Journal Home > Volume 11 , issue 4

Four high-entropy perovskite (HEP) RETa3O9 samples were fabricated via a spark plasma sintering (SPS) method, and the corresponding thermophysical properties and underlying mechanisms were investigated for environmental/thermal barrier coating (E/TBC) applications. The prepared samples maintained low thermal conductivity (1.50 W·m-1·K-1), high hardness (10 GPa), and an appropriate Young’s modulus (180 GPa), while the fracture toughness increased to 2.5 MPa·m1/2. Nanoindentation results showed the HEP ceramics had excellent mechanical properties and good component homogeneity. We analysed the influence of different parameters (the disorder parameters of the electronegativity, ionic radius, and atomic mass, as well as the tolerance factor) of A-site atoms on the thermal conductivity. Enhanced thermal expansion coefficients, combined with a high melting point and extraordinary phase stability, expanded the applications of the HEP RETa3O9. The results of this study had motivated a follow-up study on tantalate high-entropy ceramics with desirable properties.


menu
Abstract
Full text
Outline
About this article

High-entropy perovskite RETa3O9 ceramics for high-temperature environmental/thermal barrier coatings

Show Author's information Lin CHENBaihui LIJun GUOYuke ZHUJing FENG( )
Faculty of Material Science and Engineering, Kunming University of Science and Technology, Kunming 650093, China

Abstract

Four high-entropy perovskite (HEP) RETa3O9 samples were fabricated via a spark plasma sintering (SPS) method, and the corresponding thermophysical properties and underlying mechanisms were investigated for environmental/thermal barrier coating (E/TBC) applications. The prepared samples maintained low thermal conductivity (1.50 W·m-1·K-1), high hardness (10 GPa), and an appropriate Young’s modulus (180 GPa), while the fracture toughness increased to 2.5 MPa·m1/2. Nanoindentation results showed the HEP ceramics had excellent mechanical properties and good component homogeneity. We analysed the influence of different parameters (the disorder parameters of the electronegativity, ionic radius, and atomic mass, as well as the tolerance factor) of A-site atoms on the thermal conductivity. Enhanced thermal expansion coefficients, combined with a high melting point and extraordinary phase stability, expanded the applications of the HEP RETa3O9. The results of this study had motivated a follow-up study on tantalate high-entropy ceramics with desirable properties.

Keywords:

high-entropy ceramics (HECs), tantalates, thermal conductivity, nanoindentation, fracture toughness
Received: 27 August 2021 Revised: 03 November 2021 Accepted: 20 November 2021 Published: 17 March 2022 Issue date: April 2022
References(62)
[1]
Shian S, Sarin P, Gurak M, et al. The tetragonal-monoclinic, ferroelastic transformation in yttrium tantalate and effect of zirconia alloying. Acta Mater 2014, 69: 196-202.
[2]
Song WJ, Lavallée Y, Hess KU, et al. Volcanic ash melting under conditions relevant to ash turbine interactions. Nat Commun 2016, 7: 10795.
[3]
Li F, Zhou L, Liu JX, et al. High-entropy pyrochlores with low thermal conductivity for thermal barrier coating materials. J Adv Ceram 2019, 8: 576-582.
[4]
Feng J, Shian S, Xiao B, et al. First-principles calculations of the high-temperature phase transformation in yttrium tantalate. Phys Rev B 2014, 90: 094102.
[5]
Xiang HM, Xing Y, Dai FZ, et al. High-entropy ceramics: Present status, challenges, and a look forward. J Adv Ceram 2021, 10: 385-441.
[6]
Liu B, Liu YC, Zhu CH, et al. Advances on strategies for searching for next generation thermal barrier coating materials. J Mater Sci Technol 2019, 35: 833-851.
[7]
Chen L, Yang GJ. Epitaxial growth and cracking of highly tough 7YSZ splats by thermal spray technology. J Adv Ceram 2018, 7: 17-29.
[8]
Chen L, Feng J. Influence of HfO2 alloying effect on microstructure and thermal conductivity of HoTaO4 ceramics. J Adv Ceram 2019, 8: 537-544.
[9]
Liu MJ, Zhang G, Lu YH, et al. Plasma spray-physical vapor deposition toward advanced thermal barrier coatings: A review. Rare Met 2020, 39: 479-497.
[10]
Sun YN, Xiang HM, Dai FZ, et al. Preparation and properties of CMAS resistant bixbyite structured high- entropy oxides RE2O3 (RE = Sm, Eu, Er, Lu, Y, and Yb): Promising environmental barrier coating materials for Al2O3f/Al2O3 composites. J Adv Ceram 2021, 10: 596-613.
[11]
Garcia E, Lee H, Sampath S. Phase and microstructure evolution in plasma sprayed Yb2Si2O7 coatings. J Eur Ceram Soc 2019, 39: 1477-1486.
[12]
Kakisawa H, Nishimura T. A method for testing the interface toughness of ceramic environmental barrier coatings (EBCs) on ceramic matrix composites (CMCs). J Eur Ceram Soc 2018, 38: 655-663.
[13]
Zhou YX, Zhou Y, Wu P, et al. Thermal properties of Y1-xMgxTaO4-x/2 ceramics via anion sublattice adjustment. Rare Met 2020, 39: 545-554.
[14]
Chen L, Song P, Feng J. Influence of ZrO2 alloying effect on the thermophysical properties of fluorite-type Eu3TaO7 ceramics. Scripta Mater 2018, 152: 117-121.
[15]
Chen L, Jiang YH, Chong XY, et al. Synthesis and thermophysical properties of RETa3O9 (RE = Ce, Nd, Sm, Eu, Gd, Dy, Er) as promising thermal barrier coatings. J Am Ceram Soc 2018, 101: 1266-1278.
[16]
Zhao ZF, Chen H, Xiang HM, et al. High entropy defective fluorite structured rare-earth niobates and tantalates for thermal barrier applications. J Adv Ceram 2020, 9: 303-311.
[17]
Liu YC, Jia DC, Zhou Y, et al. Zn0.1Ca0.1Sr0.4Ba0.4ZrO3: A non-equimolar multicomponent perovskite ceramic with low thermal conductivity. J Eur Ceram Soc 2020, 40: 6272-6277.
[18]
Ogawa T, Matsudaira T, Yokoe D, et al. Spontaneously formed nanostructures in double perovskite rare-earth tantalates for thermal barrier coatings. Acta Mater 2021, 216: 117152.
[19]
Ye BL, Wen TQ, Nguyen MC, et al. First-principles study, fabrication and characterization of (Zr0.25Nb0.25Ti0.25V0.25)C high-entropy ceramics. Acta Mater 2019, 170: 15-23.
[20]
Wright AJ, Wang QY, Huang CY, et al. From high-entropy ceramics to compositionally-complex ceramics: A case study of fluorite oxides. J Eur Ceram Soc 2020, 40: 2120-2129.
[21]
Sun LC, Luo YX, Tian ZL, et al. High temperature corrosion of (Er0.25Tm0.25Yb0.25Lu0.25)2Si2O7 environmental barrier coating material subjected to water vapor and molten calcium-magnesium-aluminosilicate (CMAS). Corros Sci 2020, 175: 108881.
[22]
Chen L, Wang YT, Hu MY, et al. Achieved limit thermal conductivity and enhancements of mechanical properties in fluorite RE3NbO7 via entropy engineering. Appl Phys Lett 2021, 118: 071905.
[23]
Ren K, Wang QK, Shao G, et al. Multicomponent high- entropy zirconates with comprehensive properties for advanced thermal barrier coating. Scripta Mater 2020, 178: 382-386.
[24]
Sarkar A, Wang QS, Schiele A, et al. High-entropy oxides: Fundamental aspects and electrochemical properties. Adv Mater 2019, 31: 1806236.
[25]
Ye YF, Wang Q, Lu J, et al. High-entropy alloy: Challenges and prospects. Mater Today 2016, 19: 349-362.
[26]
Cantor B, Chang ITH, Knight P, et al. Microstructural development in equiatomic multicomponent alloys. Mater Sci Eng A 2004, 375-377: 213-218.
[27]
Liu B, Zhao JL, Liu YC, et al. Application of high- throughput first-principles calculations in ceramic innovation. J Mater Sci Technol 2021, 88: 143-157.
[28]
Qin Y, Liu JX, Li F, et al. A high entropy silicide by reactive spark plasma sintering. J Adv Ceram 2019, 8: 148-152.
[29]
Oses C, Toher C, Curtarolo S. High-entropy ceramics. Nat Rev Mater 2020, 5: 295-309.
[30]
Chen H, Zhao ZF, Xiang HM, et al. High entropy (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12: A novel high temperature stable thermal barrier material. J Mater Sci Technol 2020, 48: 57-62.
[31]
Ren XM, Tian ZL, Zhang J, et al. Equiatomic quaternary (Y1/4Ho1/4Er1/4Yb1/4)2SiO5 silicate: A perspective multifunctional thermal and environmental barrier coating material. Scripta Mater 2019, 168: 47-50.
[32]
Ramadass N. ABO3-type oxides—Their structure and properties—A bird’s eye view. Mater Sci Eng 1978, 36: 231-239.
[33]
Jiang SC, Hu T, Gild J, et al. A new class of high-entropy perovskite oxides. Scripta Mater 2018, 142: 116-120.
[34]
Stanek CR, McClellan KJ, Levy MR, et al. Defect behavior in rare earth REAlO3 scintillators. J Appl Phys 2006, 99: 113518.
[35]
Bai H, Li J, Hong Y, et al. Enhanced ferroelectricity and magnetism of quenched (1-x)BiFeO3-xBaTiO3 ceramics. J Adv Ceram 2020, 9: 511-516.
[36]
Lim H, Lim J, Jang S, et al. Emissions of Er3+ and Yb3+ co-doped SrZrO3 nanocrystals under near-infrared and near-ultraviolet excitations. J Adv Ceram 2020, 9: 413-423.
[37]
Chantikul P, Anstis GR, Lawn BR, et al. A critical evaluation of indentation techniques for measuring fracture toughness: II, strength method. J Am Ceram Soc 1981, 64: 539-543.
[38]
Anstis GR, Chantikul P, Lawn BR, et al. A critical evaluation of indentation techniques for measuring fracture toughness: I, direct crack measurements. J Am Ceram Soc 1981, 64: 533-538.
[39]
Sanditov DS, Belomestnykh VN. Relation between the parameters of the elasticity theory and averaged bulk modulus of solids. Tech Phys 2011, 56: 1619-1623.
[40]
Schlichting KW, Padture NP, Klemens PG. Thermal conductivity of dense and porous yttria-stabilized zirconia. J Mater Sci 2001, 36: 3003-3010.
[41]
Kittel C. Introduction to solid state physics. Phys Today 1957, 10: 43-44.
[42]
Chen L, Hu MY, Wu P, et al. Thermal expansion performance and intrinsic lattice thermal conductivity of ferroelastic RETaO4 ceramics. J Am Ceram Soc 2019, 102: 4809-4821.
[43]
Flamant Q, Gurak M, Clarke DR. The effect of zirconia substitution on the high-temperature transformation of the monoclinic-prime phase in yttrium tantalate. J Eur Ceram Soc 2018, 38: 3925-3931.
[44]
Zhao M, Ren XR, Yang J, et al. Thermo-mechanical properties of ThO2-doped Y2O3 stabilized ZrO2 for thermal barrier coatings. Ceram Int 2016, 42: 501-508.
[45]
Pugh SF. XCII. Relations between the elastic moduli and the plastic properties of polycrystalline pure metals. Lond Edinb Dublin Philos Mag J Sci 1954, 45: 823-843.
[46]
Kingery WD. Factors affecting thermal stress resistance of ceramic materials. J Am Ceram Soc 1955, 38: 3-15.
[47]
Nix WD, Gao HJ. Indentation size effects in crystalline materials: A law for strain gradient plasticity. J Mech Phys Solids 1998, 46: 411-425.
[48]
Li XD, Bhushan B. A review of nanoindentation continuous stiffness measurement technique and its applications. Mater Charact 2002, 48: 11-36.
[49]
Gong JH, Deng B, Jiang DY. On the efficiency of the “effective truncation length” of indenter tip in mechanical property determination with nanoindentation tests. Mater Today Commun 2020, 25: 101412.
[50]
Shell De Guzman M, Neubauer G, Flinn P, et al. The role of indentation depth on the measured hardness of materials. MRS Proc 1993, 308: 613.
[51]
Gong JH, Deng B, Qiu HP, et al. Description of the nanoindentation unloading curves with a universal function: Theoretical consideration and applications to brittle materials. Mater Chem Phys 2020, 251: 123165.
[52]
Li JY, Dai H, Zhong XH, et al. Lanthanum zirconate ceramic toughened by BaTiO3 secondary phase. J Alloys Compd 2008, 452: 406-409.
[53]
Popuri SR, Scott AJM, Downie RA, et al. Glass-like thermal conductivity in SrTiO3 thermoelectrics induced by A-site vacancies. RSC Adv 2014, 4: 33720-33723.
[54]
Yang J, Wan CL, Zhao M, et al. Effective blocking of radiative thermal conductivity in La2Zr2O7/LaPO4 composites for high temperature thermal insulation applications. J Eur Ceram Soc 2016, 36: 3809-3814.
[55]
Ma W, Mack DE, Vaßen R, et al. Perovskite-type strontium zirconate as a new material for thermal barrier coatings. J Am Ceram Soc 2008, 91: 2630-2635.
[56]
Chen L, Wu P, Song P, et al. Potential thermal barrier coating materials: RE3NbO7 (RE = La, Nd, Sm, Eu, Gd, Dy) ceramics. J Am Ceram Soc 2018, 101: 4503-4508.
[57]
Li GR, Lei J, Yang GJ, et al. Substrate-constrained effect on the stiffening behavior of lamellar thermal barrier coatings. J Eur Ceram Soc 2018, 38: 2579-2587.
[58]
Tian ZL, Zhang J, Zhang TY, et al. Towards thermal barrier coating application for rare earth silicates RE2SiO5 (RE = La, Nd, Sm, Eu, and Gd). J Eur Ceram Soc 2019, 39: 1463-1476.
[59]
Yeh JW. Recent progress in high-entropy alloys. Eur J Control 2006, 31: 633-648.
[60]
Ranganathan S. Alloyed pleasures: Multimetallic cocktails. Curr Sci 2003, 85: 1404-1406.
[61]
Wright AJ, Wang QY, Ko ST, et al. Size disorder as a descriptor for predicting reduced thermal conductivity in medium-and high-entropy pyrochlore oxides. Scripta Mater 2020, 181: 76-81.
[62]
Garg J, Bonini N, Kozinsky B, et al. Role of disorder and anharmonicity in the thermal conductivity of silicon- germanium alloys: A first-principles study. Phys Rev Lett 2011, 106: 045901.
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 27 August 2021
Revised: 03 November 2021
Accepted: 20 November 2021
Published: 17 March 2022
Issue date: April 2022

Copyright

© The Author(s) 2021.

Acknowledgements

This study was funded by the National Natural Science Foundation of China (NSFC) (Nos. 91960103 and 51762028) and Yunnan Province Materials Genome Engineering (No. 2018ZE019).

Rights and permissions

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

Reprints and Permission requests may be sought directly from editorial office.

Return