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Article

A Promising High-Entropy Thermal Barrier Material with the Formula (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12

1
Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
2
University of Chinese Academy of Sciences, Beijing 100049, China
3
Xiamen Key Laboratory of Rare Earth Photoelectric Functional Materials, Xiamen Institute of Rare Earth Materials, Haixi Institute, Chinese Academy of Sciences, Xiamen 361021, China
4
Nuclear Power Institute of China, The Key Nuclear Fuel and Nuclear Materials Laboratory of China, Chengdu 610213, China
5
Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China, Fuzhou 350108, China
6
Fujian Province Joint Innovation Key Laboratory of Fuel and Materials in Clean Nuclear Energy System, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, Fuzhou 350002, China
7
Advanced Energy Science and Technology Guangdong Laboratory, Huizhou 516003, China
*
Authors to whom correspondence should be addressed.
Materials 2022, 15(22), 8079; https://doi.org/10.3390/ma15228079
Submission received: 30 September 2022 / Revised: 7 November 2022 / Accepted: 8 November 2022 / Published: 15 November 2022

Abstract

:
YSZ has been widely used as a TBC material, but its phase change at high temperatures limits its development, thus the need for developing new thermal barrier materials resistant to high temperatures. Rare-earth aluminate ceramics with a garnet structure (Yb3Al5O12) have been considered as a potential thermal barrier material. The melting point of Yb3Al5O12 is 2000 °C, which has a potential high temperature application prospect. However, Yb3Al5O12 has lower thermal expansion and higher thermal conductivity than YSZ, which is a widely employed thermal barrier coating (TBC) material. To overcome these obstacles, (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, a high-entropy ceramic, was prepared by a solid-state reaction and pressureless sintering. The thermal conductivity of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was 3.48 W/(m·K) at 300 K, approximately 25.48% lower than that of the Yb3Al5O12 (4.67 W/(m·K)). The thermal expansion coefficient of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was 9.28 × 10−6 K−1 at 673-1273 K, approximately 18.52% higher than that of the Yb3Al5O12 (7.83 × 10−6 K−1, 673-1273 K). When the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was annealed at 1550 °C for 7 days, its average grain size only increased from 0.7 μm to 1.3 μm. Moreover, the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 exhibited better chemical stability and a lower grain growth rate than the Yb3Al5O12. This study reveals that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 is a promising candidate for the future generation of thermal barrier materials.

1. Introduction

Thermal barrier coatings (TBCs) are widely employed in gas turbine engines for aerospace, power generation, and marine applications and can protect the superalloy by reducing the alloy surface temperature and increasing the engine efficiency of gas turbines [1,2,3,4,5,6]. TBCs must be able to withstand extreme temperature cycling and thermal shock [7,8,9]. Therefore, the selection of TBCs is restricted by some basic requirements: (1) excellent high-temperature stability, (2) a thermal expansion coefficient (TEC) consistent with the metallic substrate, (3) a low grain growth rate, (4) low thermal conductivity, and (5) chemical inertness. To date, YSZ has been widely employed as a TBC material, but the limitations of phase transformation at a high temperature and high oxygen diffusivity make it unsuitable for the high operating temperature of gas turbine engines [10,11]. At high temperatures, the non-equilibrium tetragonal phase in YSZ is prone to decomposition to generate t-phase and c-phase, and the cumulative effect of the volume expansion due to the phase change will cause cracks in the coating. Moreover, oxygen ions from YSZ above 800 °C tend to oxidize the metal substrate through the coating [12,13,14]. Therefore, YSZ cannot serve for a long time at temperatures above 1200 °C. Thus, novel TBC materials with better high-temperature stability are urgently needed.
The physicochemical properties of rare-earth elements have made them a research priority in the field of thermal barrier coatings [15,16,17]. Wang et al. reported that the thermal barrier coating of La1.4Nd0.6Zr2O7(LNZ) on a Mo substrate was prepared by air plasma spraying with a self-developed LNZ thermal spray powder [18]. Xu et al. reported that (Sm0.2La0.8)2(Zr0.7Ce0.3)2O7 (SmLZC), as a candidate material for novel thermal barrier coatings, was prepared by electron beam-physical vapor deposition (EB-PVD) [19]. Thus, rare-earth oxides exhibit good feasibility in the field of thermal barrier coatings. Therein, Yb3Al5O12 exhibits excellent high-temperature stability, isotropic elastic properties, and low intrinsic thermal conductivity and has recently been recognized as a potential thermal barrier material [20,21,22,23]. The melting point of Yb3Al5O12 is 2000 °C, which has a potential high-temperature application prospect. Moreover, theoretical results obtained by Klemm confirmed that Yb3Al5O12 has better chemical stability than several other promising TBCs, such as Y2Si2O7 and Yb2Si2O7 [24]. However, Yb3Al5O12 has lower expansion and higher thermal conductivity than YSZ, which is a widely used TBC material [22]. The linear thermal expansion of Yb3Al5O12 was in the range from 298 to 1273 K, 7.83 × 10−6 K−1, which was lower than that of YSZ ((10-11) × 10−6 K−1). The measured thermal conductivities of Yb3Al5O12 at 300 and 1400 K are 4.67 W/(m·K) and 2.05 W/(m·K), which were greater than those of YSZ. Thus, decreasing the thermal conductivity of Yb3Al5O12 and increasing the coefficient of thermal expansion of Yb3Al5O12 are critical to expanding its applications.
Currently, the emergence of high-entropy ceramics (HECs) has attracted attention [25,26,27,28,29,30]. It has been reported that HECs efficiently enhance the thermal performance of thermal barrier materials because they have higher temperature stability, more consistent TECs, and a slower grain growth rate than single-component compounds. Lattice distortion and component disorder can increase phonon scattering and thus reduce thermal conductivity. In addition, better chemical stability can be achieved due to retarded diffusion. Some researchers have successfully synthesized different kinds of high-entropy oxides (HEOs) for TBC applications. An increase of 6 h in annealing results in only a 1 μm increase in grain size for (5RE0.2)Ta3O9, while this increases to approximately 3 μm for EuTa3O9 [31]. Sun et al. reported that the thermal conductivities of (Eu0.2Er0.2Lu0.2Y0.2Yb0.2)2O3 and (Sm0.2Er0.2Lu0.2Y0.2Yb0.2)2O3 are 5.10 W/(m·K) and 4.60 W/(m·K), which are 23.8% and 21.5% of that of Y2O3 (21.40 W/(m·K)), respectively [32]. Ren et al. prepared (Y1/4Ho1/4Er1/4Yb1/4)2SiO5 silicate as a multifunctional TBC material, and it showed good resistance to high-temperature water vapor [33]. In addition, due to the excellent properties of HECs, Chen et al. reported a high-entropy rare-earth aluminate (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12 [34]. Thus, HECs can effectively enhance the combined properties of thermal barrier materials.
Herein, we design and synthesize a promising high-entropy rare-earth aluminate ceramic with garnet, (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, by the solid-state reaction method. The standards for the component design are as follows: (1) to guarantee the formation of solid solutions, differences in the size of the rare-earth ions must not be greater than 15.0%; (2) each component must have the structure of garnet; and (3) no phase change may occur at the working temperature. In addition, in terms of the selected elements, we try to use low-cost rare-earth elements to further reduce the economic problem. The thermal expansion coefficient, thermal conductivity, high-temperature stability, chemical inertness and hardness of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 are studied in the present work. These properties are valuable and beneficial to the potential application of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 as the future generation of thermal barrier materials.

2. Experimental Section

2.1. Synthesis of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12

Y2O3 (99.99%), Dy2O3 (99.99%), Ho2O3 (99.99%), Er2O3 (99.99%), Yb2O3 (99.99%), and Al2O3 (99.999%) were purchased from Aladdin Reagent Ltd., Co. (Shanghai, China). Figure 1 shows the synthesis of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 via a solid-state reaction. The total molar ratio of rare-earth elements to Al was 3:5. First, five rare-earth oxides with equal molar ratios were mixed with Al2O3 and alcohol, and ground at 360 r/min for 10 h using a planetary ball mill. Afterward, the obtained solution was dried in an oven at 80 °C for 10 h. The obtained powder mixture was pressed and molded at 5 MPa. Afterwards, the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powders were synthesized by sintering at 1600 °C for 2 h. The as-prepared powder was ball-milled for 10 h and then dried and sieved through a 400 mesh sieve to obtain fine particles. The samples were densified by the pressureless sintering method. The process of cold isostatic pressing is that the powder is pressed through a mold, then pressed again in a cold isostatic press at a pressure of 200 MPa to make itself more dense, and then calcined in a muffle furnace at a temperature of 1650 °C for 5 h. Finally, the densified bulk samples can be obtained.

2.2. Characterization of the Materials

A scanning speed of 2°/min was used for X-ray diffraction (XRD, Miniflex 600 instrument, Tokyo, Japan) with Cu Kα radiation to determine the phase structure of the powder samples. Scanning electron microscopy (SEM, Apreo S LoVac Thermo Fisher Scientific, Waltham, MA, USA) was combined with field-emission transmission electron microscopy (TEM, FEI/Talos F200X G2, Lincoln, NE, USA) and energy-dispersive spectrometry (EDS) to examine the morphology and chemical composition of the samples. The TEC of the bulk samples was determined by a thermal expansion meter (Cryoall C15V, Beijing, China) with a size of Φ 30.0 mm × 2.0 mm. The thermal conductivity of the bulk samples was examined by a thermal constant analyzer (TPS 2500, Hot Disk, Göteborg, Sweden) with a size of Φ 6.0 mm × 10.0 mm. The thermal conductivities of the dense materials were corrected by the following Formula (1) [35].
K S K = 1 1.5 P
where KS is the thermal conductivity obtained by the test, K is the thermal conductivity of the fully dense materials, and P is the porosity.
A Vickers hardness test was conducted using a micro hardness tester (FT FM-700, Tokyo, Japan). The samples for Vickers hardness testing were cut by a diamond saw from the as-prepared bulk material and then polished down to 1.0-μm diamond grits. The Vickers hardness number was determined by a microhardness tester with loads of 1, 3, 5, and 10 N, respectively. Loads of 1, 3, 5, and 10 N were applied with a dwell time of 15 s. The Vickers hardness tests were calculated by using Formula (2).
H v = P / S = 2 P sin θ 2 / d 2 = 1854.4 P / d 2
where P is the load, and d is the diagonal length of indentation. Five measurements for each load were taken to obtain the average value of hardness.
The cell dimension was calculated by the Rietveld refinement using GSAS software (EXPGUI-GSAS), and the reliability factors of Rp and Rwp were calculated by using Formulas (3) and (4) [36].
R p = | Y o i Y c i | / Y o i
R w p = W i Y o i Y c i 2 / W i Y 2 o i 1 / 2
The Archimedes method was used to measure the bulk density (ρ), while Formula (5) was used to calculate the theoretical density.
ρ t h = m / v
where m is the mass of a unit cell of HE-RE3Al5O12 and V is the cell volume. The relative density was calculated from the ratio of the actual density to the theoretical density (ρ/ρth).
The concentrations of dissolved ions in the leachates were determined by inductivity-coupled plasma mass spectrometry (ULTIMA 2, Horiba Jobin Yvon S.A.S, Edison Township, NJ, USA). A leaching test of the bulk samples by atmospheric pressure sintering at 1640 °C for 5 h was performed in a nitric acid solution in PTFE for 1–5 d. The HE-RE3Al5O12 ceramics, which had a diameter of 15 mm and a height of 2 mm, were polished, cleaned, and dried. The ratio of the geometric surface area of the sample to the volume of the leachate was maintained at 1:10 cm−1. The normalized element mass leaching rates (LRi) of the (Al) were obtained based on Formula (6) [37].
L R i = C i · V / f i · S · t
where Ci is the concentration of elements (Al) in the leaching solution, V is the volume of the leaching solution, fi is the proportion of element I in the ceramic, S is the surface area of the ceramic, and t is the date of leaching.

3. Results and Discussion

Figure 2a shows the XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at different temperatures (1500 °C, 1550 °C, 1600 °C). As can be seen from Figure 2a, when the synthesis temperature is 1500 °C or 1550 °C, impurity phases are (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)AlO3 and Al2O3. Figure 2b shows the XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at 1600 °C for 2 h, with those of the single-component RE3Al5O12 (RE = Y, Dy, Ho, Er, Yb) obtained from JCPDF cards. As can be seen from Figure 2b, when the green bodies were heated to 1600 °C in ai with a dwell time of 2 h, no other impurity peak phase is observed. The XRD patterns of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powder matched those of a single component, indicating that the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 synthesized in this study had the same structure as a single component. No other contaminants were indicated by the diffraction peaks, confirming that a solid solution was prepared. Thus, a pure-phase (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 solid solution was successfully prepared. Figure 3a shows the XRD patterns of the calcined powder and the sintered solid. The XRD patterns were consistent before and after calcination, indicating that no impurities were introduced. The absence of holes and cracking can be seen in the SEM image in Figure 3b, indicating that the sintered (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 exhibited a high relative density.
As shown in Figure 4, the cell dimension of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was calculated by the Rietveld refinement using GSAS software, and the reliable factors calculated via the equations are Rp = 3.38% and Rwp = 4.41%. The refinement results are generally considered reliable for values of Rp and Rwp below 10.00%. The (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramic lattice parameters were found to be a = b = c = 11.992 Å, which is approximately equal to the average cell size of the five single components (11.986 Å). Table 1 shows the refined cell dimensions and theoretical density of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and the five single-component garnets obtained from jade. The theoretical density of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was 6.02 g/cm3, based on the refined cell parameters. The sintered density, calculated by Archimedes’ approach, is 5.88 g/cm3, 97.67% of the theoretical value (6.02 g/cm3).
Figure 5 shows the high-angle annular dark-field (HAADF) image and element mapping of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powders. The distribution of elements is clearly uniform, demonstrating the uniformity of the solid solution. The XRD and TEM–EDS results suggest that single-phase aluminates with excellent chemical uniformity were synthesized by the solid-state reaction approach. Figure 6a shows that the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics were further characterized by HR-TEM. Two positions were selected to calculate the lattice fringes, which exhibited typical (211) and (420) lattice planes with D-spacings of 0.488 nm and 0.267 nm, respectively. These results are consistent with the broad XRD peaks of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at 18.2° (0.48665 nm, (211)) and 33.5° (0.26662 nm, (420)). The selected area electron diffraction (SAED) pattern of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powders (Figure 6b) shows that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 has a single-crystal ordered garnet structure.
Thermal conductivity is essential for assessing the thermal insulation properties of insulating materials. Table 2 shows the thermal conductivity of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12, and Y3Al5O12 at 300 K. The thermal conductivity of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics was found to be 3.48 W/(m·K) at 300 K, approximately 25.48% and 8.66% lower than that of Yb3Al5O12 (4.67 W/(m·K)) and (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12 (3.81 W/(m·K)), indicating that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 is a potential thermal barrier material [32]. The thermal conductivities of rare-earth aluminates are slightly higher than commercial TBC material YSZ, which is 2.50–3.20 W/(m·K) [38]. Five equimolar rare-earth cations are present in (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at crystallographic sites randomly occupying the same lattice. The mismatch between the masses and radii of these cations leads to large lattice distortions and intense phonon scattering in the material. Among the four core effects of high-entropy materials is lattice distortion, which may play a significant role in the decrease in the thermal conductivity of garnets [39].
Thermal barrier materials need to possess a coefficient of thermal expansion similar to that of a high-temperature alloy matrix because a thermal expansion mismatch can cause cracking of the matrix. Figure 7 shows the curves of the linear thermal expansion of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, determined from room temperature to 1273 K. The relative changes in the length of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 samples were recorded with the increasing temperature.
In addition, the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was designed using a pressureless sintering method, with a coefficient of thermal expansion of 9.28 × 10−6 K−1 at 673–1273 K, approximately 18.52% higher than that of Yb3Al5O12 (7.83 × 10−6 K−1, 673–1273 K), and approximately 8.67% higher than that of (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12 (8.54 × 10−6 K−1, 673–1273 K); thus, this material can be applied to various substrates, such as typical high-temperature nickel-based alloys [40].
A low grain growth rate is very important for TBC materials, as it improves the crack resistance due to thermal stress and prevents an increase in thermal conductivity. Figure 8 shows the average grain sizes of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramic specimens after annealing at 1550 °C for 7 days. As seen in Figure 8, the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics have a lower average grain rate than the Yb3Al5O12 and Er3Al5O12. The grain growth rates of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, Yb3Al5O12, and Er3Al5O12 samples were similar during the annealing period of 0-5 days at 1550 °C. However, when the annealing time was extended to 7 days, the grain growth rate of the high-entropy aluminate was less than that of the Yb3Al5O12 and Er3Al5O12 under the same conditions. As a result of sluggish diffusion in HECs, (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics grow slowly because fine particles are retained under high temperatures [39].
Thermal barrier materials must have excellent chemical inertness. Figure 9 shows the normalized elemental leaching rates of Al in (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Yb3Al5O12 over 5 days. The elemental aluminum leaching rate of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 remained low during 1–5 days of corrosion in an acidic environment. However, the single-component garnet-structured aluminate ceramics exhibited a large leaching rate of elemental aluminum. This result indicated that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics have better chemical stability than Yb3Al5O12. Therefore, high-entropy aluminate ceramics are promising materials for TBCs.
The mechanical property of a TBC is also important as mechanical damage such as impact or wear can apply to the TBC. The mechanical property data of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 are also listed in Figure 10 as a comparison. As can be seen in Figure 10, the hardness of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 is significantly higher than that of Yb3Al5O12. The hardness of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 is determined to be 13.3 GPa, which is higher than that of Yb3Al5O12 (10.7 GPa), and slightly lower than YSZ (14.0 GPa). The excellent mechanical property data suggest that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 can be used as a potential thermal insulation material.

4. Conclusions

In summary, high-entropy rare-earth aluminate thermal barrier materials with garnet structures, (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics, were prepared by a solid-state reaction method. The results of XRD, SEM, and TEM analysis show that the synthesized (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramic powder consists of a pure phase with a homogeneous rare-earth element distribution, and the lattice dimensions are a = b = c = 11.992 Å. According to the refined dimensions of the cell, the theoretical density of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 was calculated to be 6.02 g/cm3. The sintered density calculated by Archimedes’ approach is 5.88 g/cm3, which is 97.67% of the theoretical value. The thermal conductivity of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 ceramics is 3.48 W/(m·K) at 300 K, approximately 25.48% and 8.66% lower than that of Yb3Al5O12 (4.67 W/(m·K)) and (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12 (3.81 W/(m·K)). The thermal expansion of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 is (9.28 × 10−6 K−1, 673-1273 K)), approximately 18.52% higher than that of Yb3Al5O12 (7.83 × 10−6 K−1, 673–1273 K) and approximately 8.67% higher than that of (Y0.2Yb0.2Lu0.2Eu0.2Er0.2)3Al5O12 (8.54 × 10−6 K−1, 673–1273 K). After annealing the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at 1550 °C, its average grain size was found to be lower than that of Yb3Al5O12 and Er3Al5O12, due to the sluggish diffusion effects. As the annealing time was extended to 7 days, the average grain size of the high-entropy aluminate became much smaller than that of the Yb3Al5O12 and Er3Al5O12 under the same conditions. In addition, (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 has excellent chemical stability compared with Yb3Al5O12. The results show that (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, in comparison with Yb3Al5O12, is a potential thermal barrier material.

Author Contributions

Conceptualization, F.Y.; methodology, Z.L. and J.Z.; software, W.Z. (Wenjuan Zhang) and Y.Z.; formal analysis, Z.L. and W.Z. (Weijun Zhao); investigation, Z.L. and H.C.; data curation, J.Z. and L.X.; writing—original draft preparation, Z.L.; writing—review and editing, H.C.; supervision, F.Y.; project administration, Z.L.; funding acquisition, F.Y. All authors have read and agreed to the published version of the manuscript.

Funding

This work was supported financially by the National Key Research and Development Program of China [Grant No. 2019YFC0605000], the independent deployment project of Fujian Science & Technology Innovation Laboratory for Optoelectronic Information of China [Grant No. 2021ZZ109], the independent deployment project of Ganjiang Innovation Research Institute of Chinese Academy of Sciences [Grant No. E055A002], the key deployment project of the Chinese Academy of Sciences [Grant No. ZDRW-CN-2021-3], the Fujian Provincial Natural Fund Project [Grant No. 2021J05101], and the CAST Young Talent Support Project.

Institutional Review Board Statement

Not applicable.

Informed Consent Statement

Not applicable.

Data Availability Statement

The data presented in this study are available from the corresponding authors upon reasonable request.

Conflicts of Interest

The authors declare no conflict of interest.

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Figure 1. Schematic illustration of the preparation process of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 by the solid-state reaction method and the pressureless sintering method.
Figure 1. Schematic illustration of the preparation process of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 by the solid-state reaction method and the pressureless sintering method.
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Figure 2. (a) XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at different temperatures (1500 °C, 1550 °C, 1600 °C); (b) XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at 1600 °C for 2 h with those of single-component RE3Al5O12 (RE = Y, Dy, Ho, Er, Yb) obtained from JCPDF cards.
Figure 2. (a) XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at different temperatures (1500 °C, 1550 °C, 1600 °C); (b) XRD patterns of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 at 1600 °C for 2 h with those of single-component RE3Al5O12 (RE = Y, Dy, Ho, Er, Yb) obtained from JCPDF cards.
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Figure 3. (a) XRD patterns of calcined powder and the sintered solid; (b) surface SEM image of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12.
Figure 3. (a) XRD patterns of calcined powder and the sintered solid; (b) surface SEM image of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12.
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Figure 4. XRD patterns of the as-synthesized (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powders, together with the Rietveld refinement data.
Figure 4. XRD patterns of the as-synthesized (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 powders, together with the Rietveld refinement data.
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Figure 5. Elemental compositions of Y, Dy, Ho, Er, Yb in HAADF images.
Figure 5. Elemental compositions of Y, Dy, Ho, Er, Yb in HAADF images.
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Figure 6. The power of (a) the high-resolution TEM image and (b) the corresponding SAED pattern.
Figure 6. The power of (a) the high-resolution TEM image and (b) the corresponding SAED pattern.
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Figure 7. The linear thermal expansion coefficient of polycrystalline (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12.
Figure 7. The linear thermal expansion coefficient of polycrystalline (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12.
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Figure 8. Average grain size of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, Er3Al5O12, and Yb3Al5O12 ceramics after annealing at 1550 °C for 7 days in air.
Figure 8. Average grain size of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12, Er3Al5O12, and Yb3Al5O12 ceramics after annealing at 1550 °C for 7 days in air.
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Figure 9. Normalized elemental leaching rates of Al in (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Yb3Al5O12 for 5 days.
Figure 9. Normalized elemental leaching rates of Al in (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Yb3Al5O12 for 5 days.
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Figure 10. Vickers hardness of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Yb3Al5O12 versus load.
Figure 10. Vickers hardness of (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Yb3Al5O12 versus load.
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Table 1. Refined cell size and theoretical density of as-synthesized (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and the five single component garnets.
Table 1. Refined cell size and theoretical density of as-synthesized (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and the five single component garnets.
CompoundsTheoretical Density (g/cm3)Relative Densitya (Å)
(Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O126.0297.70%11.992
Y3Al5O124.56-12.000
Dy3Al5O126.20-12.038
Ho3Al5O126.32-12.000
Er3Al5O126.43-11.962
Yb3Al5O126.62-11.930
Table 2. The thermal conductivity of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Y3Al5O12 at 300 K.
Table 2. The thermal conductivity of the (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12 and Y3Al5O12 at 300 K.
(Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12Yb3Al5O12YSZ
Thermal conductivity (W/(m·K))3.484.672.50–3.20
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Li, Z.; Zheng, J.; Zhang, W.; Zheng, Y.; Zhao, W.; Xue, L.; Yang, F.; Chen, H. A Promising High-Entropy Thermal Barrier Material with the Formula (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12. Materials 2022, 15, 8079. https://doi.org/10.3390/ma15228079

AMA Style

Li Z, Zheng J, Zhang W, Zheng Y, Zhao W, Xue L, Yang F, Chen H. A Promising High-Entropy Thermal Barrier Material with the Formula (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12. Materials. 2022; 15(22):8079. https://doi.org/10.3390/ma15228079

Chicago/Turabian Style

Li, Zhanqiang, Junfeng Zheng, Wenjuan Zhang, Yong Zheng, Weijun Zhao, Liyan Xue, Fan Yang, and Heng Chen. 2022. "A Promising High-Entropy Thermal Barrier Material with the Formula (Y0.2Dy0.2Ho0.2Er0.2Yb0.2)3Al5O12" Materials 15, no. 22: 8079. https://doi.org/10.3390/ma15228079

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