Extreme Materials

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Advances in ultra-high-temperature ceramic coatings with enhanced oxidation resistance for carbon-based composites

Xuanru Ren, Peipei Wang, Yuexing Chen, Wei Xie, Xiang Ji, Zhichao Shang, Chengshan Ji, Jun Zhao, Huiqun Liu, Guozheng Lv, Peizhong Feng

Extreme Materials, 2025, 1(3): 9-43. DOI: 10.1016/j.exm.2025.07.003

Coating materials	Fabrication methods	Temperature ( ^∘C )	Time (h)	Mass loss (wt%)	Refs.
HfB₂-SiC/SiC	PCP	1700	0.8	0.51 g/cm²	[115]
HfB₂-SiC-MoSi₂	LPS	1500	200	0.08%	[121]
SiO₂-MexOy	CP+HT	1700	30	-	[122]
ZrB₂-SiC-ZrC-B₄C	IMP + PYR	1500	200	1.8%	[123]
ZrB₂-SiC-ZrC	-	1500	6	1.34 %	[124]
ZrB₂-SiC-TaSi₂	SCC	1700	0.5	3.81mg/cm²	[126]
ZrB₂-SiC-WB	LPPS	1500	753	0.487 %	[127]
HfB₂-SiC-MoSi₂	LFT	1700	-	0.56 %	[128]
SiC/SiC_-MoSi₂-ZrB₂		1500	30	0.3 %	[129]
ZrB₂-MoSi₂-SiC-Si	SI+ VSI	1600	150	0.21 %	[130]
ZrB₂-xMoSi₂-Y₂O₃-yAl	SCC	1400	6.5		[133]
CeO₂-HfB₂-MoSi₂-SiC	SPS	1700	1.5	0.14 g/cm²	[134]
ZrB₂-SiC-La₂O₃/SiC	SPS	1800	0.25	1.15mg/cm²	[135]
Lu₂O₃-SiC-HfB₂	SPS	1700	130	3.8mg/cm²	[136]
LaB₆-HfB₂-SiC	LFT	1700	1.5	0.85 g/cm²	[137]

Table 2 The self-generated glass film coating has high temperature oxidation resistance above 1500^∘C.

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Fig. 1. Gradient high oxygen barrier concept of UHTC coatings. Reproduced with permission from Ref. [13], © Elsevier 2024.
Fig. 2. SEM images of SiC coatings with a Si/C weight ratio of 6:0.5 after 100 h of oxidation in air at 1500^∘C : (a) surface; (b) cross-section. Reproduced with permission from Ref. [22], © Elsevier 2015.
Fig. 3. (a) Backscattering cross-section micrographs of coated C/C composites; High-magnification backscattered electron micrograph of the (b) coating and (c) interface between the C/C composite and the internal SiC layer; (d) Energy dispersive spectroscopy elemental line analysis of the coating in (a), with the yellow arrow representing the scanning direction. Reproduced with permission from Ref. [33], © Wiley-Blackwell 2014.
Fig. 4. (a) Schematic diagram of the sprayed gradient SZM coating on SiC-coated C/C composites, (b) cross-sectional morphology, and (c) elemental line scan. Reproduced with permission from Ref. [36], © Elsevier 2017.
Fig. 5. SEM images of the bamboo-like SiC nanowires with a porous network on the surface of C/C samples: (a) low magnification; (b) high magnification.Reproduced with permission from Ref. [41], © Elsevier 2013.
Fig. 6. (a) TEM image of a single SiC nanowire; (b) HRTEM image of the core-shell interface; (c) Elemental mapping of the nanowire; HADDF image of (d) nanowires surrounding ZrB₂ and (e) the interface between ZrB₂ and SiC. Reproduced with permission from Ref. [42], © Tsinghua University Press 2024.
Fig. 7. SEM microstructure of SiC_w-HfB₂-SiC-Si/SiC coating: (a) cross-section; (b-c) cross-sectional SiC_w bridging; (d) cross-sectional SiC_w pull-out and debonding.Reproduced with permission from Ref. [46], © Elsevier 2018.
Fig. 8. Fracture surface SEM images of the SiCnws-LMS/SiC coating: (a-c) the representative nanowire pull-out feature; (d, e) the representative nanowire bridging feature. Reproduced with permission from Ref. [48], © Elsevier 2018.
Fig. 9. Vertical crack development behavior under different conditions calculated by the smart crack growth modules of ANSYS: (a) the vertical crack development model; (b) the vertical development behavior in MoSi₂ under the action of thermal stress; (c) the crack deflection behavior with weak interface; (d) the crack steering induced by micropore distribution. Reproduced with permission from Ref. [49], © Elsevier 2021. [49], © Elsevier 2021.
Table 1 High temperature oxidation resistance of single layer coating, double layer coating, gradient coating and nanomaterial coating.
Fig. 11. Schematic diagram of the slurry brushing method for preparing ZrB₂-SiC coatings. Reproduced with permission from Ref. [63], © Wiley-VCH Verlag 2023.
Fig. 12. Schematic diagram of the atmospheric plasma spraying system. Reproduced with permission from Ref. [71], © Elsevier 2021.
Fig. 13. Schematic diagram of the in-situ reaction sintering process for preparing HfB₂-MoSi₂/SiC-Si coatings on the surface of C/C composites. Reproduced with permission from Ref. [73], © Elsevier 2020.
Fig. 14. Schematic diagram of the SPS coating preparation method. Reproduced with permission from Ref. [82], © Elsevier 2019.
Fig. 16. Microstructure SEM images of HfB₂-SiC coatings with different HfB₂ contents: (a) and (b) Surface and cross-section of the 30wt_\%HfB₂-SiC coating; (c) and (d) Surface and cross-section of the 40wt\%HfB₂-SiC coating; (e) and (f) Surface and cross-section of the 50wt\%HfB₂-SiC coating; (g) and (h) Surface and crosssection of the 60wt\%HfB₂-SiC coating. Reproduced with permission from Ref. [93], © Elsevier 2022.
Fig. 17. w(a) Backscattered electron image of the cross-section of the double-layer coating on C/C composites; (b) Schematic of the preparation of the Zr_xTa_1-xB₂-SiC outer coating. Reproduced with permission from Ref. [97], © Elsevier 2015.
Fig. 18. (a)-(b) Surface EDS images of the 40HfB₂-40TaSi₂-20SiC coating samples before and after oxidation; (c)-(d) Schematic of Hf/Ta oxide peeling after oxidation. Reproduced with permission from Ref. [106], © Elsevier 2020.
Fig. 19. Surface, cross-sectional morphology, and corresponding EDS analysis of ZS and ZSL coating samples after 550 h of oxidation at 1500^∘C : (a) and (b) Secondary electron images of the surface of the ZS coating sample; (c) Backscattered electron image of the cross-section of the ZS coating sample; (d) and (e) Secondary electron images of the surface of the ZSL coating sample; (f) Backscattered electron image of the cross-section of the ZSL coating sample; (g) EDS area scan images of different elements corresponding to the cross-sectional morphology of the ZSL coating. Reproduced with permission from Ref. [110], © Elsevier 2018.
Fig. 20. Saturated vapor pressure and viscosity of SiO₂ as a function of temperature. Reproduced with permission from Ref. [112], © Elsevier 2025.
Fig. 22. Mass loss of SiO₂-Me_xO_y samples after 30 h of heat treatment at 1700^∘C. Reproduced with permission from Ref. [122], © Wiley-Blackwell 2021.
Fig. 23. TEM images of the composite glass layers: (a) Hf-B-Si-O and (d) Hf-Ta-B-Si-O; High-resolution TEM images of the composite glass layers: (b)-(c) Hf-B-Si-O and (e)-(f) Hf-Ta-B-Si-O. Reproduced with permission from Ref. [106], © Elsevier 2020.
Fig. 24. (a)-(d) High-magnification backscattered SEM morphologies of the surface of the HfB₂-SiC-LaB₆ coating after oxidation at 1700^∘C; (e) Evolution mechanism of the multiphase glass layer during the oxidation process. Reproduced with permission from Ref. [137], © Elsevier 2024.
Fig. 25. Oxidation resistance mechanism of the composite glass layer. Reproduced with permission from Ref. [25], © Elsevier 2020; Ref. [142], © Elsevier 2022; Ref. [143], © Elsevier 2021.
Fig. 26. Self-generated film formation process of the UHTC coating during service. Reproduced with permission from Ref. [13], © Elsevier 2024; Ref. [144], © Elsevier 2018; Ref. [145], © Elsevier 2019.
Fig. 27. Schematic diagram of the preparation process for the SiC/ZrB₂-CrSi₂-Si/SiC multi-layer coating. Reproduced with permission from Ref. [148], © Elsevier 2021.
Fig. 28. Schematic diagram of the combined slurry dipping (SD) and gaseous silicon infiltration (GSI) process for preparing a single-layer SiC-HfB ₂-Si coating on C/C composites. Reproduced with permission from Ref. [153], © Elsevier 2020.
Fig. 29. Weight change curve of the ZrB₂-SiC ceramic standard specimen during oxidation from room temperature to 1700^∘C. Reproduced with permission from Ref. [155], © Elsevier 2022.
Fig. 30. (a) Surface SEM image and (b) TEM image of the ZrB₂-SiC coating after 1200^∘C,120 min film formation treatment; (c) EDS surface scan map corresponding to (a); (d) high-resolution TEM image corresponding to (b). Reproduced with permission from Ref. [155], © Elsevier 2022.
Fig. 31. Schematic diagram of the coating repair process for C/C composites. Reproduced with permission from Ref. [162], © Elsevier 2022.
Fig. 32. In-situ micro-area self-healing during oxidation of HfB₂-HfSi₂-SiC coating prepared by SHS +SPS. Reproduced with permission from Ref. [165], © Elsevier 2023.
Fig. 33. Isothermal oxidation curve of the coated C/C composite in air at 1773 K. Reproduced with permission from Ref. [167], © Elsevier 2014.
Fig. 34. Thickness measurements of thermally grown oxide (TGO) layers on three Si specimens after water vapor corrosion at 1300^∘C : (a) APS-deposited Si coating; (b) polycrystalline Si; (c) single-crystal Si; (d) thickness comparison between unoxidized and oxidized crystalline Si. Reproduced with permission from Ref. [175], © Elsevier 2025.
Fig. 35. Oxidation curves of coated samples at 1773 K under different OPP conditions. Reproduced with permission from Ref. [124], © Elsevier BV 2016.
Fig. 36. Oxidation curve of SiC/ glaze precursor-coated samples in air from room temperature to 1600^∘C. Reproduced with permission from Ref. [184], © Elsevier 2017.
Fig. 37. Experimental and simulation results under thermal shock environment: (a) mass change curves of the coated samples with monolayer MoSi ₂ coating and with laminated MoSi₂/Cr coating after 30 thermal cycles; (b) BSE image of monolayer MoSi₂ coating (inset of figure is the surface view of (b)) and (c) BSE image of laminated MoSi₂/Cr coating along the cross-section (inset of figure is the surface view of (c)) after thermal shock test; (d) and (e) stress distribution diagram along the cross-section of monolayer MoSi₂ coating and laminated MoSi₂/Cr coating during a thermal cycle; (f) stress distribution curves through the thickness of the coating and substrate under thermal shock environment. Reproduced with permission from Ref. [190], © Elsevier 2020.
Fig. 38. Temperature and thermal stress distribution in coated C/C composites. Reproduced with permission from Ref. [46], © Elsevier 2018.
Fig. 39. Macroscopic images and cantilever beam model of coated samples in wind tunnel. Reproduced with permission from Ref. [199], © Elsevier 2015.
Fig. 40. Data distortion in traditional evaluation methods. Reproduced with permission from Ref. [143], © Elsevier 2021.

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