Typical structures and thermal expansion coefficients of ABO4-type (A=Ga, In, Cr; B=Nb, Ta) oxides as EBC candidates

Guiyu Xue; Lin Chen; Luyang Zhang; Jiankun Wang; Jing Feng

doi:10.1016/j.exm.2024.12.002

›› 2025, Vol. 1 ›› Issue (1) : e0002 DOI: 10.1016/j.exm.2024.12.002

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Typical structures and thermal expansion coefficients of ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides as EBC candidates

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Abstract

It is of great significance to search oxide thermal/environmental barrier coatings (T/EBCs) with high working temperatures and thermal expansion coefficients (TECs) matching to different substrates. ABO₄-type oxides have been widely studied due to their high working temperatures, adjustable TECs, and low thermal conductivity. In this work, ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides are studied as EBC candidates based on their relatively low TECs. The influences of crystal structures, distortion degree, types of polyhedrons, as well as the A- and B-site ionic radii and atomic weights on TECs are discussed. It is found out that the TECs of ABO₄-type oxides are not depended on one single factor, and reducing A-site ionic radius may be a good way to decrease their TECs. Based on the TECs, AlNbO₄, InNbO₄, and GaTaO₄ are chosen as EBCs for C-, SiC-, and Al₂O₃-based substrates, respectively. The similar TECs between ABO₄-type oxide EBCs and substrates are beneficial for reducing interfacial thermal stress, which is good for their long-term applications. This work shows that the applications of ABO₄-type oxides can be expanded by effectively regulating TECs.

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Keywords

Environmental barrier coatings / Thermal expansion coefficients / Distortion degree / Thermal stress

Highlight

1.	This work screens ABO₄-type oxides as T/EBCs for different substrates.
2.	Changing the A-site ionic radius is a good way to regulate TECs of ABO4-type oxides.
3.	AlNbO₄, InNbO₄, and GaTaO₄ are chosen as EBCs for C-, SiC-, and Al₂O₃-based substrates, respectively.

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Guiyu Xue, Lin Chen, Luyang Zhang, Jiankun Wang, Jing Feng. Typical structures and thermal expansion coefficients of ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides as EBC candidates. , 2025, 1(1): e0002 DOI:10.1016/j.exm.2024.12.002

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1. INTRODUCTIONS

Protective coatings are widely used on surface of various materials, including Ni-, Nb-, and Ti-based alloys [1 ⇓-3], SiC [4,5], C [6,7], Al₂O₃ [8,9], and so on. The functions of protective coatings are different, which are relied on the demands of multifarious substrates. For example, thermal barrier coatings (TBCs) are used to provide thermal insulation for Ni-based alloys to boost their working temperatures and life time [1,2,10 ⇓-12]. Accordingly, high working temperatures and low thermal conductivity are necessary for TBCs [13]. Environmental barrier coatings (EBCs) are used to insulate high-temperature steam and air for C and SiC substrates because these two substrates are severely corroded by the high-temperature steam and air, and their properties and life time are dramatically reduced after the corrosions [4,7,14 ⇓-16]. To prolong the life time of various substrates, numerous materials are studied as protective coatings for alloy and ceramic substrates, and TBCs and EBCs are extensively investigated during the past decades. The typical structures of TBCs and EBCs consist of four parts, including top coat (TC) oxide ceramics, bond coat (BC), thermal growth oxides (TGO), and substrates [17]. The TGO is formed after the high-temperature service of TBC and EBC systems because their BC (MCrAlY and Si, respectively) will be oxidized to for Al₂O₃ and SiO₂, respectively [17 ⇓-19]. It is noted that BC and substrates usually have similar thermal expansion coefficients (TECs) to reduce thermal stress between their interfaces, and great thermal stress will be triggered at the interfaces between TC and BC due to their differences in TECs and mechanical properties [17,20,21]. The great interfacial thermal stress between TC and BC is one of the main reasons leading to failures of TBCs and EBCs, subsequently, searching materials with TECs matching to different substrates is essential for the applications of protective coatings.

The working temperatures of alloys and TBCs are limited attributed to the relatively low melting points of Ni-based alloys (<1500 ºC), and EBCs are vastly studied for ceramic matrix composites (CMCs) of SiC, C, and Al₂O₃ based on their high working temperatures (1500~3000 ºC), low density, excellent mechanical properties, and other advantages [22 ⇓-24]. Current EBCs are RE₂SiO₅ and RE₂Si₂O₇ (RE is rare-earth elements), which have excellent chemical compatibility with SiO₂ and relatively low TECs [4,14,25 ⇓-27]. RE₂SiO₅ and RE₂Si₂O₇ are corroded by high-temperature steam and CaO-MgO-AlO_1.5-SiO₂ (CMAS), which lead to their failure, and novel EBC materials with adjustable TECs are needed for different CMCs. Oxide tantalates are widely studied as protective coatings materials [1,10,11,28 ⇓-30], while their density is high and price is expensive, and their price is several times of those of YSZ, RE₂SiO₅, and RE₂Si₂O₇. A high density leads to a large centrifugal force, while a high price is unacceptable for industrial applications. Previous studies show that ABO₄-type tantalates have the lowest TECs among various tantalates, and their TECs can be further regulated to match to those of different CMCs, indicating their great potential as EBCs [31 ⇓-33]. To reduce the density and price of tantalates, two ways can be tried. First, other elements can be used to replace RE elements, such as Al, In, Ga, and Cr. Second, Nb can be used to replace Ta because the price of Nb₂O₅ is approximately one-tenth of that of Ta₂O₅. Furthermore, AlMO₄ (M=Nb, Ta) and CrTaO₄ have advantages of low TECs, high melting points and toughness (1.9~2.6 MPa·m^1/2), as well as excellent high-temperature stability, implying their potential as EBCs [10,30].

Accordingly, this work studies the typical structures and TECs of ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides as candidate EBCs. Also, the TECs and structures of AlTaO₄ and AlNbO₄ are discussed for comparisons, which have been reported in our previous study [30]. Thus, the experiments of AlTaO₄ and AlNbO₄ are not repeated in this work. TECs matching to CMCs are essential for EBCs, and they are mainly dominated by crystal structures and an-harmonic vibrations of latices. We analysis the changes of TECs of ABO₄-type oxides from the aspects of crystal structures, cationic coordination, and characteristics of A-site cations. The results show that GaTaO₄, InNbO₄, and AlNbO₄ are candidate EBCs for Al₂O₃, SiC, and C, respectively, based on their TECs. Furthermore, the thermal stress between interface of GaTaO₄/Al₂O₃, InNbO₄/SiC, and AlNbO₄/C is estimated, which can service for their subsequent engineering applications.

2. EXPERIMENTS AND METHODS

2.1 Materials synthesis

ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides were synthesized via a solid-state reaction, and A₂O₃ (A=Ga, In, Cr) and B₂O₅ (B=Nb, Ta) oxides with purity beyond 99.99% were used as raw materials, which were from MACKLIN company. The A₂O₃ and B₂O₅ oxides were weighted based on their chemical ratio, and then ball milled within C₂H₅OH at a speed of 300 rpm for 10 h. The mixtures were further held at 100 ºC for 10 h, and the dried mixtures were compresses as discs with a height of 1.5 mm and diameter of 15 mm, and finally sintered at 1300~1600 ºC for 10 h to obtain samples.

2.2 Structural characterizations

The crystal structure was identified using an X-ray diffraction device (XRD, MiniFlex 600, Rigaku, Japan), and the Rietveld refinement was conducted to obtain the detail lattice constants. The grains were observed using a scanning electronic microscope (SEM, JSM-7800F, JEOL, Japan), and elemental distributions were detected using an electronic probe microanalysis (EPMA, 1720H, Shimadzu, Japan).

2.3 Measurements of TECs

TECs were measured using a thermal expansion device (DIL402, Netzsch, Germany) at 30~1200 ºC with a heating rate of 5 ºC·min^-1. The sample was cut as a cuboid with a dimension of approximately 1×2×10 mm³ before the TECs measurements. The raw length was denoted as L₀, the length at high temperatures T was denoted as L_T, and the TECs at temperature T were calculated as:

(1)

T E C s = L T - L 0 T - 30 · L 0 - 1

3. RESULTS AND DISCUSSION

3.1 Crystal structures

Figs. 1(A)~(C) show the XRD patterns and the corresponding standard PDF cards of the studied ABO₄-type oxides, and it is confirmed that CrTaO₄ and CrNbO₄ are crystallized into a tetragonal phase (t), which agree well with CrTaO₄ reported in S. Zhang’s work [10]; while the rest are crystallized into a monoclinic phase (m). GaTaO₄ and GaNbO₄ have different crystal structures, and InTaO₄ and InNbO₄ have a same crystal structure. The XRD patterns of GaNbO₄ are slightly different from those of PDF#16-0739 due to existences of Ga₂O₃. Some minor peaks are not obvious in Fig. 1(A) and (B) for GaTaO₄, InTaO₄, and InNbO₄ due to their relatively low intensities. The changes of both A- and B-site elements result in a variation in crystal structures of ABO₄-type oxides, and a similar phenomenon is detected in their TECs in subsequent parts. The detail lattice constants are obtained from their XRD Rietveld refinements shown in Figs. 1(D)~(I). Table 1 shows that GaNbO₄ has a monoclinic crystal structure far different from those of GaTaO₄, InNbO₄, and InTaO₄, whereas it is similar to those of AlTaO₄ and AlNbO₄ [30]. Fig. 2 shows the crystal structures, and GaNbO₄ may has a higher distortion degree of polyhedrons than others. It can be seen that both A- and B-site cations are coordinated by six oxygen atoms to form [AO₆] and [BO₆] octahedrons, which is the same as the situations of AlTaO₄ and AlNbO₄ [30].

Table 1 lists that CrNbO₄ and CrTaO₄ have the smallest unit cell volume, and the volume of GaNbO₄ is approximately twice of those of GaTaO₄, InTaO₄, and InNbO₄. The changes in crystal structures also affect their distortion degree, structural stability, and TECs. The distortion degrees (Δd) of [AO₆] and [BO₆] polyhedrons are further determined by the A-O and B-O bond lengths (l) [34,35].

(2)

Δ d = 16 ∑ 6 (l i - L L) 2

Where l_i is the length of the i^th bond, and L is the mean bond length. AlTaO₄ and AlNbO₄ have the total distortion degree of 3.45% and 1.76%, respectively [30]; and RETaO₄ have a total distortion degree less than 0.4% [36]. Table 2 lists that GaNbO₄ has the highest distortion degree (10.13%) among the studied oxides, which is much higher than those of RETaO₄, AlTaO₄, and AlNbO₄. GaTaO₄, InTaO₄, and InNbO₄ have distortion degrees similar to those of RETaO₄, while CrTaO₄ and CrNbO₄ have a distortion degree less than 0.01% due to their high-symmetry tetragonal phase. A high distortion degree may lead to high TECs and affect their high-temperature stability, and it will be discussed below.

3.2 Microstructures

Fig. 3 shows the grains and elemental distributions of ABO₄-type oxides, and they have micron-scale grains. CrNbO₄ has much smaller grains than GaNbO₄, which is caused by the different sintering temperatures. Some grains of GaNbO₄ are bigger than 20 μm, while most grains of CrNbO₄ are less than 10 μm. The sintering temperature of GaNbO₄ is 1300 °C, which is close to its melting point (1425 °C), and leads to a large grain size. Due to the changes of elements, the sintering temperatures of ABO₄-type oxides are stretched from 1300 to 1600 ºC, and their relative density is higher than 90%. Figs. 3(D)~(G) show elemental distributions of InNbO₄ obtained from EPMA, and each element is even within the grains, while O is relatively rare in the grain boundaries due to its small atomic number. Also, the grain boundary usually has a lower altitude than the grains, which reduces the detected signal of each element. Accordingly, ABO₄-type oxides are successfully synthesized in this work, which can be used for various measurements.

3.3 Thermal expansion properties

Fig. 4(A) shows the thermal expansion rate of each sample, including AlNbO₄ and AlTaO₄, which increases with the increasing temperature, except GaNbO₄ and AlNbO₄. An obvious reduction in thermal expansion rate is found in AlNbO₄ and GaNbO₄ at temperatures higher than 1150 and 1100 ºC, respectively, which is caused by their relatively low melting points. AlNbO₄ and GaNbO₄ have a melting point of 1540 ºC and 1420 ºC [37,38], respectively, and other ABO₄-type oxides have higher melting points. The changes of TECs of ABO₄-type oxides are shown in Fig. 4(B). The TECs of GaNbO₄ decrease slightly at 900~1100 °C, while they decrease dramatically at 1100~1200 °C. GaNbO₄ has the lowest melting point among the studied oxides, and high temperatures will soften GaNbO₄ to reduce its TECs. GaTaO₄ has the highest TECs (8.23×10^-6 K^-1, 1200 ºC) among the studied oxides, which approaches those of Al₂O₃ CMCs (8.80×10^-6 K^-1), and its TECs increase with the increasing temperature. Except AlNbO₄ and GaNbO₄, the TECs of other ABO₄-type oxides are 5.32~8.23×10^-6 K^-1 at 1200 ºC, which are suitable for EBC applications for different CMCs. C-, SiC-, and Al₂O₃-based CMCs have TECs of approximately 3.5×10^-6 K^-1, 5.4×10^-6 K^-1, and 8.8×10^-6 K^-1 at 1200 ºC, respectively as shown in Fig. 4(C) [39 ⇓-41]. The thermal stress between oxide EBCs and substrates is dominated by TECs, and it is obvious that AlNbO₄, InNbO₄, and GaTaO₄ are potential EBCs for C-, SiC-, and Al₂O₃-based CMCs, respectively.

TECs are affected by bonding strength, distortion degree of polyhedrons, and types of polyhedrons, and we discuss the dominant factors of TECs for ABO₄-type oxides from above aspects. For ABO₄-type oxides with an m phase, ANbO₄ have lower TECs than ATaO₄ as shown in Fig. 4(C). AlTaO₄ has a higher modulus (E=243.3 GPa) and Debye temperature (T_D=540 K) than AlNbO₄ (E=77.8 GPa and T_D=369 K) [30]. The higher of modulus and Debye temperature, the stronger of bonding strength, which may restrict vibrations of lattices [42,43]. The niobates usually have lower modulus than tantalates, indicating that TECs are not dominated by their bonding strengths in ABO₄-type oxides. The relationship between polyhedron and TECs can be estimated based on Hazen’s and Prewitt’s theory, which is related to the coordination number (P) and cation charge (Z) [28,44,45].

(3)

M T E C s = 32.9 0.75 - Z P × 10 - 6 K - 1

Where M_TECs means the TECs of A-O and B-O bonds in this work. Both A³⁺ and B⁵⁺ cations are coordinated by six oxygen atoms to form [AO₆] and [BO₆] polyhedrons as shown in Fig. 4(D), and Eq. (3) indicates that A-O bonds have higher TECs (M_TECs=8.23×10^-6 K^-1) than B-O bonds (M_TECs=-2.74×10^-6 K^-1). It is clear that A-site cations have significant effects on TECs of ABO₄-type oxides. Two oxygen atoms are shared by [AO₆] and [BO₆] polyhedrons in ABO₄ (A=Al, Cr; B=Nb, Ta) oxides, while only one oxygen atom is shared by [AO₆] and [BO₆] polyhedrons in the rest oxides, this difference in crystal structures also affect their TECs. The ionic radii of A-site cations are listed as Al (0.053 nm) < Cr (0.061 nm) < Ga (0.062 nm) < In (0.080 nm), when Ta and Nb have the same ionic radii of 0.064 nm. The bonding lengths and strengths are affected by their ionic radii. Table 2 lists that GaNbO₄ has the highest distortion degree, which reduces its high-temperature stability, and leads to the lowest melting point among the studied oxides. A high distortion degree may lead to high TECs, while this is not the case for current study. GaTaO₄, InTaO₄, and InNbO₄ have similar distortion degree, while their TECs are far different from each other. Accordingly, TECs of the studied oxides are not dominated by a single factor.

To further investigate the dominators of TECs for ABO₄-type oxides, we compare the TECs of RENbO₄, RETaO₄, and ABO₄-type oxides without RE elements as shown in Fig. 5 [36,46]. The influenced factors include the A-site ionic radius and atomic weight (M), as well as A/B ionic radius (ΔR) and atomic weight (ΔM) ratio. The dependence between TECs and above factors can be indicated by the Pearson’s coefficient (r). Fig. 5(A) shows that the studied ABO₄-type oxides have lower TECs than most RETaO₄ and RENbO₄, and TECs increase with the increasing A-site ionic radius. The Pearson’s coefficient between TECs and R is 0.824, which is higher than that (r=0.642) between TECs and A-site atomic weight as shown in Fig. 5(B). The relationships shown in Figs. 5(C) and (D) are similar with those shown in Figs. 5(A) and (B), respectively. The dependence between A-site ionic radius and TECs is the highest in present discussion. In RETaO₄ and RENbO₄, TECs decrease with the decreasing RE³⁺ ionic radius because the lanthanide contraction will shorten the RE-O bond lengths and increase their bonding strength, which restricts the vibrations of lattices to reduce TECs [36,46].

For the studied ABO₄-type oxides, their crystal structures and elements are far different from each other, and it is difficult to dominate their TECs based on one single factor. Current results indicate that reducing A-site ionic radius may further reduce TECs of ABO₄-type oxides, which can boost their applications as EBCs. AlNbO₄, InNbO₄, and GaTaO₄ are potential EBCs for C-, SiC-, and Al₂O₃-based CMCs, respectively, according to their TECs. The relatively low TECs of ABO₄-type oxides can reduce the interfacial thermal stress between oxide EBCs and CMCs.

3.4 Interfacial thermal stress

Thermal stress (σ) between interface of T/EBCs and substrates can be estimated based on their differences in TECs (ΔTECs) and temperatures (ΔT), as well as modulus (E) and Poisson’s ratio (ⅴ) [47,48].

(4)

σ = E 1 - ⅴ · Δ T E C s · Δ T

Eq. (4) shows that the thermal stress is proportional to ΔTECs, ΔT, and E. Also, T/EBCs and substrates are subjected to different thermal stress due to their discrepancies in modulus and Poisson’s ratio [10,49 ⇓-51]. Based on Eq. (4) and the relevant parameters of ABO₄-type oxides and different CMCs, Fig. 6 shows the thermal stress between the interface of GaTaO₄/Al₂O₃, InNbO₄/SiC, and AlNbO₄/C with a temperature difference of 50 ºC. Fig. 6(A) shows the set parameters for calculations of thermal stress, and the thickness of EBCs and CMCs is 300 μm. Figs. 6(B)~(D) show that ABO₄-type oxides are subjected to tensile stress, while CMCs are subjected to compressive stress. Thermal stress in InNbO₄/SiC and AlNbO₄/C systems is less than 10 MPa because the EBCs and CMCs have similar TECs. In GaTaO₄/Al₂O₃ systems, the thermal stress is relatively high, however, it is still lower than 100 MPa. Previous researches show that the interfacial thermal stress in T/EBC systems can be as high as 1~2 GPa before their failure [17,52]. It can be seen that the adjustable TECs of ABO₄-type oxides are favorable for their T/EBC applications.

4. CONCLUSIONS AND PERSPECTIVE

This work focuses on the typical structures and thermal expansion properties of ABO₄-type (A=Ga, In, Cr; B=Nb, Ta) oxides as potential EBC candidates, and the interfacial thermal stress is estimated based on their TECs and mechanical properties. It is found out that the A-site elements and their ionic radii have vital effects on their TECs, and reducing A-site ionic radius may be a good way to reduce their TECs. The TECs do not merely rely on one single factor, such as crystal structure, distortion degree of polyhedrons, ionic radius, or types of polyhedrons. Based on their TECs, AlNbO₄, InNbO₄, and GaTaO₄ are potential EBCs for C-, SiC-, and Al₂O₃-based CMCs, respectively. The similar TECs in GaTaO₄/Al₂O₃, InNbO₄/SiC, and AlNbO₄/C systems are beneficial for reducing thermal stress, which is favorable for their EBC applications. Multifunctional T/EBCs are widely required in various fields, and thermal insulation performance and CMAS corrosion resistance are also vital for their applications, which will be reported in the following studies. Also, to further regulate their TECs and optimize properties, the high-entropy engineering can be tried in the future studies.

Declaration of interest statement

The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

ACKNOWLEDGEMENTS

Thanks for supports from Yunnan Major Scientific and Technological Projects (NO. 202302AG050010), the Academician (Expert) Workstation of Yunnan Province Program (NO. 202305AF150005), and Project of Innovation Team in Yunnan Province (NO. 202305AS350018).

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