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Article(id=1210601624486147012, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210601623135581115, articleNumber=null, orderNo=null, doi=10.16790/j.cnki.1009-9239.im.2024.10.011, pmid=null, cstr=null, oa=null, hot=null, price=null, onlineType=0, articleFormat=0, articleType=null, articleTypeStr=research-article, receivedDate=1714060800000, receivedDateStr=2024-04-26, revisedDate=1717516800000, revisedDateStr=2024-06-05, acceptedDate=null, acceptedDateStr=null, onlineDate=1766559519168, onlineDateStr=2025-12-24, pubDate=1729353600000, pubDateStr=2024-10-20, doiRegisterDate=null, doiRegisterDateStr=null, onlineIssueDate=1766559519168, onlineIssueDateStr=2025-12-24, onlineJustAcceptDate=null, onlineJustAcceptDateStr=null, onlineFirstDate=null, onlineFirstDateStr=null, sourceXml=null, magXml=null, createTime=1766559519168, creator=13701087609, updateTime=1766559519168, updator=13701087609, issue=Issue{id=1210601623135581115, tenantId=1146029695717560320, journalId=1149653034449285133, year='2024', volume='57', issue='10', pageStart='1', pageEnd='141', issueExtLink='null', onlineDate='null', pubDate='null', beforeIssueId=null, nextIssueId=null, price=null, status=1, issueComplete=1, articleOrder=1, issueType=-1, specialIssue=null, createTime=1766559518846, creator=13701087609, updateTime=1766564021205, updator=13701087609, preIssue=null, nextIssue=null, ext={EN=IssueExt(id=1210620507448275814, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210601623135581115, language=EN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=), CN=IssueExt(id=1210620507448275815, tenantId=1146029695717560320, journalId=1149653034449285133, issueId=1210601623135581115, language=CN, specialIssueTitle=, coverIllustrator=null, specialIssueEditor=, specialIssueAbout=)}, issueFiles=null}, startPage=84, endPage=90, ext={EN=ArticleExt(id=1210601624721028040, articleId=1210601624486147012, tenantId=1146029695717560320, journalId=1149653034449285133, language=EN, title=Molecular dynamics study on mechanism of atomic oxygen erosion resistance of polysiloxane-polyimide composites, columnId=1203281640207393262, journalTitle=Insulating Materials, columnName=Special Issue on High Performance Polyimide Materials, runingTitle=null, highlight=null, articleAbstract=

In order to investigate the improving mechanism of polysiloxane with different substituents on atomic oxygen (AO) erosion resistance of polyimide in space environments, reactive molecular dynamics (MD) simulations was used to analyze the AO erosion resistance of PI composited with polyhedral oligomeric silsesquioxane (POSS) with trifluoromethyl (-CF3) group and methyl (-CH3) group. The results show that both the composites exhibit strong AO erosion resistance by forming an SiO2 layer that blocks AO propagation into the polymer matrix and and heat transfer. The PI/CF3-POSS shows the best performance, and its normalized mass is 0.83 after 35 ps of AO exposure, while the nomalized mass of the PI/CH3-POSS composite is 0.78.

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为了探究不同取代基聚硅氧烷提升聚酰亚胺在太空环境中抵抗原子氧（AO）侵蚀能力的作用机制，本研究采用反应分子动力学（MD）模拟，分析了取代基分别为三氟甲基（-CF3）和甲基（-CH3）的多面体笼型聚硅氧烷（POSS）复合聚酰亚胺纳米材料的抗原子氧侵蚀性能。结果表明：PI/CH3-POSS和PI/CF3-POSS复合材料均表现出较强的抗AO侵蚀能力，其作用机制是通过形成SiO2层以阻止AO向聚合物基体的传播和热量的传递，其中PI/CF3-POSS复合材料的效果最优，经35 ps的AO侵蚀模拟后其归一化质量为0.83，而PI/CH3-POSS复合材料的归一化质量为0.78。

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张黎（1979-），男（汉族），山东济宁人，副教授，研究方向为高电压与绝缘技术。
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周生睿（1999-），男（汉族），山东枣庄人，博士生，研究方向为高电压与绝缘技术。

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周生睿（1999-），男（汉族），山东枣庄人，博士生，研究方向为高电压与绝缘技术。

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周生睿（1999-），男（汉族），山东枣庄人，博士生，研究方向为高电压与绝缘技术。

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聚硅氧烷-聚酰亚胺复合材料抗原子氧侵蚀机理分子动力学研究
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周生睿 1 , 张黎 1 , 邹亮 1 , 孙秋芹 2
绝缘材料 | 高性能聚酰亚胺材料专题 2024,57(10): 84-90
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绝缘材料 | 高性能聚酰亚胺材料专题 2024, 57(10): 84-90
聚硅氧烷-聚酰亚胺复合材料抗原子氧侵蚀机理分子动力学研究
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周生睿1, 张黎1, 邹亮1, 孙秋芹2
作者信息
  • 1山东大学 电气工程学院,山东 济南 250061
  • 2湖南大学 电气与信息工程学院,湖南 长沙 410082

    • 周生睿（1999-），男（汉族），山东枣庄人，博士生，研究方向为高电压与绝缘技术。

通讯作者:

张黎（1979-），男（汉族），山东济宁人，副教授，研究方向为高电压与绝缘技术。
Molecular dynamics study on mechanism of atomic oxygen erosion resistance of polysiloxane-polyimide composites
Shengrui ZHOU1, Li ZHANG1, Liang ZOU1, Qiuqin SUN2
Affiliations
  • 1School of Electrical Engineering, Shandong University, Jinan 250061, China
  • 2College of Electrical and Information Engineering, Hunan University, Changsha 410082, China
出版时间: 2024-10-20 doi: 10.16790/j.cnki.1009-9239.im.2024.10.011
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摘要
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为了探究不同取代基聚硅氧烷提升聚酰亚胺在太空环境中抵抗原子氧（AO）侵蚀能力的作用机制，本研究采用反应分子动力学（MD）模拟，分析了取代基分别为三氟甲基（-CF3）和甲基（-CH3）的多面体笼型聚硅氧烷（POSS）复合聚酰亚胺纳米材料的抗原子氧侵蚀性能。结果表明：PI/CH3-POSS和PI/CF3-POSS复合材料均表现出较强的抗AO侵蚀能力，其作用机制是通过形成SiO2层以阻止AO向聚合物基体的传播和热量的传递，其中PI/CF3-POSS复合材料的效果最优，经35 ps的AO侵蚀模拟后其归一化质量为0.83，而PI/CH3-POSS复合材料的归一化质量为0.78。

聚酰亚胺  /  原子氧  /  笼型聚硅氧烷  /  三氟甲基

In order to investigate the improving mechanism of polysiloxane with different substituents on atomic oxygen (AO) erosion resistance of polyimide in space environments, reactive molecular dynamics (MD) simulations was used to analyze the AO erosion resistance of PI composited with polyhedral oligomeric silsesquioxane (POSS) with trifluoromethyl (-CF3) group and methyl (-CH3) group. The results show that both the composites exhibit strong AO erosion resistance by forming an SiO2 layer that blocks AO propagation into the polymer matrix and and heat transfer. The PI/CF3-POSS shows the best performance, and its normalized mass is 0.83 after 35 ps of AO exposure, while the nomalized mass of the PI/CH3-POSS composite is 0.78.

polyimide  /  atomic oxygen  /  polyhedral oligomeric silsesquioxane  /  trifluoromethyl
周生睿, 张黎, 邹亮, 孙秋芹. 聚硅氧烷-聚酰亚胺复合材料抗原子氧侵蚀机理分子动力学研究. 绝缘材料, 2024 , 57 (10) : 84 -90 . DOI: 10.16790/j.cnki.1009-9239.im.2024.10.011
Shengrui ZHOU, Li ZHANG, Liang ZOU, Qiuqin SUN. Molecular dynamics study on mechanism of atomic oxygen erosion resistance of polysiloxane-polyimide composites[J]. Insulating Materials, 2024 , 57 (10) : 84 -90 . DOI: 10.16790/j.cnki.1009-9239.im.2024.10.011
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0 引言
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聚酰亚胺（PI）是一种具有优异耐高低温和电气绝缘性能的芳香杂环聚合物，广泛用于航空航天领域[1-4]。然而在低地球轨道（LEO），高浓度原子氧（AO）与聚合物表面的相对撞击能量为4.5～5.0 eV[5-7]，具有高反应活性的原子氧可导致聚合物材料表面开裂和性能劣化[8-9]，成为低地球轨道航天用聚合物材料的首要威胁，会显著降低航天器的在轨寿命。因此，研究PI抵抗AO侵蚀的调控方法至关重要。
在聚合物表面涂覆抗氧化涂层是一种有效的抵抗AO侵蚀方法。典型的防护涂层包括多面体倍半硅氧烷（POSS）[10-13]、Al2O3[14]、SiO2[15]和石墨烯（Gr）[16-18]等。其中通过POSS涂层增强聚合物抵抗AO侵蚀的研究备受关注，POSS在AO的侵蚀作用下可转化为致密的SiOx碳化层[19]，表现出优异的隔热、阻燃和抗原子氧侵蚀性能[20-22]。R Y M LOPEZ等[23]制备了含POSS的环氧树脂复合材料，发现AO的侵蚀使材料表面形成硅富集涂层，降低了侵蚀后表面的粗糙度。LIU F等[24]制备了PI和多面体倍半硅氧烷铵盐复合纤维并进行AO侵蚀实验，结果发现随着POSS铵盐含量的增加，复合纤维在AO环境下表现出更低的侵蚀率和更好的力学性能保持率。XU H Z等[25]通过射频磁控溅射技术得到了具有不同生长时间的SiO2/POSS/Kapton样品，发现处理6 h后样品的AO侵蚀率仅为原始材料的6%，表现出优异的抗AO侵蚀能力。XU C等[26]在PI表面原位生长氨基化的POSS层，并通过溶胶-凝胶法在此POSS层上制备了SiO2涂层，这种复合材料表现出卓越的抗AO侵蚀性能。
在此基础上，针对POSS的改性尤为重要，其中通过引入氟元素对POSS进行功能化是提高聚合物性能的有效策略。M IACOB等[27]通过水解-缩合法合成了含氟多面体倍半硅氧烷（F-POSS），并以不同比例掺入聚二甲基硅氧烷（PDMS）中，结果表明，F-POSS的加入增强了复合材料的机械强度和介电性能。LIU Y等[28]使用溶剂蒸发方法制备了不同氟丙基聚倍半硅氧烷（FP-POSS）含量的聚偏二氟乙烯纳米复合材料，实验结果表明FP-POSS的均匀分布在纳米级别上改善了PVDF的力学性能。LIANG J Y等[29]研究加入含氟单元和多面体倍半硅氧烷对聚二甲基硅氧烷热稳定性的影响，发现共聚物的热稳定性有所提高。
通过分布式计算进行全原子分子动力学（MD）模拟已被广泛用于研究航空级聚合物表面分解和温度演化行为。R FARZIN等[30]利用反应性分子动力学模拟方法，研究了在PI基体中引入不同纳米粒子（包括石墨烯和碳纳米管）对原子氧侵蚀的抵抗效果，结果表明加入随机取向的石墨烯和碳纳米管后PI具有较好的AO侵蚀抵抗能力。J INSEOK等[31]通过反应分子动力学模拟，研究了Kapton型聚酰亚胺纳米复合材料在原子氧和氮气侵蚀下的温度演化过程，结果发现由于轰击分子的能量传递和材料的化学反应性不同，Kapton模型暴露在不同类型和数量的轰击分子下的温度上升速率有所不同。WEI D H等[32]详细记录了在AO持续撞击下PI的温度演化过程，发现当撞击负荷达到一定阈值后，原子的热运动显著增强并伴随着更严重的PI基质损伤。
基于此，本研究通过ReaxFF分子动力学综合研究全氟甲基多面体笼型聚硅氧烷（CF3-POSS）和全甲基多面体笼型聚硅氧烷（CH3-POSS）聚酰亚胺纳米复合材料在AO侵蚀中的耐蚀表现和温度演化过程。定量分析AO侵蚀过程中复合系统的质量损失、侵蚀产物、损伤传播深度和温度演化过程，阐明AO侵蚀过程中PI的降解机制。希望能为抗AO侵蚀分子材料的结构设计提供理论依据。
1 方法与模型
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本研究使用LAMMPS软件中的Reax模块模拟AO碰撞。Reaxff力场在每个MD模拟步长中对键长、键级以及键级与键能的关系进行更新与分析，从而能够在模拟过程中实现键的形成与断裂[33-34]。同时在一定程度上忽略原子内电子转移和相对论效应等细节，从而保证计算效率。此外，它还考虑了分子间的相互作用，如范德华力和库仑力。Reaxff力场中的总势能表示为式（1）。
Esystem=Ebond+Eover+Eunder+Eval+Epen+Etors+Econj+EvdWaals+ECoulomb
式（1）中：Ebond代表键能；Eover和Eunder是过配位和欠配位的能量修正项；Eval代表价角能量；Epen代表处罚能量；Etors代表扭转能量；Econj表示分子共轭效应； EvdWaals代表非键合范德华作用力；ECoulomb代表非键合库仑作用力。
图1展示了本研究中所采用的每种分子构型以及PI、PI/CH3-POSS和PI/CF3-POSS三种平衡晶胞结构。首先，向尺寸为20 Å×20 Å×60 Å的空白周期性单元盒中填充42个Kapton型PI单体进行建模，然后对模型进行目标温度为298 K、大气压条件下的NPT（恒定压强，恒定温度）系综弛豫，以获得致密的晶胞块体结构。在此过程中，晶胞的密度逐渐减小至平衡密度（ρPI=1.35 g/cm3），与实测密度(1.41±0.2) g/cm3接近，稳定的晶胞尺寸为20.14 Å×20.14 Å×50.34 Å。为防止AO侵蚀过程中模型发生偏移，将模型底部20 Å固定设置为基底缓冲层，同时取消Z方向的周期性边界条件并延长至120 Å，最后对模型进行温度为300 K、时间为500 ps的NVT（恒定体积，恒定温度）系综弛豫。使用与纯PI模型相同的建模过程对聚硅氧烷主笼质量分数为9.07%的PI/CH3-POSS和PI/CF3-POSS纳米复合材料进行建模，得到平衡密度分别为ρCH3=1.33 g/cm3和ρCF3=1.40 g/cm3，稳定的晶胞尺寸分别为20.70 Å×20.70 Å×53.99 Å和20.52 Å×20.52 Å×53.51 Å。
在此项计算中将动能为5 eV的AO插入到模型表面上方50 Å处，剂量率为5 atoms/ps，模拟的时间步长为0.1 fs。为了直观地观察模型表面的结构变化，所有的AO侵蚀模拟都在NVE（恒定体积，恒定能量）系综下完成。建模过程使用BIOVIA Materials Studio（MS）完成，使用的是A R AHNAMDUN等[35]开发的力场参数集。
2 结果与讨论
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2.1 纯PI、PI/CH3-POSS和PI/CF3-POSS纳米复合材料侵蚀动力学
图2展示了AO侵蚀过程中3个模型的结构变化。从图2可以看出，由于高能AO的侵蚀，3个模型都出现不同程度的损伤，聚合物分子开始裂解生成大量的气态分子碎片，其中纯PI底部出现了松散和裂解现象，这是因为高活性AO不仅会与PI分子发生反应，还会将大量的热量注入聚合物中，当底部的PI分子温度升高到热解阈值时，PI分子开始大规模热解。相比之下，PI/CH3-POSS和PI/CF3-POSS模型底部保持相对致密和完整的状态，整体比纯PI模型的损伤程度低。这是因为PI/CH3-POSS和PI/CF3-POSS模型在AO侵蚀过程中产生了大量的SiOx产物，并作为物理屏障覆盖在复合材料表面最先与AO发生反应，显著减少了AO对复合材料的冲击。
为了定量分析不同模型的耐AO侵蚀效果，计算了AO侵蚀过程中聚合物模型的归一化质量，将模拟过程中AO侵蚀后剩余的模型质量除以初始模型质量即可得到归一化质量，如图3所示。从图3可以看出，AO侵蚀35 ps后，PI/CF3-POSS保留的质量最多（0.83），表现出最佳的耐AO侵蚀效果，PI/CH3-POSS的耐AO侵蚀效果次之。在侵蚀过程中归一化质量有很大范围的波动，这是因为从模型分离出的小分子碎片游离到模型上方，遇到高速AO冲击后可能重新回到模型表面，使模型表面变得粗糙。在AO侵蚀的初始阶段，3个模型的归一化质量都出现了不同程度的上升，这是因为初始阶段AO的能量注入尚未达到PI大量裂解的阈值，AO被PI基体吸收，表现出对AO的“耐受性”，其中PI/CF3-POSS的耐AO侵蚀性能最佳。
提取了模拟过程中AO侵蚀的最大损伤传播深度，结果如图4所示。从图4可以看出，与纯PI模型相比，PI/CH3-POSS和PI/CF3-POSS复合模型较大程度地抑制了AO侵蚀对聚合物的损伤传播，说明表层的CH3-POSS和CF3-POSS吸收了AO的冲击能量。由于氟原子具有强电负性，C-F键具有较高的键能，表现出较强的化学稳定性，极难与AO发生氧化反应，因此即使在较高AO密度的侵蚀作用下，-CF3也表现出相对的惰性，使CF3-POSS对AO侵蚀的抵抗效果最好，最大损伤传播深度为28%。
2.2 AO侵蚀过程中模型的温度演化
为了研究3个模型在AO侵蚀下的温度演化规律，计算了3个模型的整体温度分布和PI/CH3-POSS和PI/CF3-POSS复合模型中PI成分的温度分布，如图5所示。
从图5可以看出，3个模型整体的温度变化趋势基本相同，经过35 ps的AO侵蚀后，复合模型的整体平均温度均达到了1 200 K左右，纯PI模型达到了1 400 K左右，局部的高温会使PI分子大量裂解。PI/CH3-POSS和PI/CF3-POSS复合模型中的PI成分温升得到了有效抑制，表明CH3-POSS和CF3-POSS的存在有效减缓了热量向内部传递，经过AO的持续侵蚀后，POSS中的Si-O-Si键裂解，被AO氧化生成大量的SiOx成分并覆盖在PI的上方，阻止AO与PI碰撞的同时也带走了体系大量的热量。
分别计算了3个模型在模拟的第10、15、20 ps时Z=30～35 Å部分的局部温度，如图6所示。
从图6可以看出，在AO侵蚀的初始阶段（前10 ps），3个模型均未出现大规模的局部热点，随着AO侵蚀的持续进行，高反应活性AO的撞击使得温度持续升高，PI模型出现局部热点并开始裂解。当模拟进行到20 ps时，PI模型已出现大量的局部热点，相比之下，PI/CH3-POSS和PI/CF3-POSS复合模型的温度分布相对均匀。PI/CF3-POSS复合模型出现的热点最少，这是因为-CF3的高稳定性使得大量的AO都无法穿透表层CF3-POSS。由此可以推断，AO的持续撞击和氧化反应导致的PI分子裂解是模型质量损失的主要原因，而CH3-POSS和CF3-POSS附着在聚合物表面有效阻挡了AO向PI内部侵蚀和热量传递，因此PI/CH3-POSS和PI/CF3-POSS表现出较好的耐AO侵蚀效果。
2.3 AO侵蚀副产物分析
在模拟过程中，统计了距板胚表面10 Å以上分离出来的小分子物质种类和数量，结果如图7所示。从图7可以看出，收集的主要产物有羟基自由基、CO、O2、H2O以及C3～C4、C5～C7小分子碳链。由于CH3-POSS中甲基的存在，PI/CH3-POSS模型分离出大量的羟基自由基和CO，在AO与PI的反应过程中，羟基自由基由AO碰撞脱氢产生，游离的羟基自由基与PI分子再次发生脱氢反应生成H2O；O2分子由AO与亚胺环或含氧取代基直接碰撞形成，由于破坏了原本的电子系统平衡，苯环和亚胺环开始分解生成CO。由于CF3-POSS的反应惰性，只有一定数量的AO持续注入后，PI/CF3-POSS中的PI成分暴露在AO环境中，才开始大量生成小分子副产物，因此总体的副产物数量都居于较低水平。
为了系统地研究AO侵蚀过程中模型分离产生副产物的规律，以PI/CF3-POSS复合模型为例，研究了动能为10、15、20 eV的AO能量注入下的侵蚀规律，其中10 eV能量注入下的副产物分离曲线和侵蚀快照如图8所示。从图8可以看出，随着侵蚀时间的增加，CF3-POSS失去侵蚀抵抗能力，裂解为大量碎片，PI完全暴露在AO侵蚀环境中，PI/CF3-POSS复合模型发生剧烈崩解，PI分子结构的断裂变得更加明显。CO和OH的生成数量也随侵蚀时间的增加而逐渐上升，表明AO与酰亚胺环的碰撞和PI的脱氢成为主导反应，CO和OH成为主要生成产物，O2和H2O的变化相对稳定。
3 结论
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（1）在纯PI、PI/CH3-POSS以及PI/CF3-POSS复合模型的AO侵蚀模拟中发现，AO对聚合物的侵蚀作用体现在使聚合物温度升高导致的聚合物热解和AO氧化侵蚀两部分，其中，由于氟原子的强电负性使得C-F键具有较高的键能，PI/CF3-POSS复合模型表现出较强的化学稳定性，耐AO侵蚀效果最佳，经35 ps的AO侵蚀模拟后其归一化质量为0.83，最大损伤传播深度为27%；PI/CH3-POSS复合模型的归一化质量为0.78，最大损伤传播深度为36%。在高活性AO的作用下，POSS转换为大量的SiOx，阻止AO进一步向PI基体的侵蚀。
（2）在AO侵蚀过程中模型整体温度上升，而PI/CH3-POSS和PI/CF3-POSS复合模型中PI成分的温升得到了明显的抑制，局部热点显著减少，这归因于POSS充当了AO侵蚀的物理屏障，其中-CF3具有较强的稳定性，使CF3-POSS能更有效地阻挡AO热量向内部传递。
（3）在AO侵蚀过程中，3个模型均产生大量的小分子产物，主要包括CO和OH，这些产物是由AO与PI发生碰撞和脱氢反应生成的，随着侵蚀时间的增加，产物数量也呈现出逐步上升的趋势。
基金
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  • 国家自然科学基金资助项目(52077127)
文献
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2024年第57卷第10期
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doi: 10.16790/j.cnki.1009-9239.im.2024.10.011
  • 接收时间：2024-04-26
  • 首发时间：2025-12-24
  • 出版时间：2024-10-20
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  • 收稿日期：2024-04-26
  • 修回日期：2024-06-05
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国家自然科学基金资助项目(52077127)
作者信息
    1山东大学 电气工程学院,山东 济南 250061
    2湖南大学 电气与信息工程学院,湖南 长沙 410082

通讯作者:

张黎（1979-），男（汉族），山东济宁人，副教授，研究方向为高电压与绝缘技术。
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2种不同金属材料的力学参数
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Number of
species		 占总种数比例
Percentage of
total species (%)		 属
Genus		 种数
Number of
species		 占总种数比例
Percentage of total
species (%)
鹅膏菌科Amanitaceae 2 11 5.26 鹅膏菌属 Amanita 10 4.78
小菇科 Mycenaceae 2 12 5.74 丝盖伞属 Inocybe 5 2.39
多孔菌科 Polyporaceae 8 14 6.70 蜡蘑属 Laccaria 5 2.39
红菇科 Russulaceae 3 23 11.00 小皮伞属 Marasmius 6 2.87
小菇属 Mycena 11 5.26
光柄菇属 Pluteus 5 2.39
红菇属 Russula 17 8.13
栓菌属 Trametes 5 2.39
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