目的 聚酰亚胺材料（PI）凭借优异的热稳定和耐弯折等特性,广泛应用在各类航天器上。随着卫星技术的发展,特别是低地球轨道卫星和空间站等任务提出的更高通量原子氧（AO）防护要求,PI材料空间耐久性试验评价变得十分困难,急需要开展试验和模拟相结合的方法,较低成本完成PI在原子氧辐照环境下的寿命评价工作。目前,PI降解模型的构建细节和从模拟结果到实验的外推方法仍需要进一步完善。方法 本研究基于第一性原理计算和分子动力学计算组合方法来构建PI纳米尺度模型,通过调控聚合度和AO剂量率等参数优化模型,基于实验关键节点的表征结果来验证模拟结果。结果 研究发现,聚合密度约为1.32 g/cm3、表面积为12.2 nm2的PI模型,在5 AOs/ps剂量率的AO连续辐照下,在90 ps时质量损失达50%（质量分数）,PI受严重剥蚀,等效于实际厚度为50 μm、表面积4.5 cm2的PI薄膜经历9.26× 1020 atoms/cm2的AO通量辐照后的质量损失结果;相应地,地面试验时间约24 h。此外,在模拟运行时间为10~140 ps时,计算得到的侵蚀率在3×10-24 cm3/atom附近,由模拟得到的质量损失规律等都能和实验结果匹配。结论 通过计算模拟和实验关键节点验证相结合,可获得PI材料的AO辐照寿命评价模拟方法。该方法有望推广到PI基复合材料和其他有机薄膜材料的长期寿命评估上,在航天工程领域意义重大。
Abstract
Polyimides (PI) are widely used in many spacecrafts due to their excellent properties (such as exceptional thermal stability, remarkable resistance to flexural wear, excellent dielectric properties, etc.). With the development of satellite technology, particularly the increased demands for atomic oxygen (AO) protection in low earth orbit satellites and space station missions, the durability evaluation of PI in space has become extremely challenging. There is an urgent need to develop a method that combines experiments and simulations to cost-effectively complete the lifetime assessment of PI in the AO irradiation environment. Up to now, the specifics of constructing the PI degradation model and the extrapolation methods from simulation results to experiments still require further refinement to evaluate the lifetime of PI and its composites in the AO irradiation. Hence, the study tries to construct a nano-scale PI model through the combination of first-principle calculations (DFT) and molecular dynamics (MD) simulations. The model is optimized by adjusting some parameters. The exchange- correlation potential is approximated with the Perdew-Burke-Ernzerhof (PBE) functional; both geometry optimization and energy optimization of the system are calculated until the maximum force and self-consistent field (SCF) tolerance is lower than threshold value. The degree of polymerization is selected as 1, 5, 10, 50 and 100, which can adjust the final density of the nanoscale model; the AO dose rate is adjusted from 200 to 5 AOs/ps. These simulation results are verified based on the experimental characterization of the key nodes (an AO exposure experiment is carried with AO fluence of 1.43×1020, 4.33×1020, 5.65×1020, 9.26×1020 and 1.93×1021 atoms/cm2, respectively; then some macroscale and microscale morphology characterization and structural characterization are done to obtain sample information. Meanwhile, simulation data need to match experimental data, such as density, normalized mass loss, erosion yield, etc. Here, when the simulation is carried out with a PI density of ~1.32 g/cm3, a PI surface area of 12.2 nm2, at a dose rate of 5 AOs/ps, with the "ppf" boundary condition and continuous injection of AOs, the mass loss reaches 50% (mass fraction) at the 90 ps, and large amounts of gases (like CO and H2O) are produced. The PI is severely eroded, equivalent to the mass loss of the PI film with an actual thickness of 50 micrometers and a surface area of 4.5 cm2 with an AO fluence of 9.26×1020 atoms/cm2. The corresponding ground test time is approximately 24 hours. In addition, when the running time of simulation is approximately 10-140 ps, the erosion yield is between 0.77×10-24 and 6.38×10-24 cm3/atom, which is close to the erosion yield of the PI sample (3×10-24 cm3/atom). The transformation law of normalized mass loss obtained from the simulation can match the experimental characterization results. Therefore, by combining multiscale simulation and experimental key-node verification, a proper simulation method for the lifetime evaluation of PI under AO irradiation is obtained. This method is expected to be extended to the long-term lifetime assessment of PI-based composites and other organic materials, and it is of prominent significance in aerospace engineering.
关键词
低地球轨道 /
原子氧 /
聚酰亚胺 /
分子动力学计算 /
侵蚀率
Key words
low Earth orbit /
atomic oxygen /
polyimide /
molecular dynamics calculation /
erosion yield
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基金
国家自然科学基金项目（12305289,12475277）; 甘肃省重点研发计划-工业类项目（26YFGA013）; 装备预研重点实验室基金项目（6142207220102）
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