管状C/SiC复合材料高温空气氧化行为与宏细观建模研究

doi:10.15541/jim20240002

无机材料学报 ›› 2024, Vol. 39 ›› Issue (8): 920-928.DOI: 10.15541/jim20240002

管状C/SiC复合材料高温空气氧化行为与宏细观建模研究

全文心(), 余艺平, 方冰, 李伟, 王松()

国防科技大学空天科学学院, 新型陶瓷纤维及其复合材料重点实验室, 长沙 410073

收稿日期:2024-01-02 修回日期:2024-03-13 出版日期:2024-08-20 网络出版日期:2024-03-30
通讯作者: 王松, 研究员. E-mail: wangs0731@163.com
作者简介:全文心(2000-), 男, 硕士研究生. E-mail: quanwenxin18@nudt.edu.cn
基金资助:
湖南省自然科学基金面上项目(2023JJ30634);国家重点实验室基金(6142907230202)

Oxidation Behavior and Meso-macro Model of Tubular C/SiC Composites in High-temperature Environment

QUAN Wenxin(), YU Yiping, FANG Bing, LI Wei, WANG Song()

Science and Technology on Advanced Ceramic Fibers and Composites Laboratory, College of Aerospace Science and Engineering, National University of Defense Technology, Changsha 410073, China

Received:2024-01-02 Revised:2024-03-13 Published:2024-08-20 Online:2024-03-30
Contact: WANG Song, professor. E-mail: wangs0731@163.com
About author:QUAN Wenxin (2000-), male, Master candidate. E-mail: quanwenxin18@nudt.edu.cn
Supported by:
Natural Science Foundation of Hunan Province(2023JJ30634);State Key Laboratory Program(6142907230202)

摘要/Abstract

摘要：

氧化损伤是影响火箭发动机用C/SiC复合材料喷管寿命的主要因素之一。为准确评估C/SiC复合材料喷管的氧化损伤, 本研究以近似喷管结构的管状C/SiC复合材料为实验对象, 研究了管状C/SiC复合材料在高温(900~1300 ℃)空气环境下的氧化行为, 包括其组成、结构及力学性能的演变规律, 发现管状C/SiC复合材料在该高温空气环境下表现出受扩散控制的氧化特征, 质量与剩余强度随时间呈幂函数下降趋势, 下降速率与温度正相关。在此基础上, 从氧化动力学与传质学理论角度出发, 建立了管状C/SiC复合材料细观/宏观尺度氧化模型, 模拟了管状C/SiC复合材料高温空气氧化过程, 并预测了材料的质量与剩余强度。模型预测结果与实验数据拟合程度较高, 可为C/SiC复合材料喷管的寿命评估提供参考。

关键词: C/SiC复合材料, 高温氧化, 氧化模型, 寿命预测

Abstract:

Oxidation damage is one of the main factors affecting the life of C/SiC composite nozzle used in rocket engines. To accurately predict the oxidation damage of C/SiC composite nozzle, we explored the oxidation behavior of the tubular C/SiC composites which had a similar shape to nozzle. Evolution of their composition, structure, and mechanical properties was investigated at different temperatures ranging from 900 to 1300 ℃. The results showed that the tubular C/SiC composites exhibited diffusion-controlled oxidation characteristics under the high-temperature environment. Their mass and residual strength decreased as a power function with time, and decline rate was positively correlated with temperature. Moreover, based on the theory of oxidation kinetics and mass transfer, a macro-meso oxidation model was established to simulate the oxidation process of tubular C/SiC composites in high-temperature environment to timely predict the evolution of their mass and residual strength. Consequentely, all the predicted results of the model fitted well with the experimental data. Our investigation consolidate that this macro-meso oxidation model is powerfull to predict the oxidation behavior and the life-span of C/SiC composite nozzle.

Key words: C/SiC composite, high-temperature oxidation, oxidation model, life prediction

中图分类号:

TB332

全文心, 余艺平, 方冰, 李伟, 王松. 管状C/SiC复合材料高温空气氧化行为与宏细观建模研究[J]. 无机材料学报, 2024, 39(8): 920-928.

QUAN Wenxin, YU Yiping, FANG Bing, LI Wei, WANG Song. Oxidation Behavior and Meso-macro Model of Tubular C/SiC Composites in High-temperature Environment[J]. Journal of Inorganic Materials, 2024, 39(8): 920-928.

图/表 16

图1 管状C/SiC复合材料样品

Fig. 1 Tubular specimen of C/SiC composite

图2 管状C/SiC复合材料环的拉伸实验

Fig. 2 Ring tensile experiment of C/SiC composite

图3 SiC基体热膨胀与氧化愈合裂纹示意图

Fig. 3 Crack healed through thermal expansion and oxidation of SiC matrix

图4 氧气在SiC裂纹中的扩散(a)与在C纤维氧化通道中的扩散(b)

Fig. 4 Diffusion of oxygen in SiC cracks (a) and oxidation channel of carbon fibers (b)

图5 管状C/SiC复合材料管材等效氧化深度示意图

Fig. 5 Equivalent oxidation depth of tubular C/SiC composite

图6 管状C/SiC复合材料高温空气氧化质量保留率(a)、$ \left(1-\eta_{\mathrm{m}}\right)^{2}-t$关系曲线(b)、强度保留率(c)和$ \left(1-\eta_{\mathrm{R}}\right)^{2}-t$关系曲线(d)

Fig. 6 Mass retention rate (a), function fitting of $ \left(1-\eta_{\mathrm{m}}\right)^{2}$ with t (b), strength retention rate (c), and function fitting of $ \left(1-\eta_{\mathrm{R}}\right)^{2}$ with t (d) for tubular C/SiC composites after high-temperature air oxidation

图7 管状C/SiC复合材料表面形貌与元素分布

Fig. 7 Morphology and distributions of elements on the surface of tubular C/SiC composite

图8 管状C/SiC复合材料高温空气氧化拉伸断口微观形貌

Fig. 8 Microstructures at fractures of tubular C/SiC composites after high-temperature air oxidation

图9 管状C/SiC复合材料纤维束的高温空气氧化断口特征形貌

Fig. 9 Microstructures at fractures of carbon fibers in tubular C/SiC composites after high-temperature air oxidation

图10 管状C/SiC复合材料的高温空气氧化截面特征形貌

Fig. 10 Microstructures of cross-sections of tubular C/SiC composites after high-temperature air oxidation

图11 在1100 ℃-1 h(a)、1300 ℃-0.5 h(b)和1300 ℃-1 h(c)高温空气氧化后管状C/SiC复合材料的截面氧元素含量的EDS分布

Fig. 11 EDS distributions of oxygen contents at cross sections of tubular C/SiC composites after 1100 ℃-1 h (a), 1300 ℃-0.5 h (b) and 1300 ℃-1 h (c) high-temperature air oxidation

表1 SiC空气氧化抛物线速率常数

Table 1 Parabolic rate constant of SiC in air oxidation

Parameter	900 ℃	1000 ℃	1100 ℃	1200 ℃	1300 ℃
B/(nm²∙min^-1)	1.05	10.29	39.48	84.84	163.17

表2 氧化10 h的参数计算结果

Table 2 Parameters of oxidation for 10 h

Parameter	900 ℃	1100 ℃	1300 ℃
$ D_{\mathrm{O}_{2}}^{z} $/(m²∙s^–1)	3.18×10^-5	3.53×10^-5	3.86×10^-5
B/(nm²∙s^-1)	0.0175	0.658	2.720
Z/μm	0.0251	0.1539	0.3129
e/μm	1.980	1.835	1.658
$ R_{\mathrm{O}_{2}}^{z} $/(mol∙m^–3∙s^–1)	1.937×10^-2	1.128×10^-2	2.880×10^-1

图12 SiC基体微裂纹中氧气的摩尔分数分布(a)、氧气摩尔分数的梯度分布(b)及氧气摩尔分数随扩散进度的分布(c)

Fig. 12 Distributions of mole fraction of oxygen (a), gradient of mole fraction (b) and mole fraction with diffusion progress (c) in microcracks of SiC matrix

表3 等效氧化深度修正因子

Table 3 Modifying factor of equivalent oxidation depth

Modifying factor	900 ℃	1100 ℃	1300 ℃
$ \beta $	1.2×10^-5	3.1×10^-5	6.0×10^-5

图13 强度保留率(a)与质量保留率(b)的预测结果

Fig. 13 Predicted results of strength retention rate (a) and mass retention rate (b)

参考文献 29

[1]	栾新刚. 3D C/SiC在复杂耦合环境中的损伤机理与寿命预测. 西安: 西北工业大学博士学位论文, 2007.
[2]	张紫煜. 陶瓷基复合材料应用. 中国科技投资, 2016, 18: 308.
[3]	XU Y, ZHANG W. Numerical modelling of oxidized microstructure and degraded properties of 2D C/SiC composites in air oxidizing environments below 800 ℃. Materials Science and Engineering, 2011, 528(27): 7974.
[4]	LACOMBE A, PICHON T, LACOSTE M. High temperature composite nozzle extensions: a mature and efficient technology to improve upper stage liquid rocket engine performance. 43rd AIAA/ASME/SAE/ASEE Joint Propulsion Conference & Exhibit, Cincinnati, 2007: 5471.
[5]	张立同, 成来飞, 梅辉, 等. 陶瓷基复合材料. 北京: 中国铁道出版社, 2020: 12- 42.
[6]	张立同, 成来飞. 连续纤维增韧陶瓷基复合材料可持续发展战略探讨. 复合材料学报, 2007, 2: 1.
[7]	HALBIG M C, MCGUFFIN-CAWLEY J D, ECKEL A J, et al. Oxidation kinetics and stress effects for the oxidation of continuous carbon fibers within a microcracked C/SiC ceramic matrix composite. Journal of the American Ceramic Society, 2008, 2: 519.
[8]	成来飞, 栾新刚, 张立同, 等. 超高温结构复合材料服役行为模拟:理论与方法. 北京: 化学工业出版社, 2020: 174-237.
[9]	CHEN X, SUN Z, CHEN P, et al. Modeling thermal expansion behavior of 2.5D C/SiC composites in air oxidizing environments between 400 ℃ and 800 ℃. Applied Composite Materials, 2020, 6: 861.
[10]	MEI H, TAN Y, CHANG P, et al. Simplified approach to study oxidative damage of C/SiC composites induced from notch defects. Ceramics International, 2019, 45(17): 22464.
[11]	LAMOUROUX F, CAMUS G, THEBAULT J. Kinetics and mechanisms of oxidation of 2D woven C/SiC composites: I. experimental approach. Journal of the American Ceramic Society, 1994, 8: 2049.
[12]	LAMOUROUX F, NASLAIN R, JOUIN J. Kinetics and mechanisms of oxidation of 2D woven C/SiC composites: II, theoretical approach. Journal of the American Ceramic Society, 1994, 8: 2058.
[13]	SULLIVAN R M. A model for the oxidation of carbon silicon carbide composite structures. Carbon, 2005, 43(2): 275.
[14]	ZHAO C, TU Z, MAO J. The dynamic thermophysical properties evolution and multi-scale heat transport mechanisms of 2.5D C/SiC composite under high-temperature air oxidation environment. Composites Part B, 2023, 263: 110831.
[15]	DING J, SUN Z, CHEN X, et al. A progressive oxidative damage model of C/SiC composites under stressed oxidation environments. Applied Composite Materials, 2021, 28(5): 1609.
[16]	颜淮. C/SiC复合材料微细观氧化损伤分析. 哈尔滨: 哈尔滨工业大学硕士学位论文, 2021.
[17]	CHEN P, NIU X, CHEN X, et al. Modeling the failure time and residual strength of C/SiC composites under stress-oxidation environment. Transactions of the Indian Ceramic Society, 2020, 4: 212.
[18]	ZHAO C, TU Z, MAO J. Thermal-oxidation coupled analysis method for unidirectional fiber-reinforced C/SiC composites in air oxidizing environments below 1000 ℃. International Communications in Heat and Mass Transfer, 2023, 143: 106678.
[19]	ECKEL A J, CAWLEY J D, PARTHASARATHY T A. Oxidation kinetics of a continuous carbon phase in a nonreactive matrix. Journal of the American Ceramic Society, 1995, 4: 972.
[20]	OPILA E J, SERRA J L. Oxidation of carbon fiber-reinforced silicon carbide matrix composites at reduced oxygen partial pressures. Journal of the American Ceramic Society, 2011, 7: 2185.
[21]	XIANG Y, CAO F, PENG Z, et al. Evolution of microstructure and mechanical properties of PIP-C/SiC composites after high- temperature oxidation. Journal of Asian Ceramic Societies, 2017, 3: 370.
[22]	SU F, HUANG P, WU J, et al. Creep behavior of C/SiC composite in hot oxidizing atmosphere and its mechanism. Ceramics International, 2017, 12: 9355.
[23]	DRAWIN S, BACOS M, DORVAUX J, et al. Oxidation model for carbon-carbon composites. 4th Symposium on Multidisciplinary Analysis and Optimization, Cleveland, 1992: 5016.
[24]	国义军, 石卫波, 曾磊, 等. 高超声速飞行器烧蚀防热理论与应用. 北京: 科学出版社, 2019: 112.
[25]	DEAL B E, GROVE A S. General relationship for the thermal oxidation of silicon. Journal of Applied Physics, 1965, 12: 3770.
[26]	FILIPUZZI L, NASLAIN R, JAUSSAUD C. Oxidation kinetics of SiC deposited from CH₃SiCl₃/H₂ under CVI conditions. Journal of Materials Science, 1992, 12: 3331.
[27]	SONG Y, DHAR S, FELDMAN L C. Modified deal grove model for the thermal oxidation of silicon carbide. Journal of Applied Physics, 2004, 9: 4953.
[28]	FULLER E N, SCHETTLER P D, GIDDINGS J C. New method for prediction of binary gas-phase diffusion coefficients. Industrial & Engineering Chemistry, 1966, 5: 18.
[29]	KNUDSEN M. The laws of molecular flow and of inner friction flow of gases through tubes. Journal of Membrane Science, 1995, 1: 23.

管状C/SiC复合材料高温空气氧化行为与宏细观建模研究

Oxidation Behavior and Meso-macro Model of Tubular C/SiC Composites in High-temperature Environment

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