Review on accelerated aging and natural aging studies of composites under wet-heat-load conditions
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摘要: 针对复合材料在湿-热-载荷作用下的加速老化与自然老化问题，综述了国内外纤维增强树脂基复合材料在加速老化环境(高温环境、湿热环境、湿-热-载荷耦合)和自然老化条件下的微观老化机制(化学性能、表面裂纹)、宏观力学性能(拉伸、剪切、弯曲)的变化规律，总结了耐久性预测方法的一般流程及其应用进展，提出了复合材料老化失效研究的未来发展趋势。研究结果表明：复合材料受湿-热-载荷影响，在微观性能上主要表现为基体、基体与纤维界面、纤维在物质成分或者组织形态损伤等方面的变化，在宏观上主要表现为拉伸、压缩、剪切、弯曲等力学性能的变化；复合材料老化失效预测方法主要包括选择老化性度量参量、建立耐久性预测模型(线性回归、强度中值老化方程、阿伦尼乌斯模型、人工智能模型)、确定加速老化与自然老化等效关系等环节；未来应深入研究复合材料在老化环境中的微观老化机制和宏观老化性能的内在联系、不同老化环境下老化规律的相关性和定量性分析，进一步揭示复合材料在复杂环境下的老化失效机制；在此基础上，积累各种类型复合材料的加速老化和自然老化失效试验数据，建立更为精准的加速老化与自然老化等效关系，从而实现复合材料的耐久性预测。Abstract: For the accelerated aging and natural aging of composites under wet-heat-load conditions, the change laws of micro aging mechanism (chemical properties and surface cracks) and macroscopic mechanical properties (tensile, shear, and bending) of fiber reinforced resin matrix composites in China and abroad under accelerated aging environments (high temperature environment, hygrothermal environment, and wet-heat-load coupling) and natural aging conditions were reviewed. The general process of durability prediction methods and their application progress were summarized, and the future development trends of aging failure studies of composites were pointed out. Research results show that composites are affected by wet-heat-loading, which is mainly manifested as the changes of matrix, matrix/fiber interface, fiber in terms of material composition or tissue morphology damage in microscopic properties, as well as the changes in mechanical properties such as tensile, compression, shear, and bending in macroscopic properties. The aging failure prediction methods of composites mainly involve the selection of aging metric parameters, the establishment of durability prediction models (linear regression, median strength aging equation, Arrhenius model, and artificial intelligence model), and the determination of an equivalent relationship between accelerated aging and natural aging. In the future, in-depth research should be carried out on the intrinsic connection between the microscopic aging mechanism and macroscopic aging performance of composites in aging environments and the correlation and quantitative analysis of aging laws in different aging environments, so as to further reveal the aging failure mechanism of composites in complex environments. On this basis, accelerated aging and natural aging failure test data of various types of composites can be accumulated, and a more accurate equivalent relationship between accelerated aging and natural aging can be established, so as to realize the prediction of durability of composites. 11 tabs, 122 refs.
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表 1 高温环境对复合材料拉伸性能影响
Table 1. Effects of high temperature environment on tensile properties of composites
材料类型 高温条件/℃ 性能类型 变化规律 文献 CFRP 110、120、130、140 拉伸强度、拉伸模量 变化幅度小且无规律 [21] 80 层间拉伸强度 随着高温老化时间的延长而缓慢降低 [22] 80、-40~80 层间剩余强度 先升高后下降 [23] 175 杨氏模量、拉伸强度 UD试样略有增加，QI试样均有所降低 [24] BFRP 50、100、200、300 拉伸强度 随温度和时间的增加，退化的越快 [25] 25、40、80、120、160、200 拉伸强度 拉伸强度先小幅度升高后线性下降 [26] BFRP、GFRP 20、100、200、300、350 拉伸强度 BFRP筋下降，GFRP筋先升高后下降 [27] 
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表 2 高温环境对复合材料剪切性能影响
Table 2. Effects of high temperature environments on shear properties of composites
材料类型 高温条件/℃ 性能类型 变化规律 文献 CFRP 210、230、250 层间剪切强度 层间剪切强度以线性的方式逐渐降低 [28] 80 层间剪切强度 老化前期层间剪切强度显著提高，后期出现下降趋势 [22] 20、200、350、420、420、500 层间剪切强度 [0°]14层合板先下降后稍有提高，[±45°/0°/90°/45°/0°]2s与之相反 [29] BFRP 120、200 层间剪切强度 先升高后下降 [30] 25、40、80、120、160、200 层间剪切强度 先升高后下降 [26] BFRP、GFRP 20、100、200、300、400、500 剪切强度、最大剪切变形 均呈现先升高后降低的趋势，GFRP下降程度比BFRP大 [27]
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表 3 高温环境对复合材料弯曲性能影响的研究
Table 3. Effects of high temperature environments on bending properties of composites
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表 4 湿热环境对复合材料拉伸性能影响
Table 4. Effects of hygrothermal environments on tensile properties of composite materials
材料类型 湿热环境 性能类型 变化规律 文献 CFRP 70 ℃自来水浸泡 拉伸强度 出现轻微的降低 [49] 70 ℃、25 ℃、85 ℃与烘干、水浴、85%RH组合 拉伸强度 85%RH下，拉伸强度随温度升高而降低，在70℃水浴条件下进一步降低 [50] 25 ℃、50 ℃水浴 拉伸强度 温度越高，下降幅度越大 [51] 80 ℃下95%，-40 ℃下30%RH与80 ℃下95%RH湿热循环 层间强度 随老化时间的增加而降低 [23] BFRP棒材 20 ℃、40 ℃、60 ℃海水环境 拉伸强度、弹性模量 拉伸强度随温度升高和老化时间的延长而下降愈快，弹性模量下降程度很小 [52] BFRP 60 ℃去离子水或碱性溶液 拉伸强度、弹性模量 拉伸强度先迅速下降后较缓慢下降，弹性模量的变化趋势相似，但降解速率较小 [37] GFRP (30±1) ℃和(60±1) ℃的去离子水和盐水 拉伸强度 均略有提高后进入降解阶段，在去离水中吸水量更大，拉伸性能下降幅度也更大 [53] (50±2) ℃、(90±3)%RH 拉伸强度、伸长率、模量 均先略微增加，后以曲线的趋势急剧下降，至某一阶段后平稳下降 [54] GFRP、CFRP 80 ℃水浴 拉伸强度、断裂伸长率 均显著下降，但GFRP比CFRP更容易受到湿热侵蚀 [55]
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表 5 湿热环境对复合材料剪切性能影响
Table 5. Effects of hygrothermal environments on shear properties of composite materials
材料类型 湿热条件 性能类型 变化规律 文献 CFRP 80 ℃、90%RH 层间剪切强度、剪切模量 较大程度的降低 [56] 100 ℃去离子水 层间剪切强度 先上升后下降，下降幅度很小 [57] 40 ℃、60 ℃、80 ℃水浴 短梁剪切强度 初期下降相对较快，而后逐渐减慢 [43] GFRP (20±5) ℃、(30±1) ℃和(60±1) ℃的去离子水和盐水 层间剪切强度 浸泡温度越高，层间剪切性能的下降幅度越大，而盐水对其影响较小 [53] CFRP、GFRP 40 ℃、60 ℃和80 ℃去离子水 界面剪切强度 随着时间和温度的增加显著降低 [58] CFRP、BFRP、GFRP 25 ℃、40 ℃、55 ℃的海水溶液环境 水平剪切强度 随着暴露时间和温度的增加而降低，BFRP下降幅度最大 [59]
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表 6 v
Table 6. Effects of hygrothermal environments on bending properties of composite materials
材料类型 湿热条件 性能类型 变化规律 文献 CFRP 25 ℃、50 ℃水浴 弯曲强度、弯曲模量 随着水浴温度的升高下降越显著 [51] 25 ℃、70 ℃蒸馏水 弯曲强度 前期下降趋势非常剧烈，后期变得较为缓慢 [39] 90 ℃、30%RH 弯曲强度、弯曲模量 强度先升高后下降最后趋于平缓，模量未发生变化 [60] 100 ℃去离子水 弯曲强度、弯曲模量 强度先急剧下降后略有升高再显著降低，模量初始阶段保持不变后略有降低 [57] 60 ℃蒸馏水和碱性溶液 弯曲强度 前期下降较快，后期下降速率较为缓慢，试件厚度越厚弯曲强度保持率越高 [36] 30 ℃、50 ℃水浴 弯曲强度、弯曲模量 随着水浴温度的升高下降越显著 [61] BFRP 35 ℃去离子水 弯曲强度、弯曲模量、弯曲刚度 强度显著降低，模量和刚度未发生明显变化 [62] GFRP 60 ℃、95%RH 弯曲强度、弯曲模量 弯曲强度下降幅度较小，弯曲模量变化不大 [63]
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表 7 湿-热-载荷耦合作用对纤维增强复合材料力学性能影响
Table 7. Effects of moisture-thermal-load coupling on mechanical properties of fiber reinforced composites
材料类型 耦合作用条件 性能类型 变化规律 文献 BFRP 25 ℃、40 ℃和55 ℃盐碱性水，冲击载荷 拉伸强度 暴露温度和冲击能量越高，拉伸强度保持率越低 [69] GFRP 40 ℃、70 ℃水浴，横向预载荷 拉伸强度 温度越高、预载荷量越大，拉伸强度下降越明显 [70] HFRP 25 ℃、40 ℃和55 ℃水浸，弯曲载荷 剪切强度 随着浸泡温度和负载水平的提高而逐渐降低 [73] CFRP 湿热循环(-40 ℃下30%RH与80 ℃下95%RH) 和高低温循环(-40 ℃~80 ℃)，载荷水平1 MPa 拉伸强度、剪切强度 强度降低，湿热循环的影响更大 [23] (37.0±0.5) ℃的蒸馏，弯曲载荷 剪切强度 剪切强度在初期时下降速度加快，后期正好相反 [72] 70 ℃水浸，弯曲载荷 弯曲强度 负荷水平越高，强度下降幅度越大 [39] 80 ℃、23 ℃、-35 ℃，80%RH、50%RH，弯曲载荷 弯曲强度 载荷水平越高、孔隙率越大，弯曲强度下降幅度越大 [74]
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表 8 自然老化对纤维增强复合材料拉伸性能影响
Table 8. Effects of natural aging on tensile properties of fiber reinforced composites
材料类型 地区选择 性能类型 变化规律 文献 CFRP 北京 拉伸强度、弹性模量、伸长率 拉伸强度有较小幅度的下降，而弹性模量和伸长率的变化不明显 [80]、[81] 葡萄牙 拉伸强度、弹性模量 均有所增加，但随着老化时间的继续增加其拉伸性能依旧会降低 [82] 海南省万宁市 拉伸强度 先升高后降低 [1] GFRP 西双版纳 拉伸强度、拉伸弹性模量 拉伸强度和模量先升高后降低 [83] 马来西亚 拉伸强度 下降较明显 [84] 里斯本市中心 拉伸强度、拉伸模量 呈现先轻微地下降后升高 [85] GFRP、BFRP 郑州 拉伸强度 BFRP筋小幅度下降后升高又出大幅度下降，GFRP筋升高后降低再升高到初始值相近 [86] GFRP、CFRP 吉林 拉伸强度 降低后升高再降低，最终下降幅度均较小 [87]
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表 9 自然老化对纤维增强复合材料剪切性能影响
Table 9. Effects of natural aging on shear properties of fiber reinforced composites
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表 10 自然老化对纤维增强复合材料弯曲性能影响
Table 10. Effect of natural aging on flexural properties of fiber reinforced composites
材料类型 地区 性能类型 变化规律 文献 CFRP 黑龙江省漠河县 挠度 无明显变化 [75] 海南省万宁市 纵向弯曲强度 呈现逐步升高的趋势 [1] GFRP 里斯本市中心 弯曲强度、弯曲模量 VE型材的弯曲性能退化程度较高，UP型材无明显变化 [85] 西双版纳 弯曲强度、弯曲弹性模量 弯曲强度先小幅度下降后出现较大幅度的下降趋势，弯曲弹性模量无明变化 [83] 黑龙江省漠河县 剩余弯曲强度 呈现出先逐渐上升后下降的趋势 [92] FFRP 南京 弯曲强度、弯曲模量 弯曲模量降低程度比弯曲强度大 [93] 稻壳-PE复合材料 黑龙江省哈尔滨市 弯曲强度、弹性模量 下降后有所升高，基本上没有变化 [94]
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表 11 纤维增强复合材料耐久性预测结果
Table 11. Durability prediction results of fiber reinforced composites
材料类型 加速老化环境 位置 分析方法 文献 CFRP 加速腐蚀试验 厦门鼓浪屿 强度中值老化方程、老化损伤等效原则 [121] 紫外-湿热交替循环(60 ℃、5%NaCl溶液) 南中国海海域(实海随舰) 强度中值老化方程、老化损伤等效原则 [122] 紫外照射试验 南海环境 强度中值老化方程、老化损伤等效原则 [88] GFRP 光老化、高温浸水、湿热老化、热空气老化 万宁、拉萨 灰色关联分析、线性回归方程、老化损伤等效原则 [97] 不同温度(20 ℃、40 ℃、60 ℃)碱溶液及盐溶液环境 湖北武汉 灰色关联分析、线性回归方程、老化损伤等效原则 [101] 热空气加速老化、光加速老化湿热老化 西双版纳、厦门、济南、万宁、拉萨、漠河 方差分析、二元线性回归方程 [102] 不同pH环境和不同温度的不同溶液 西弗吉尼亚大学 阿伦尼乌斯模型、时间-温度叠加原理 [90] 大麻纤维增强PP生物复合材料 人工风化 法国西南部 PCA、老化损伤等效原则 [100] FFRP 湿热环境(60 ℃、100%RH) 南京 PCA、老化损伤等效原则 [93]
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