZr)N coatings Lai, Chia-Han; Cheng, Keng-Hao; Lin, Su-Jien Surface and Coatings Technology, Vol. 202, Issue 15 https://doi.org/10.1016/j.surfcoat.2008.01.014	journal	April 2008
Characteristics of (TiAlCrNbY)C films deposited by reactive magnetron sputtering Braic, M.; Braic, V.; Balaceanu, M. Surface and Coatings Technology, Vol. 204, Issue 12-13 https://doi.org/10.1016/j.surfcoat.2009.10.049	journal	March 2010
Stability and Compressibility of Cation-Doped High-Entropy Oxide MgCoNiCuZnO ₅ Chen, Jian; Liu, Weixin; Liu, Junxiu The Journal of Physical Chemistry C, Vol. 123, Issue 29 https://doi.org/10.1021/acs.jpcc.9b04992	journal	July 2019
The Binary Rare Earth Oxides Adachi, Gin-ya; Imanaka, Nobuhito Chemical Reviews, Vol. 98, Issue 4 https://doi.org/10.1021/cr940055h	journal	June 1998
Kinetic Studies on Reactions of Praseodymium Oxides in an Oxygen Atmosphere: PrO _1.83 + O ₂ ⇄ PrO ₂ Hyde, B. G.; Garver, E. E.; Kuntz, U. E. The Journal of Physical Chemistry, Vol. 69, Issue 5 https://doi.org/10.1021/j100889a037	journal	May 1965
Entropy-stabilized oxides Rost, Christina M.; Sachet, Edward; Borman, Trent Nature Communications, Vol. 6, Issue 1 https://doi.org/10.1038/ncomms9485	journal	September 2015
High entropy oxides for reversible energy storage Sarkar, Abhishek; Velasco, Leonardo; Wang, Di Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-05774-5	journal	August 2018
Giant Enhancement of Exchange Coupling in Entropy-Stabilized Oxide Heterostructures Meisenheimer, P. B.; Kratofil, T. J.; Heron, J. T. Scientific Reports, Vol. 7, Issue 1 https://doi.org/10.1038/s41598-017-13810-5	journal	October 2017
High-Entropy Metal Diborides: A New Class of High-Entropy Materials and a New Type of Ultrahigh Temperature Ceramics Gild, Joshua; Zhang, Yuanyao; Harrington, Tyler Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep37946	journal	November 2016
Room temperature lithium superionic conductivity in high entropy oxides Bérardan, D.; Franger, S.; Meena, A. K. Journal of Materials Chemistry A, Vol. 4, Issue 24 https://doi.org/10.1039/C6TA03249D	journal	January 2016
Multicomponent equiatomic rare earth oxides with a narrow band gap and associated praseodymium multivalency Sarkar, Abhishek; Loho, Christoph; Velasco, Leonardo Dalton Transactions, Vol. 46, Issue 36 https://doi.org/10.1039/C7DT02077E	journal	January 2017
Entropy-stabilized metal oxide solid solutions as CO oxidation catalysts with high-temperature stability Chen, Hao; Fu, Jie; Zhang, Pengfei Journal of Materials Chemistry A, Vol. 6, Issue 24 https://doi.org/10.1039/C8TA01772G	journal	January 2018
Low temperature synthesis and characterization of single phase multi-component fluorite oxide nanoparticle sols Anandkumar, Mariappan; Bhattacharya, Saswata; Deshpande, Atul Suresh RSC Advances, Vol. 9, Issue 46 https://doi.org/10.1039/C9RA04636D	journal	January 2019
Multicomponent equiatomic rare earth oxides Djenadic, Ruzica; Sarkar, Abhishek; Clemens, Oliver Materials Research Letters, Vol. 5, Issue 2 https://doi.org/10.1080/21663831.2016.1220433	journal	August 2016
Effective ionic radii in oxides and fluorides Shannon, R. D.; Prewitt, C. T. Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 25, Issue 5 https://doi.org/10.1107/S0567740869003220	journal	May 1969
High‐entropy, phase‐constrained, lanthanide sesquioxide Tseng, Kuo‐Pin; Yang, Qun; McCormack, Scott J. Journal of the American Ceramic Society, Vol. 103, Issue 1 https://doi.org/10.1111/jace.16689	journal	July 2019
A fracture-resistant high-entropy alloy for cryogenic applications Gludovatz, B.; Hohenwarter, A.; Catoor, D. Science, Vol. 345, Issue 6201 https://doi.org/10.1126/science.1254581	journal	September 2014
High-Pressure B-Type Polymorphs of Some Rare-Earth Sesquioxides Hoekstra, H. R.; Gingerich, K. A. Science, Vol. 146, Issue 3648 https://doi.org/10.1126/science.146.3648.1163	journal	November 1964
Single-Phase Concentrated Solid-Solution Alloys: Bridging Intrinsic Transport Properties and Irradiation Resistance Jin, Ke; Bei, Hongbin Frontiers in Materials, Vol. 5 https://doi.org/10.3389/fmats.2018.00026	journal	April 2018
Multicomponent equiatomic rare earth oxides Djenadic, Ruzica; Sarkar, Abhishek; Clemens, Oliver Karlsruhe https://doi.org/10.5445/ir/1000059932	text	January 2017
High entropy oxides for reversible energy storage Sarkar, Abhishek; Velasco, Leonardo; Wang, Di Karlsruhe https://doi.org/10.5445/ir/1000085833	text	January 2018
Multicomponent equiatomic rare earth oxides Djenadic, Ruzica; Sarkar, Abhishek; Clemens, Oliver Taylor & Francis https://doi.org/10.6084/m9.figshare.3582009	text	January 2016
Multicomponent equiatomic rare earth oxides Djenadic, Ruzica; Sarkar, Abhishek; Clemens, Oliver Taylor & Francis https://doi.org/10.6084/m9.figshare.3582009.v1	text	January 2016

Similar Records

Structural and Optical Properties of High Entropy (La,Lu,Y,Gd,Ce)AlO₃ Perovskite Thin Films

Journal Article · 2022 · Advanced Science · OSTI ID:1893696

Corey, Zachary J.; Lu, Ping; Zhang, Guangran; +9 more

Microstructure and Mechanical Properties of Low-Activation Fe-Cr-V Multicomponent Single-Phase Alloys

Journal Article · 2018 · Journal of Materials Engineering and Performance · OSTI ID:22860394

Sun, Zhiping; Cui, Huachun

Cubic-to-tetragonal displacive transformation in Gd[sub 2]O[sub 3]-Bi[sub 2]O[sub 3] ceramics

Journal Article · 1993 · Journal of the American Ceramic Society; (United States) · OSTI ID:5629615

Su, P; Virkir, A V; Hubbard, C R; +2 more

Related Subjects

36 MATERIALS SCIENCE
phase transformations
rare earths
reaction sintering

Title: Solid–state synthesis of multicomponent equiatomic rare–earth oxides

Citation Formats

References (48)

Similar Records

Related Subjects