Startseite Wide temperature range protection performance of Zr–Ta–B–Si–C ceramic coating under cyclic oxidation and ablation environments
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Wide temperature range protection performance of Zr–Ta–B–Si–C ceramic coating under cyclic oxidation and ablation environments

  • Xiaoyang Guo , Yuan Tian , Na Wang EMAIL logo und Yan Jiang EMAIL logo
Veröffentlicht/Copyright: 15. Juli 2025
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High Temperature Materials and Processes
Aus der Zeitschrift High Temperature Materials and Processes Band 44 Heft 1

Abstract

In order to improve the oxidation and ablation resistance of carbon materials, Zr–Ta–Si–C–B coatings with different Zr/Ta ratios were successfully prepared on the graphite surface by combining slurry impregnation and reactive melt infiltration (RMI). The coatings after RMI are dense, Zr–Ta–B solid solution, SiC, and Si coexist in the coating where ceramic particles are tightly wrapped by Si. The cycle oxidation test results at 1,600°C for 100 h (5 h × 20 cycles) show that the Zr–Ta–Si–C–B coating with a Zr/Ta ratio of 4:6 has a better anti-oxidation effect; the mass change rate of the coated specimen is −0.26%. Its good oxidation protection performance is mainly due to the generated Zr and Ta oxides on the coating surface, which increase the viscosity of the SiO2 layer and effectively block the diffusion channels of oxygen. After ablation at 2,300°C for 480 s, the mass ablation rate and linear ablation rate of the Z4T6 coating are 1.48 × 10−2 mg·s−1 and 0.94 μm·s−1, respectively. The Zr–Ta–Si–O composite glass layer composed of (Zr,Ta)O2 and SiO2 is relatively intact at the early stage of ablation, and it can effectively prevent plasma flame ablation. After four cycles of ablation (120 s × 4 cycles), the (Zr,Ta)O2 solid solution and SiO2 generated by the ablation reaction are insufficient to resist the invasion of high-temperature oxygen and flame erosion, ultimately leading to the failure of coating protection.

Keywords: oxidation resistance; ultra high temperature ceramic; coating; solid solution; ablation resistance

1 Introduction

Carbon materials possess high strength, good thermal conductivity, and excellent high-temperature stability, making them highly potential thermal structure materials in the field of aerospace [1,2,3,4,5]. However, carbon materials are prone to react with oxygen at temperatures above 400°C and also have poor resistance to ablation in high-speed-airflow scouring environment, limiting their widespread application [6,7,8,9,10]. Although matrix modification can only provide a certain protective effect, it cannot completely isolate oxygen, corresponding to a limited protective capability. Coating technology can flexibly select coating components based on the service environments, which are therefore considered more promising protective technology [7,11–16].

Among the numerous coating materials, ultra-high-temperature ceramic borides (ZrB2, HfB2, TaB2) [17–22] have become a research focus due to their inherent advantages. For instance, Ren et al. [23] prepared ZrB2–SiC coatings on graphite surfaces via spark plasma sintering technology. During oxidation, the Zr–Si–O vitreous oxide film formed on the surface effectively blocked oxygen channels and provided good protection for the graphite substrate. Aliasgarian et al. [24] and Hao et al. [25] developed ZrB2–SiC coatings to prevent high-temperature oxygen erosion by forming Zr–Si–O glassy layers. Qu et al. [26] fabricated TaB2–SiC coatings on C/C composite surfaces, and during ablation, the formed Ta–Si–O composite oxide layer significantly reduced the linear ablation rate (LAR) of C/C composites. Additionally, Chen et al. [27] and Ren et al. [28] also confirmed that the Ta–Si–O composite oxide layers produced by the oxidation of TaB2–SiC coatings possess a good protective effect. In view of this, if Zr–Ta oxides have a combined action, high-temperature protection performance of the coatings may be further enhanced. Tong et al. [29] combined the pack cementation method and slurry method to prepare (ZrTa)B2–SiC coatings on C/C composites, after ablation, Zr–Ta–O composite oxide phases were formed on the surfaces; according to the research of Ren et al. [30] about Zr x Ta1−x B2–SiC/SiC coatings, the Zr–Ta–Si–O compound glass layer was formed on the surface of the coating after oxidation, the combined effect of Zr–Ta oxide improves the high-temperature stability of the glass phase [31]. Based on the above reports, (ZrTa)B2 solid solution combined with SiC coatings can be oxidized or ablated to Zr–Ta–Si–O composite glass phases in high-temperature oxygen-containing environments, which are capable of constructing more reliable protective systems. In other words, (ZrTa)B2 composite SiC coatings are expected to provide broad temperature range oxidation and ablation protection for carbon-based materials.

Although some studies have already conducted certain research on Zr/Ta solid solution coatings, these works are limited to short-time evaluation or single solid solution component, research on their oxidation behavior over a wide temperature range, or the ablation resistance performance for extended durations (>400 s) above 2,000°C remains limitation. Therefore, it is crucial to develop protective coatings that can offer a long service life, excellent oxidation, and ablation resistance across a wide temperature range. Currently, the preparation method and technology of coatings with good protective performance have developed rapidly, but their limitations still exist. Chemical vapor deposition [32] and plasma spraying [33] involve specific processes and equipment, which are usually expensive. Sol–gel [34], slurry [35], and pack cementation [36] face challenges like difficulty in controlling coating thickness, low bonding strength, and insufficient coating compactness. In response to the aforementioned issues, in our previous work, we employed a combination of the slurry method and reactive melt infiltration (RMI) to prepare a dense TaB2–SiC–Si coating on the surface of graphite; this coating has a interfacial bonding strength above 20 MPa, which can provide 321 and 168 h oxidation protection at 1,050 and 1,550°C, respectively, as well as a ablation protection of 120 s under a heat flux of 2.38 MW·m−² [37]. Therefore, based on previous research, we propose the use of the slurry-RMI method to fabricate dense Si-based ceramic coatings containing (ZrTa)B2, aiming to enhance the service life of the coatings under a wide temperature range.

In this study, a combination of the slurry method and RMI was employed to fabricate Zr–Ta–B–Si–C composite coatings with varying Zr/Ta molar ratios on the surfaces of graphite. The impact of different Zr/Ta ratios on the coating’s performance during cyclic oxidation resistance at 1,600°C was examined. By optimizing the Zr/Ta ratio, the most effective coating was selected for the ablation resistance test at 2,300°C. Additionally, the oxidation resistance, ablation resistance, and the failure mechanisms related to ablation protection of the coating were thoroughly analyzed.

2 Experimental procedure

2.1 Preparation of the Zr–Ta–B–Si–C coating

Taking graphite with a density of 1.80 g·cm−³ as the matrix, it was cut into cubes with dimensions of 10 mm × 10 mm × 5 mm (for antioxidant performance testing) and cylinders with dimensions of Ф18 mm × 10 mm (for ablation resistance performance testing). After that, the graphite was polished and chamfered with 400# sandpaper and then placed into a beaker filled with absolute ethanol for ultrasonic cleaning and drying. Using 6560# phenolic resin as the binder and carbon source and absolute ethanol as the solvent, a resin-absolute ethanol solution was prepared according to a mass ratio of 3:10. SiC powder (10 μm) was slowly added into the above solution, and under the action of magnetic stirring, a uniform SiC slurry was obtained. The graphite samples were immersed in the SiC slurry; after taking out, they were dried at room temperature for 1 h and cured at 150°C for 3–5 h. Afterwards, the samples were heated in a vacuum tubular furnace at 800°C for 1 h. After cooling, SiC transition coating specimens were obtained. Next, according to the mass ratio of m(SiC):m(ZrB2/TaB2) = 1:1, SiC, ZrB2 (10 μm), and TaB2 (10 μm) powders (where the molar ratio of ZrB2/TaB2 was 2:8, 4:6, and 6:4) were added into the resin–ethanol solution and mixed evenly to obtain the ZrB2–TaB2–SiC slurry. The SiC transition coating specimens were placed into the ZrB2–TaB2–SiC slurry and then taken out; after curing, these samples were heated at 800°C to obtain the pre-coated specimens. Finally, the pre-coated specimens were placed into a graphite crucible with Si blocks at the bottom and then heated in a vacuum environment at 1,700°C for 20–30 min to obtain the Zr–Ta–B–Si–C coating specimens. For the convenience of description, the specimens were named as Z2T8, Z4T6, and Z6T4 according to the Zr/Ta molar ratio in the prepared slurry, and the preparation flow chart is shown in Figure 1.

Figure 1 Preparation process of Zr–Ta–B–Si–C coatings.
Figure 1

Preparation process of Zr–Ta–B–Si–C coatings.

2.2 Anti-oxidation tests of the Zr–Ta–B–Si–C coated sample

The specimen was placed in an alumina crucible and then loaded into a high-temperature resistance furnace (static oxidation, no air flow). The furnace temperature was increased to 1,600°C at a heating rate of 8°C·min−1 and held at this temperature. After the holding period, the specimen was allowed to cool to room temperature (each test involving a holding time of 5 h and a cumulative duration of 100 h). The mass change rate of the specimen was calculated by weighing the specimen before and after oxidation using an analytical balance; the oxidation data were the average of three samples.

2.3 Ablation tests of the Zr–Ta–B–Si–C coated sample

The ablation resistance performance of the coating was evaluated using a plasma welding and cutting machine. The instrument voltage was set to 160 V, and the current was adjusted to 9.5 A. The diameter of the ablation gun nozzle was 2 mm. The sample surface was positioned perpendicular to the flame nozzle, with a 10 mm distance between them. The ablation temperature of the coating surface was maintained at 2,300 ± 20°C (measured by an infrared thermometer). The mass and thickness of the sample before and after ablation were measured, and the mass ablation rate (MAR) and LAR were calculated using the following formulas [38]:

(1) MAR = Δ M / t ,

(2) LAR = Δ L / t ,

where ΔM and ΔL are the mass change and thickness change of the coated sample, respectively; and t is the ablation time.

2.4 Characterization

Scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS), and X-ray diffraction (XRD) were used to analyze the microscopic morphology, elemental distribution, and phase composition before and after oxidation and ablation. SEM images were taken using backscattering mode (BSE) and secondary electronic mode (SE).

3 Results and discussion

3.1 The phase composition and microstructure of the Zr–Ta–B–Si–C coating

XRD patterns of the Zr–Ta–B–Si–C coatings with three distinct compositions (as depicted in Figure 2) all display characteristic peaks that correspond to (ZrTa)B2(PDF#96-151-0838), SiC(PDF#00-029-1127), and Si(PDF#01-078-2500), respectively. Notably, both ZrB2 and TaB2 have a hexagonal crystal structure, with the ionic radii of Zr2+ and Ta2+ being 84 and 79 pm, respectively. By applying the solid solution calculation formula (3), the value of ∆r < 6% [39]; this value satisfies the prerequisites for the formation of a continuous solid solution. Consequently, ZrB2 and TaB2 undergo in situ reaction to give rise to the (ZrTa)B2 solid solution at 1,700°C (formula (4))

(3) ∆ r = | r 1 − r 2 | | r 1 | < 15 % ,

(4) ZrB 2 + TaB 2 = ( ZrTa ) B 2 ,

where r 1 represents the ionic radius of Zr, and r 2 represents the ionic radius of Ta.

Figure 2 XRD spectrums of the Zr–Ta–B–Si–C coatings.
Figure 2

XRD spectrums of the Zr–Ta–B–Si–C coatings.

The pyrolytic carbon presented in the precoating is converted into SiC during the RMI process, and some silicon remains on the coating surface, corresponding to the diffraction peaks of SiC and Si in Figure 2, respectively.

Figure 3 shows the surface microstructures and EDS element analysis of the Zr–Ta–B–Si–C coatings with three different compositions. Figure 3(a1)–(c1) demonstrate that the surface of the coatings is smooth and dense, with no noticeable cracks or pores. It can be clearly observed that white particles and dark gray particles are tightly packed together, embedded in the surface of the coating. From Figure 3(a2)–(c2), the coatings with different components have similar surface structure, consisting of white particles, gray particles, and gray continuous phase. Combined with the XRD diffraction patterns in Figure 2 and the EDS element analysis in Figure 3(a3)–(c3), (a4)–(c4), the white particles are identified as (ZrTa)B2 solid solution, while the dark gray particles are SiC, and the light gray phase is Si. The Si phase has an extremely fine grain size (strong Si diffraction peaks) filling the depressions of surface, thus making the coating more uniform at a macroscopic level. (ZrTa)B2, SiC, and Si are tightly bonded, forming a dense coating structure.

Figure 3 Microstructures (BSE) and EDS elemental analysis of Zr–Ta–B–Si–C coatings surface: (a1) surface image of Z2T8 coating; (a2) enlarge image of (a1); (a3) mapping element analysis of (a2); (a4) spot element analysis of (a2); (b1) surface image of Z4T6 coating; (b2) enlarge image of (b1); (b3) mapping element analysis of (b2); (b4) spot element analysis of (b2); (c1) surface image of Z6T4 coating; (c2) enlarge image of (c1); (c3) mapping element analysis of (c2); and (c4) spot element analysis of (c2).
Figure 3

Microstructures (BSE) and EDS elemental analysis of Zr–Ta–B–Si–C coatings surface: (a1) surface image of Z2T8 coating; (a2) enlarge image of (a1); (a3) mapping element analysis of (a2); (a4) spot element analysis of (a2); (b1) surface image of Z4T6 coating; (b2) enlarge image of (b1); (b3) mapping element analysis of (b2); (b4) spot element analysis of (b2); (c1) surface image of Z6T4 coating; (c2) enlarge image of (c1); (c3) mapping element analysis of (c2); and (c4) spot element analysis of (c2).

Figure 4 clearly presents the cross-sectional microstructure and EDS element analysis of the Zr–Ta–B–Si–C coatings with three different compositions. As can be seen from Figure 4, the internal structure of the coatings is dense, with no penetrating cracks. In Figure 4(a1)–(c1), it can be seen that the cross-sections are divided into three parts, namely, graphite matrix, transition layer, and outer layer containing ultra-high-temperature ceramic particles. As shown in Figure 4(a2)–(c2), white ceramic particles are embedded in the cross-sections, and they can be identified as (ZrTa)B2 solid solution based on Figure 4(a3)–(c3), (a4)–(c4). In addition, it can be found that some Si elements exist in the graphite matrix in Figure 4(a3)–(c3), this is because that during the RMI process, Si penetrates into the graphite substrates through the pores, existing in the form of SiC or Si. This interlocking structure contributes to enhancing the bonding strength between the coating and the substrate, as well as the thermal shock resistance of coating.

Figure 4 Microscopic morphology (BSE) and EDS elemental analysis of cross-sections of the Zr–Ta–B–Si–C coatings: (a1) cross-section image of Z2T8 coating; (a2) enlarge image of (a1); (a3) mapping element analysis of (a1); (a4) spot element analysis of (a2); (b1) cross-section image of Z4T6 coating; (b2) enlarge image of (b1); (b3) mapping element analysis of (b1); (b4) spot element analysis of (b2); (c1) cross-section image of Z6T4 coating; (c2) enlarge image of (c1); (c3) mapping element analysis of (c1); (c4) spot element analysis of (c2).
Figure 4

Microscopic morphology (BSE) and EDS elemental analysis of cross-sections of the Zr–Ta–B–Si–C coatings: (a1) cross-section image of Z2T8 coating; (a2) enlarge image of (a1); (a3) mapping element analysis of (a1); (a4) spot element analysis of (a2); (b1) cross-section image of Z4T6 coating; (b2) enlarge image of (b1); (b3) mapping element analysis of (b1); (b4) spot element analysis of (b2); (c1) cross-section image of Z6T4 coating; (c2) enlarge image of (c1); (c3) mapping element analysis of (c1); (c4) spot element analysis of (c2).

3.2 Anti-oxidation performance analysis of the Zr–Ta–B–Si–C coatings

Figure 5(a) shows the mass change curves of the Zr–Ta–B–Si–C coated samples, and it can be observed that all three types of coatings experience varying degrees of mass loss after oxidation for 100 h (20 cycles) at 1,600°C. The Z2T8-coated sample exhibits a relatively stable mass change before reaching 50 h of oxidation, but after the oxidation time exceeds 50 h, it begins to experience significant mass loss. After 100 h of oxidation, the mass change reaches −6.01%. The mass of Z4T6 and Z6T4 coatings increases initially and then decreases with the increase in oxidation time. Among them, the mass loss trend of the Z4T6 coating after 50 h of oxidation is the most gradual, with a mass change rate of −0.26% after 100 h of oxidation, while the Z6T4 coating shows a mass change rate of −1.33%. Obviously, the Z4T6 coating demonstrates better oxidation resistance.

Figure 5 (a) The curve of mass change with oxidation time of Zr–Ta–B–Si–C coatings during the oxidation process at 1,600°C; (b) XRD pattern of the surface of the Z4T6 coating after 100 h of oxidation.
Figure 5

(a) The curve of mass change with oxidation time of Zr–Ta–B–Si–C coatings during the oxidation process at 1,600°C; (b) XRD pattern of the surface of the Z4T6 coating after 100 h of oxidation.

In the XRD pattern of Z4T6 coating after being oxidized at 1,600°C for 100 h (Figure 5(b)), diffraction peaks of SiO2(PDF#96-900-8228), (Zr,Ta)O2, and ZrSiO4(PDF#01-083-1377) were observed. In contrast to the XRD pattern of the coating prior to oxidation, the diffraction peaks of (ZrTa)B2, SiC, and Si completely disappear, which indicates that the surface of the coating has been completely oxidized and the generated multiphase oxides are adhered to the coating surface. The diffraction peaks of B2O3 are not detected; this is due to the relatively low melting point of B2O3 and its high vapor pressure of 724.4 Pa at 1,600°C, leading to its rapid evaporation. The appearance of SiO2 is attributed to the reaction between SiC, Si, and oxygen. The diffraction peaks of (Zr,Ta)O2 are present because of the oxidation of (ZrTa)B2 solid solution and reaction of Zr–Ta oxides. During the oxidation process, a portion of ZrO2 and Ta2O5 undergo a solid solution reaction to form the (Zr,Ta)O2 solid solution, while another part of ZrO2 reacts in situ with SiO2 to produce ZrSiO4. Both (Zr,Ta)O2 and ZrSiO4 have high melting points, which allows them to create a stable skeletal structure. This structure enhances the viscosity of the SiO2 glassy phase, thereby improving the protective performance of the coating.

Figure 6 shows the microscopic morphology and EDS analysis of the surface and cross-section of the Z4T6 coating after 100 h of oxidation at 1,600°C. From Figure 6(a1), it can be observed that the surface of the coating is dense without obvious cracks, but several “needle-like” pores are present. These pores are mainly due to the escaping of gaseous products produced during oxidation, such as CO, CO2, SiO, and B2O3. Furthermore, droplet-like particles are observed on the surface of the coating (Figure 6(a1)), which are the result of Si and SiC being gradually oxidized during extended oxidation, forming small SiO2 particles that eventually gather and coalesce into larger droplet-like particles. From Figure 6(a2), the coating surface is composed of a gray phase surrounding a white phase. EDS elemental analysis in Figure 6(a3, a4) combined with the XRD pattern result (Figure 5(b)) reveals that the white phase is Zr–Ta oxide solid solution comprising Zr, Ta, Si, and O elements that are coated with SiO2, while the gray phase is SiO2. A small number of microcracks on the surface of coating can be observed; these microcracks are mainly caused by thermal stress generated inside the material during thermal cycling, resulting in the cracking of the SiO2 layer. Upon closer inspection, it can be seen that the flowability of SiO2 at high temperatures gives these microcracks a self-healing tendency.

Figure 6 Microscopic morphology (BSE) and EDS elemental analysis of the surface and cross-section of the Z4T6 coating after 100 h of oxidation: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) mapping element analysis of (a2); (a4) spot element analysis of (a2); (b1) cross-section microscopic morphology; (b2) enlarge image of (b1); (b3) mapping element analysis of (b2); (b4) spot element analysis of (b2).
Figure 6

Microscopic morphology (BSE) and EDS elemental analysis of the surface and cross-section of the Z4T6 coating after 100 h of oxidation: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) mapping element analysis of (a2); (a4) spot element analysis of (a2); (b1) cross-section microscopic morphology; (b2) enlarge image of (b1); (b3) mapping element analysis of (b2); (b4) spot element analysis of (b2).

Figure 6(b1) exhibits the cross-sectional morphology of Z4T6 coating after oxidation. It is evident that the bond between the Z4T6 outer coating, the SiC transition layer, and the graphite substrate remains intact. There are no significant cracks or pores inside the coating. Figure 6(b2) shows an enlarged image of Figure 6(b1), and based on Figure 6(b3, b4), it can be observed that the oxygen element only distributes on the surface, and unoxidized ceramic particles still exist in the cross-section of coating. In addition, (ZrTa)B2 on the surface of Z4T6 coating undergoes oxidation to form (Zr,Ta)O2 and ZrSiO4, both of which are high-temperature phases with melting points. These phases exist within the SiO2 oxide layer and can increase its viscosity; they work together with SiO2 to form a Zr–Ta–Si–O oxide layer that has a relatively low oxygen permeability, effectively preventing oxygen from penetrating into the coating.

3.3 Anti-ablation performance analysis of the Z4T6 coating

According to the oxidation resistance results of the composite coatings, the Z4T6 coating presents better protection performance. To evaluate its ablation resistance, an ablation test was conducted using plasma flame. After 120 s of ablation, the MAR and LAR of the Z4T6 coating were −1.67 × 10−3 mg·s−1 and 0.3 × 10⁻³ μm·s−1, respectively. The coating showed a slight increase in weight, indicating good ablation resistance. Figure 7 shows the XRD spectrum of the coating surface after 120 s of ablation. Similar to the oxidized coating, the (ZrTa)B2, SiC, and Si on the surface are completely oxidized during the ablation process, forming a composite oxide layer composed of (Zr,Ta)O2, ZrSiO4(PDF#01-089-2655), and SiO2(PDF#96-900-1580). This Zr–Ta–Si–O layer adheres to the coating surface and can enhance the coating’s ablation resistance.

Figure 7 XRD pattern of the surface of the Z4T6 coating after 120 s of ablation.
Figure 7

XRD pattern of the surface of the Z4T6 coating after 120 s of ablation.

Figure 8 shows the surface and cross-sectional morphology of the Z4T6 coating after 120 s of ablation, along with EDS elemental analysis. Upon observation, it can be seen that the central ablation region of the coating surface (Figure 8(a1)) is covered with a large amount of glassy oxide composed of gray and white phases, where the gray phase tightly envelops the white phase (Figure 8(a2)). Combined with the EDS elemental analysis (Figure 8(c1, c2)) and surface XRD pattern (Figure 7), it can be confirmed that, similar to the oxidation process, the white phase is formed by the oxidation of (ZrTa)B2 during ablation, which leads to the formation of a Zr–Ta–O solid solution that gradually precipitates and eventually sinters together. This solid solution has good high-temperature stability and can effectively resist the mechanical erosion force of the flame during ablation. However, it is prone to the formation of cracks and voids during sintering. Meanwhile, SiC and Si are oxidized to form SiO2, which exhibits a certain fluidity at high temperatures, quickly filling some defects and blocking the oxygen channels. The Zr–Ta–O solid solution embedded in SiO2 further increases the viscosity of the oxide layer, ultimately forming a Zr–Ta–Si–O composite oxide layer that enhances the ablation resistance of the coating. In the Zr–Ta–O oxide region, a contrast difference (light and dark) can be observed (Figure 8(a1)), which is due to the higher atomic number of Ta compared to Zr. As Ta gradually diffuses, the contrast of the oxide film decreases under the secondary electron imaging mode. Figure 8(a3) shows the microstructure of the ablation transition zone on the surface after ablation for 120 s. It can be observed that many needle-like pores exist, which are caused by the oxidation reactions occurring inside the coating as oxygen penetrates. The gas byproducts (such as SiO, CO, and CO2 [40]) generated during ablation accumulate under the oxide layer, and due to thermal convection with the external flame, they eventually lead to the rupture of the oxide film and the extrusion of these products to the coating surface.

Figure 8 Microscopic morphology (BSE) and EDS element analysis of the surface and cross-section at the Ablation Center of the Z4T6 Coating after 120 s of ablation: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) microscopic morphology of the surface transition zone; (b1) cross-section microscopic morphology; (b2) enlarge image of (b1); (b3) enlarge image of (b2); (c1) spot element analysis of (a2, b3); (c2) mapping element analysis of (a2); (c3) mapping element analysis of (b3).
Figure 8

Microscopic morphology (BSE) and EDS element analysis of the surface and cross-section at the Ablation Center of the Z4T6 Coating after 120 s of ablation: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) microscopic morphology of the surface transition zone; (b1) cross-section microscopic morphology; (b2) enlarge image of (b1); (b3) enlarge image of (b2); (c1) spot element analysis of (a2, b3); (c2) mapping element analysis of (a2); (c3) mapping element analysis of (b3).

In Figure 8(b1), the microstructure of the coating’s cross-section after ablation clearly shows that the coating is firmly bonded to the graphite substrate, with no oxidation defects in the interior. After ablation, there is a relatively hard oxide layer at the center of the ablation. However, the oxide layer is scratched out by the diamond grinding disc during the polishing process of the sample cross-section. Therefore, in the central ablation region, an ablation pit is present, and the overall thickness of the coating remains basically unchanged. Figure 8(b2, b3) show the magnified view of the coating cross-sections, combined with the EDS elemental analysis (Figure 8(c1, c3)), it is evident that oxygen accumulates extensively on the coating surface, but no such accumulation is observed in the interior of the coating. This indicates that the ablation reaction occurs only on the surface, while the interior of the coating remains intact and unoxidized. This demonstrates that the Z4T6 coating exhibits considerable ablation resistance, providing effective protection for the carbon substrate.

Carbon-based materials are often used in high-temperature environments for long durations, and the coatings are not able to provide permanent protection. Therefore, studying the failure mechanisms of coatings is particularly important. In this study, the Z4T6 coating was subjected to a 480 s (120 s × 4 cycles) ablation test using a plasma flame to investigate the coating’s failure mechanisms. After 480 s of ablation (4 cycles), the MAR and LAR of the coating are 1.48 × 10−2 mg·s−1 and 0.94 μm·s−1, respectively. From the XRD spectrum of the coating surface after ablation (Figure 9), it can be seen that a Zr–Ta–Si–O composite oxide still exists on the coating surface. The microstructure of the surface (Figure 10(a1, a2)) shows a large amount of “scaly” and continuous gray oxide in the center of the ablation zone, which adheres firmly to the ablated surface (Figure 10(a3)). XRD analysis and surface EDS elements (Figure 10(b2, b3)) indicate that the “scaly” oxide is a Zr–Ta–O solid solution, while the gray continuous oxide is a Zr–Si–O composite oxide layer formed by the partial dissolution of Zr into the SiO2 layer. Additionally, numerous pores have appeared on the coating surface. Combining the cross-sectional microstructure (Figure 10(b1)), it can be concluded that the protective effect of the coating has failed. This is because that, during the prolonged ablation process, the oxide products in the ablation center continuously precipitate and are blown away by the mechanical erosion of flame, which are gradually consumed. After 480 s of ablation, the coating has been penetrated by the flame and is no longer able to provide new oxides to resist the erosive effects of the ablation flame or fill the defects caused by the volatilization of gaseous products, leading to the protection failure of the Z4T6 coating.

Figure 9 XRD pattern of the surface of the Z4T6 coating after 480 s of ablation.
Figure 9

XRD pattern of the surface of the Z4T6 coating after 480 s of ablation.

Figure 10 Microscopic morphology (SE) of the surface and cross-section at the ablation center as well as EDS elemental analysis of the surface at the ablation center of the Z4T6 coating after ablation for 480 s: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) enlarge image of (a2); (b1) cross-section microscopic morphology; (b2) mapping element analysis of (a3); (b3) spot element analysis of (a3).
Figure 10

Microscopic morphology (SE) of the surface and cross-section at the ablation center as well as EDS elemental analysis of the surface at the ablation center of the Z4T6 coating after ablation for 480 s: (a1) surface microscopic morphology; (a2) enlarge image of (a1); (a3) enlarge image of (a2); (b1) cross-section microscopic morphology; (b2) mapping element analysis of (a3); (b3) spot element analysis of (a3).

3.4 Anti-oxidantion and anti-ablation mechanisms of the Zr–Ta–B–Si–C coating

In order to study the oxidation mechanism of the Zr–Ta–B–Si–C coating, the Gibbs free energy of the possible reactions during the oxidation process is calculated by using HSC 6.0 software. The calculation results are shown in Figure 11(a). The main occurring reactions during the oxidation process of the coating are as follows [14,32,36,41,42]:

(5) 4 ( ZrTa ) B 2 ( s ) + 15 O 2 ( g ) = 4 ZrO 2 ( s ) + 2 Ta 2 O 5 ( s ) + 4 B 2 O 3 ( l ) ,

(6) ZrB 2 ( s ) + O 2 ( g ) = B 2 O 3 ( g ) + ZrO 2 ( s ) ,

(7) TaB 2 ( s ) + O 2 ( g ) = Ta 2 O 5 ( s ) + B 2 O 3 ( g ) ,

(8) B 2 O 3 ( l ) → B 2 O 3 ( g ) ,

(9) ZrO 2 ( s ) + Ta 2 O 5 ( s ) = ( Zr , Ta ) O 2 ( s ) ,

(10) ZO 2 ( s ) + SiO 2 ( l ) = ZrSiO 4 ( s ) ,

(11) Si ( s ) + O 2 ( g ) = SiO 2 ( s ) ,

(12) 2 SiC ( s ) + 3 O 2 ( g ) = SiO 2 ( s ) + 2 CO ( g ) ,

(13) SiC ( s ) + 2 O 2 ( g ) = SiO 2 ( s ) + CO 2 ( g ) ,

(14) SiC ( s ) + O 2 ( g ) = SiO ( g ) + CO ( g ) ,

(15) SiC ( s ) + 2 SiO 2 ( s ) = CO ( g ) + 3 SiO ( g ) ,

(16) 2 SiC ( s ) + SiO 2 ( s ) = 2 CO ( g ) + 3 Si ( s ) ,

(17) SiC ( s ) + SiO 2 ( s ) = C ( s ) + 2 SiO ( g ) .

Figure 11 (a) The curve of Gibbs free energy varying with temperature during the oxidation process of the Z4T6 coating. (b) The vapor pressure versus temperature curve of the oxide products of Z4T6 coating.
Figure 11

(a) The curve of Gibbs free energy varying with temperature during the oxidation process of the Z4T6 coating. (b) The vapor pressure versus temperature curve of the oxide products of Z4T6 coating.

The change in Gibbs free energy (∆G) is an important indicator for evaluating whether a chemical reaction can occur thermodynamically. As can be seen from Figure 11(a), during the oxidation process, the Gibbs free energies of the reactions of Si, SiC, TaB2, and ZrB2 with oxygen at 1,600°C are all negative, indicating that these components can spontaneously undergo oxidation reactions at this temperature. The light green area in Figure 11(a) represents the change in Gibbs free energy of formula (5). From a thermodynamic perspective, SiO2 can be continuously and stably generated at 1,600°C, demonstrating that the coating has the ability to maintain its performance over time. As shown in Figure 12, during the oxidation process, SiC and Si on the coating surface are oxidized to form a layer of SiO2 adhering to the coating surface (formulas (11–13)). After the (ZrTa)B2 solid solution is oxidized, oxidation products such as ZrO2, Ta2O5, and B2O3 are generated (formula (5)). Among them, B2O3 rapidly evaporates due to its high vapor pressure at 1,600°C (formula (8), Figure 11(b)). At high temperatures, ZrO2 will react with Ta2O5 and SiO2, respectively, to form a (Zr,Ta)O2 solid solution (formula (9)) and ZrSiO4 (formula (10)) silicate with good high-temperature stability. These products are embedded in the SiO2 layer, increasing the viscosity of the oxide layer and forming a Zr–Ta–Si–O composite glass phase. This composite glass phase has an extremely low oxygen permeability, effectively delaying the oxidation rate of the coating and providing good protection for the substrate. Therefore, the coating experiences a weight gain phenomenon in the early stage of oxidation (Figure 5(a)). With the increase in oxidation time, oxygen gradually penetrates into the interior of coating to consume it, which is accompanied by the generation of gas byproducts (CO, CO2, SiO, and B2O3). They accumulate under the SiO2 film to form bubbles, and once the pressure exceeds the critical value, the bubbles will burst. Whereupon, the gaseous products escape from the coating surface, resulting in the formation of holes. As the gaseous products continue to evaporate, along with the peeling of the oxide film caused by multiple cycle oxidation, the coating gradually experiences damage, causing a decrease in protective performance.

Figure 12 Schematic of the oxidation process for the Z4T6 coating sample.
Figure 12

Schematic of the oxidation process for the Z4T6 coating sample.

Figure 13 is a schematic diagram of the ablation process of the Z4T6-coated sample. Coating components, such as Si, SiC, and (ZrTa)B2, are easy to react with O2 (Gibbs free energy of all reactions are negative). In the initial stage of ablation, the coating mainly undergoes endothermic oxidation (Figure 13(a)). After (ZrTa)B2, Si and SiC on the coating surface are oxidized, ZrO2, Ta2O5, SiO2, and some gaseous products (such as B2O3, CO, and CO2) are generated. At this ablation stage, the volatilization of the gaseous products can be neglected. Subsequently, ZrO2 and Ta2O5 react to form a (Zr,Ta)O2 solid solution, which are embedded in the SiO2 layer to form a comparatively stable Zr–Ta–Si–O composite glass phase, making the coating exhibit a relatively intact state.

Figure 13 Schematic diagram of the ablation process of Z4T6 coating: (a) ablation initial stage; (b) ablation middle stage (ablation for 120 s); (c) failure of coating protection (ablation for 480 s).
Figure 13

Schematic diagram of the ablation process of Z4T6 coating: (a) ablation initial stage; (b) ablation middle stage (ablation for 120 s); (c) failure of coating protection (ablation for 480 s).

As the ablation time increases, some of the oxides on the coating surface volatilize into the surrounding environment, such as B2O3 and SiO2. B2O3 has a vapor pressure as high as 4.21 × 10⁵ Pa at 2,300°C and thus evaporates vigorously. As the ablation proceeds, the temperature on the coating surface rises, and a part of SiO2 volatilizes. The Zr–Ta–O solid solution is gradually generated and sintered together under the action of the high temperature flame, forming a high-temperature-resistant Zr–Ta–Si–O component that can effectively resist the incipient mechanical erosion force of the flame. However, prolonged cyclic erosion is easy to cause pores and cracks in the multiphase oxide layer. Although SiO2 has fluidity to fill some defects, due to the high vapor pressure and mechanical erosion caused by the plasma flame, newly generated SiO2 cannot be well replenished into the oxide layer, leading to the continuous expansion of ablation defects (Figure 13(b)). Oxygen gradually penetrates into the interior of the coating to consume the coating; those gaseous products (SiO, CO, and CO2) still keep volatilizing, causing the number of defects in the oxide layer to gradually increase. When the ablation time further increases, the oxide film continuously undergoes the “formation-consumption” process, as the final Zr–Ta–Si–O composite oxide layer at the ablation center is consumed completely, the ablation flame penetrates through the coating to graphite, and the protective effect of the coating disappears (Figure 13(c)).

4 Conclusions

This work combines the slurry method and reactive infiltration to prepare Zr–Ta–Si–B–C composite coatings with different Zr/Ta molar ratios on the surface of graphite. The prepared coatings are dense and bonded tightly to the substrates, with (Zr,Ta)B2, SiC, and Si uniformly distributed within the coatings. After oxidation at 1,600°C for 100 h, the Z4T6 coating sample exhibits better protective performance, with a mass change rate of −0.26%, which is primarily attributed to the formation of (Zr,Ta)O2 and ZrSiO4 that have strong high-temperature stability on the coating surface. (Zr,Ta)O2 and ZrSiO4 are embedded in SiO2, forming a Zr–Ta–Si–O composite glass layer, which increases the viscosity of the oxide layer and reduces the oxygen diffusion rate, thereby enhancing the coating’s protective performance. The Z4T6 coating was subjected to a 480 s ablation test at 2,300°C, yielding a MAR of 1.48 × 10−2 mg·s−1 and a LAR of 0.94 μm·s−1. During the ablation process, (Zr,Ta)O2 solid solution gradually precipitate and sinter together to resist the mechanical erosion force from the ablation flame. The SiO2, which has a certain flowability at the early stage of ablation, can fill the defects of the oxide layer, ultimately forming a Zr–Ta–Si–O composite oxides that prevent oxygen diffusion and effectively resist flame impingement. As the ablation time increases, gaseous products (CO, CO2, SiO, B2O3, SiO2, etc.) continuously volatilize, the Zr–Ta–Si–O layer gradually bursts, and high melting point (Zr,Ta)O2 are blown away. Thereafter, internal coating is constantly being eroded, and the Zr–Ta–Si–O composite phase undergoes a “formation-consumption” process, until the Z4T6 coating is consumed completely and loses its protective effect.

Acknowledgments

This project was supported by the Liaoning Province Science and Technology Plan Joint Program (Natural Science Foundation General Project, 2024-MSLH-381) and Youth Project of the Liaoning Provincial Department of Education (JYTQN2023371).

  1. Funding information: This work is funded by the Liaoning Province Science and Technology Plan Joint Program (Natural Science Foundation General Project, 2024-MSLH-381) and Youth Project of the Liaoning Provincial Department of Education (JYTQN2023371).

  2. Author contributions: Xiaoyang Guo: investigation, experiment, writing-original draft. Yan Jiang: investigation, editing and funding acquisition. Yuan Tian: investigation, experiment, data analysis. Na Wang: supervision and editing.

  3. Conflict of interest: The authors state no conflict of interest.

  4. Data availability statement: The data of the findings in this study can be obtained from the corresponding author upon reasonable request.

  5. Declaration of generative AI and AI-assisted technologies in the writing process: After the writing of this article was completed, it was polished by AI.

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Received: 2025-03-04
Revised: 2025-05-19
Accepted: 2025-06-02
Published Online: 2025-07-15

© 2025 the author(s), published by De Gruyter

This work is licensed under the Creative Commons Attribution 4.0 International License.

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https://doi.org/10.1515/htmp-2025-0086
Schlagwörter für diesen Artikel
oxidation resistance; ultra high temperature ceramic; coating; solid solution; ablation resistance
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Heruntergeladen am 26.9.2025 von https://www.degruyterbrill.com/document/doi/10.1515/htmp-2025-0086/html
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