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Rare-earth aluminates (REAlO3) are potential thermal barrier coating (TBC) materials, but the relatively high thermal conductivity (k0, ~13.6 W·m−1·K−1) and low fracture toughness (KIC, ~1.9 MPa·m1/2) limit their application. This work proposed a strategy to improve their properties through the synergistic effects of high-entropy engineering and particulate toughening. High-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)AlO3 (HEAO)-based particulate composites with different contents of high-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 (HEZO) were designed and successfully prepared by solid-state sintering. The high-entropy feature of both the matrix and secondary phases causes the strong phonon scattering and the incorporation of the HEZO secondary phase, remarkedly inhibiting the grain growth of the HEAO phase. As a result, HEAO–xHEZO (x = 0, 5%, 10%, 25%, and 50% in volume) ceramic composites show low thermal conductivity and high fracture toughness. Compared to the most commonly applied TBC material—yttria stabilized-zirconia (YSZ), the HEAO–25%HEZO particulate composite has a lower thermal conductivity of 0.96–1.17 W·m−1·K−1 (298–1273 K), enhanced fracture toughness of 3.94±0.35 MPa·m1/2, and comparable linear coefficient of thermal expansion (CTE) of 10.5×10−6 K−1. It is believed that the proposed strategy should be revelatory for the design of new coating materials including TBCs and environmental barrier coatings (EBCs).


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Synergistic effects of high-entropy engineering and particulate toughening on the properties of rare-earth aluminate-based ceramic composites

Show Author's information Tian-Zhe TuJi-Xuan Liu( )Yue WuLin ZhouYongcheng LiangGuo-Jun Zhang( )
State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Materials Science and Engineering, College of Science, Institute of Functional Materials, Donghua University, Shanghai 201620, China

Abstract

Rare-earth aluminates (REAlO3) are potential thermal barrier coating (TBC) materials, but the relatively high thermal conductivity (k0, ~13.6 W·m−1·K−1) and low fracture toughness (KIC, ~1.9 MPa·m1/2) limit their application. This work proposed a strategy to improve their properties through the synergistic effects of high-entropy engineering and particulate toughening. High-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)AlO3 (HEAO)-based particulate composites with different contents of high-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 (HEZO) were designed and successfully prepared by solid-state sintering. The high-entropy feature of both the matrix and secondary phases causes the strong phonon scattering and the incorporation of the HEZO secondary phase, remarkedly inhibiting the grain growth of the HEAO phase. As a result, HEAO–xHEZO (x = 0, 5%, 10%, 25%, and 50% in volume) ceramic composites show low thermal conductivity and high fracture toughness. Compared to the most commonly applied TBC material—yttria stabilized-zirconia (YSZ), the HEAO–25%HEZO particulate composite has a lower thermal conductivity of 0.96–1.17 W·m−1·K−1 (298–1273 K), enhanced fracture toughness of 3.94±0.35 MPa·m1/2, and comparable linear coefficient of thermal expansion (CTE) of 10.5×10−6 K−1. It is believed that the proposed strategy should be revelatory for the design of new coating materials including TBCs and environmental barrier coatings (EBCs).

Keywords: mechanical properties, thermal properties, thermal barrier coating (TBC), high-entropy particulate composites, fine grains

References(65)

[1]
Padture NP, Gell M, Jordan EH. Thermal barrier coatings for gas-turbine engine applications. Science 2002, 296: 280–284.
[2]
Vaßen R, Jarligo MO, Steinke T, et al. Overview on advanced thermal barrier coatings. Surf Coat Tech 2010, 205: 938–942.
[3]
Darolia R. Thermal barrier coatings technology: Critical review, progress update, remaining challenges and prospects. Int Mater Rev 2013, 58: 315–348.
[4]
Bakan E, Vaßen R. Ceramic top coats of plasma-sprayed thermal barrier coatings: Materials, processes, and properties. J Therm Spray Techn 2017, 26: 992–1010.
[5]
Wei ZY, Meng GH, Chen L, et al. Progress in ceramic materials and structure design toward advanced thermal barrier coatings. J Adv Ceram 2022, 11: 985–1068.
[6]
Luo LR, Chen Y, Zhou M, et al. Progress update on extending the durability of air plasma sprayed thermal barrier coatings. Ceram Int 2022, 48: 18021–18034.
[7]
Cao X, Vassen R, Fischer W, et al. Lanthanum–cerium oxide as a thermal barrier-coating material for high-temperature applications. Adv Mater 2003, 15: 1438–1442.
[8]
Liu XQ, Chen XM. Dielectric and mechanical characteristics of lanthanum aluminate ceramics with strontium niobate addition. J Eur Ceram Soc 2004, 24: 1999–2004.
[9]
Schmitt MP, Stokes JL, Rai AK, et al. Durable aluminate toughened zirconate composite thermal barrier coating (TBC) materials for high temperature operation. J Am Ceram Soc 2019, 102: 4781–4793.
[10]
Schnelle W, Fischer R, Gmelin E. Specific heat capacity and thermal conductivity of NdGaO3 and LaAlO3 single crystals at low temperatures. J Phys D Appl Phys 2001, 34: 846–851.
[11]
Vourdas N, Marathoniti E, Pandis PK, et al. Evaluation of LaAlO3 as top coat material for thermal barrier coatings. T NonferrMetal Soc 2018, 28: 1582–1592.
[12]
Wu J, Wei XZ, Padture NP, et al. Low-thermal-conductivity rare-earth zirconates for potential thermal-barrier-coating applications. J Am Ceram Soc 2004, 85: 3031–3035.
[13]
Vassen R, Cao XQ, Tietz F, et al. Zirconates as new materials for thermal barrier coatings. J Am Ceram Soc 2000, 83: 2023–2028.
[14]
Han J, Wang YF, Liu RJ, et al. Lanthanum zirconate ceramic toughened by ferroelastic domain switching of LaAlO3. Ceram Int 2018, 44: 15954–15958.
[15]
Wang YF, Han J, Du JP, et al. The toughening of pyrochlore La2Zr2O7 by a ferroelastic NdAlO3 second phase for potential thermal barrier coating applications. J Am Ceram Soc 2021, 104: 3508–3517.
[16]
Lozano-Mandujano D, Poblano-Salas CA, Ruiz-Luna H, et al. Thermal spray deposition, phase stability and mechanical properties of La2Zr2O7/LaAlO3 coatings. J Therm Spray Techn 2017, 26: 1198–1206.
[17]
Hong WC, Chen F, Shen Q, et al. Microstructural evolution and mechanical properties of (Mg,Co,Ni,Cu,Zn)O high-entropy ceramics. J Am Ceram Soc 2019, 102: 2228–2237.
[18]
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.
[19]
Ni DW, Cheng Y, Zhang JP, et al. Advances in ultra-high temperature ceramics, composites, and coatings. J Adv Ceram 2022, 11: 1–56.
[20]
Zhang GR, Wu YQ. High-entropy transparent ceramics: Review of potential candidates and recently studied cases. Int J Appl Ceram Tec 2022, 19: 644–672.
[21]
Cai FY, Ni DW, Bao WC, et al. Ablation behavior and mechanisms of Cf/(Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C–SiC high-entropy ceramic matrix composites. Compos Part B-Eng 2022, 243: 110177.
[22]
Qin MD, Gild J, Hu CZ, et al. Dual-phase high-entropy ultra-high temperature ceramics. J Eur Ceram Soc 2020, 40: 5037–5050.
[23]
Zhu JT, Meng XY, Xu J, et al. Ultra-low thermal conductivity and enhanced mechanical properties of high-entropy rare earth niobates (RE3NbO7, RE = Dy, Y, Ho, Er, Yb). J Eur Ceram Soc 2021, 41: 1052–1057.
[24]
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.
[25]
Chen H, Xiang HM, Dai FZ, et al. High entropy (Yb0.25Y0.25Lu0.25Er0.25)2SiO5 with strong anisotropy in thermal expansion. J Mater Sci Technol 2020, 36: 134–139.
[26]
Chen L, Li BH, Guo J, et al. High-entropy perovskite RETa3O9 ceramics for high-temperature environmental/thermal barrier coatings. J Adv Ceram 2022, 11: 556–569.
[27]
Liu DB, Shi BL, Geng LY, et al. High-entropy rare-earth zirconate ceramics with low thermal conductivity for advanced thermal-barrier coatings. J Adv Ceram 2022, 11: 961–973.
[28]
Zhou L, Li F, Liu JX, et al. High-entropy thermal barrier coating of rare-earth zirconate: A case study on (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Zr2O7 prepared by atmospheric plasma spraying. J Eur Ceram Soc 2020, 40: 5731–5739.
[29]
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.
[30]
Xue Y, Zhao XQ, An YL, et al. High-entropy (La0.2Nd0.2Sm0.2Eu0.2Gd0.2)2Ce2O7: A potential thermal barrier material with improved thermo-physical properties. J Adv Ceram 2022, 11: 615–628.
[31]
Zhao ZF, Chen H, Xiang HM, et al. High-entropy (Y0.2Nd0.2Sm0.2Eu0.2Er0.2)AlO3: A promising thermal/environmental barrier material for oxide/oxide composites. J Mater Sci Technol 2020, 47: 45–51.
[32]
Liu HL, Pang S, Liu CQ, et al. High-entropy yttrium pyrochlore ceramics with glass-like thermal conductivity for thermal barrier coating application. J Am Ceram Soc 2022, 105: 6437–6448.
[33]
Zhao ZF, Xiang HM, Chen H, et al. High-entropy (Nd0.2Sm0.2Eu0.2Y0.2Yb0.2)4Al2O9 with good high temperature stability, low thermal conductivity, and anisotropic thermal expansivity. J Adv Ceram 2020, 9: 595–605.
[34]
Zhao ZF, Chen H, Xiang HM, et al. (La0.2Ce0.2Nd0.2Sm0.2Eu0.2)PO4: A high-entropy rare-earth phosphate monazite ceramic with low thermal conductivity and good compatibility with Al2O3. J Mater Sci Technol 2019, 35: 2892–2896.
[35]
Zhu JT, Lou ZH, Zhang P, et al. Preparation and thermal properties of rare earth tantalates (RETaO4) high-entropy ceramics. J Inorg Mater 2021, 36: 411–417. (in Chinese)
[36]
Luo XW, Luo LR, Zhao XF, et al. Single-phase rare-earth high-entropy zirconates with superior thermal and mechanical properties. J Eur Ceram Soc 2022, 42: 2391–2399.
[37]
Xu MY, Yuan JY, Lu XR, et al. Infrared radiation and thermal cyclic performance of a high-entropy rare-earth hexaaluminate coating prepared by atmospheric plasma spraying. Ceram Int 2022, 48: 26003–26012.
[38]
Wright AJ, Huang CY, Walock MJ, et al. Sand corrosion, thermal expansion, and ablation of medium-and high-entropy compositionally complex fluorite oxides. J Am Ceram Soc 2021, 104: 448–462.
[39]
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.
[40]
Tu TZ, Liu JX, Zhou L, et al. Graceful behavior during CMAS corrosion of a high-entropy rare-earth zirconate for thermal barrier coating material. J Eur Ceram Soc 2022, 42: 649–657.
[41]
Deng SX, He G, Yang ZC, et al. Calcium–magnesium–alumina–silicate (CMAS) resistant high entropy ceramic (Y0.2Gd0.2Er0.2Yb0.2Lu0.2)2Zr2O7 for thermal barrier coatings. J Mater Sci Technol 2022, 107: 259–265.
[42]
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.
[43]
Lu K, Liu JX, Wei XF, et al. Microstructures and mechanical properties of high-entropy (Ti0.2Zr0.2Hf0.2Nb0.2Ta0.2)C ceramics with the addition of SiC secondary phase. J Eur Ceram Soc 2020, 40: 1839–1847.
[44]
Parker WJ, Jenkins RJ, Butler CP, et al. Flash method of determining thermal diffusivity, heat capacity, and thermal conductivity. J Appl Phys 1961, 32: 1679–1684.
[45]
Leitner J, Voňka P, Sedmidubský D, et al. Application of Neumann–Kopp rule for the estimation of heat capacity of mixed oxides. Thermochim Acta 2010, 497: 7–13.
[46]
Schlichting KW, Padture NP, Klemens PG. Thermal conductivity of dense and porous yttria-stabilized zirconia. J Mater Sci 2001, 36: 3003–3010.
[47]
Fabrichnaya O, Lakiza S, Wang C, et al. Assessment of thermodynamic functions in the ZrO2–La2O3–Al2O3 system. J Alloys Compd 2008, 453: 271–281.
[48]
Weber MJ, Bass M, Andringa K, et al. Czochralski growth and properties of YAlO3 laser crystals. Appl Phys Lett 1969, 15: 342–345.
[49]
Morelli DT. Thermal conductivity of high temperature superconductor substrate materials: Lanthanum aluminate and neodymium aluminate. J Mater Res 1992, 7: 2492–2494.
[50]
Clarke DR. Materials selection guidelines for low thermal conductivity thermal barrier coatings. Surf Coat Tech 2003, 163–164: 67–74.
[51]
Klemens P, Simon F. The thermal conductivities of some dielectric solids at low temperatures. P Roy Soc A-Math Phy 1951, 208: 108–133.
[52]
Klemens PG. Phonon scattering by oxygen vacancies in ceramics. Physica B 1999, 263: 102–104.
[53]
Petrov D, Angelov B, Lovchinov V. Magnetic susceptibility and surface properties of EuAlO3 nanocrystals. J Alloys Compd 2011, 509: 5038–5041.
[54]
Zhang YL, Zhou YB, Peng C, et al. Enhanced activity and stability of copper oxide/γ-alumina catalyst in catalytic wet-air oxidation: Critical roles of cerium incorporation. Appl Surf Sci 2018, 436: 981–988.
[55]
Liu SX, Du MR, Ge YF, et al. Enhancement of high entropy oxide (La0.2Nd0.2Sm0.2Gd0.2Y0.2)2Zr2O7 mechanical and photocatalytic properties via Eu doping. J Mater Sci 2022, 57: 7863–7876.
[56]
Kim D, Jin YH, Jeon KW, et al. Blue-silica by Eu2+-activator occupied in interstitial sites. RSC Adv 2015, 5: 74790–74801.
[57]
Liu Y, Yin SB, Shen PK. Asymmetric 3D electronic structure for enhanced oxygen evolution catalysis. ACS Appl Mater Interfaces 2018, 10: 23131–23139.
[58]
Zou ZH, Wang TT, Zhao XH, et al. Expediting in-situ electrochemical activation of two-dimensional metal–organic frameworks for enhanced OER intrinsic activity by iron incorporation. ACS Catal 2019, 9: 7356–7364.
[59]
Dicks OA, Shluger AL, Sushko PV, et al. Spectroscopic properties of oxygen vacancies in LaAlO3. Phys Rev B 2016, 93: 134114.
[60]
Zhang Y, Lu T, Ye YK, et al. Stabilizing oxygen vacancy in entropy-engineered CoFe2O4-type catalysts for Co-prosperity of efficiency and stability in an oxygen evolution reaction. ACS Appl Mater Interfaces 2020, 12: 32548–32555.
[61]
Wright AJ, Huang CY, Walock MJ, et al. Sand corrosion, thermal expansion, and ablation of medium- and high-entropy compositionally complex fluorite oxides. J Am Ceram Soc 2021, 104: 448–462.
[62]
Chang K, Feng WM, Chen LQ. Effect of second-phase particle morphology on grain growth kinetics. Acta Mater 2009, 57: 5229–5236.
[63]
Wang YF, Yang F, Xiao P. Role and determining factor of substitutional defects on thermal conductivity: A study of La2(Zr1−xBx)2O7 (B = Hf, Ce, 0 ≤ x ≤ 0.5) pyrochlore solid solutions. Acta Mater 2014, 68: 106–115.
[64]
Yang F, Zhao XF, Xiao P. Thermal conductivities of YSZ/Al2O3 composites. J Eur Ceram Soc 2010, 30: 3111–3116.
[65]
Zhang P, Feng YJ, Li Y, et al. Thermal and mechanical properties of ferroelastic RENbO4 (RE = Nd, Sm, Gd, Dy, Er, Yb) for thermal barrier coatings. Scripta Mater 2020, 180: 51–56.
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Publication history

Received: 28 November 2022
Revised: 20 January 2023
Accepted: 27 January 2023
Published: 14 March 2023
Issue date: April 2023

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© The Author(s) 2023.

Acknowledgements

We acknowledge the financial supports from the National Natural Science Foundation of China (Nos. 52032001 and 52211540004) and the Fundamental Research Funds for the Central Universities (No. 2232021A-01).

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