本文主要研究内容
作者任萍(2019)在《过渡族金属碳(氮)化物基薄膜的强韧化设计及其摩擦学性能研究》一文中研究指出:过渡族金属碳(氮)化物基薄膜的强韧化设计及其摩擦学性能研究过渡族金属碳(氮)化物(TMC(N))薄膜由于其高硬度、高熔点及高化学惰性的特点被认为是一种非常重要的表面防护用材料,可用于防止各种零部件表面的划擦、磨损和腐蚀,在精密机械、生物植入、交通运输、刀具、航空工业和地质勘探等领域表现出巨大的应用潜力。随着工业技术的飞速发展,复杂的使用环境对薄膜材料的硬度提出了更高的需求,通过强化TMC(N)基薄膜来拓宽其应用领域已成为当前的研究热点。然而,硬度与韧性通常此消彼长,硬度的增强往往以牺牲韧性为代价。显然,对于TMC(N)薄膜来说,追求更高的硬度并改善其韧性仍然是一个重要的挑战。此外,在改善TMC(N)薄膜硬度和韧性的同时,低摩擦系数(CoF)和低磨损率对提高其耐久性和服役寿命也至关重要。因此,在设计和选取强韧化方案时,降低CoF和改善薄膜的抗磨损性能也被视为重要的评价标准。基于以上分析,我们采用三种不同的策略来实现TMC(N)基薄膜的强韧化设计并观察其对摩擦学性能的影响:(1)通过Ag合金化的方式来调控其电子结构,进而优化薄膜的硬度、韧性和摩擦磨损行为;(2)插入软质延性金属Ag层以构建纳米多层膜,并探究延性层的尺度效应对其强韧化行为和摩擦学性能的影响;(3)引入高熔点的韧性金属Ta层以形成有序包裹的纳米复合结构,借助有序的包裹结构为改善薄膜的综合性能提供新的可能。(1)传统观念一直认为软质贵金属(Au、Ag、Cu等)会以纳米粒子的形式存在于TMC(N)的晶界中,而我们发现具有高价电子浓度(VEC)的贵金属Ag在含量较低时能够与TMN进行合金化并固溶进其晶格中。且引入微量固溶Ag原子便可以实现TMN薄膜综合性能的显著改善,主要包括:硬度、韧性、摩擦、磨损、疏水以及抑菌等性能。具体的实验方案为:通过共溅射的方法将微量的固溶Ag引入到NbN亚晶格中以获得Nb-Ag-N纳米固溶薄膜,并探究固溶Ag原子的含量对其强韧化行为和摩擦学性能的影响;研究发现微量固溶Ag原子(1.5 at.%)的引入不仅提高了薄膜的硬度、韧性和抗磨损能力,并且显著降低了CoF。通过理论计算进一步确认了固溶Ag原子导致的硬度增强主要来源于Ag 5s、4d和N p电子轨道之间的强杂化,而韧性的提高主要归因于Ag eg态的出现。除了观察到高硬度和高韧性可以显著降低磨损率外,还确认了CoF减小的主要原因是固溶Ag原子通过激活摩擦化学反应而促进形成了自润滑相?铌酸银(AgNbO3)。此外,固溶Ag原子可以有效地剪裁薄膜表面的化学键态,加速形成Ag2O疏水基团,使薄膜呈现出高疏水性。最后我们验证了该方案的普适性,结果表明受固溶Ag原子的诱导,Hf-Ag-N、Ta-Ag-N纳米固溶薄膜均获得了优异的强韧化行为及摩擦学性能。特别是,Hf-Ag-N薄膜中微量的固溶Ag原子(1.48 at.%)在油润滑下能够催化滑动界面处的基础油(PAO 10),使其原位自组装形成润滑的洋葱碳转移膜,从而显著改善基础油的润滑性能。更有趣的是,Ta-Ag-N薄膜中少量的固溶Ag原子(3.08at.%)对大肠杆菌有强烈的抑制作用,进而使薄膜呈现出优异的抑菌活性。(2)在TM-Ag-N固溶薄膜研究的基础上,通过插入软质延性金属Ag层来探究纳米Ag层的尺度效应对Ag/TMC纳米多层膜的强韧化行为和摩擦化学反应的影响。当延性金属Ag层较薄时,所形成的不连续纳米多层结构能够显著提高薄膜的硬度和韧性,并降低薄膜的CoF和磨损率;而当Ag层较厚时,连续Ag层的出现导致薄膜的硬度、韧性和抗磨损性能均出现大幅度地降低。因此,向TMC(N)中引入较薄的Ag层以构建不连续的纳米多层结构可能会成为一种有效策略来提高薄膜的强韧化行为并改善其摩擦学性能。具体的实验方案为:采取磁控溅射的方法制备具有不同Ag层厚度(lAg,2 nm14 nm)的Ag/TaC纳米多层膜,并进一步研究受lAg作用的薄膜生长、强韧化行为及摩擦化学反应。结果显示,当lAg=2 nm时,受固态去润湿作用而形成的不连续纳米多层结构可使薄膜实现超硬度、高韧性及优异的耐摩擦和抗磨损性能。其中,CoF的降低(0.227)主要归因于摩擦产物—润滑Ag纳米团簇和钽酸银(AgTaO3)的协同作用。然而,当lAg较厚时(lAg?7nm),易滑移连续Ag层的形成导致薄膜的硬度、韧性和抗磨损能力均发生明显降低。(3)除构建纳米多层结构外,形成由韧性金属层包裹的核-壳纳米结构也是实现TMC(N)基薄膜强韧化的有效方式。然而,目前仍然缺乏有效的制备途径来获得该有序结构,特别对于实现TMC(N)与“高熔点TM”之间(易混溶体系)的复合更是存在巨大的挑战。为此,我们提出一种新策略:在磁控溅射分层沉积过程中通过激活固态去润湿(solid-state dewetting)过程而制备出有序共格的核-壳结构TMC(N)@TM纳米复合薄膜,即较薄Ta-壳(lTa1.5 nm)在TaC-核的模板效应下共格生长成赝晶c-Ta。这个特殊的核-壳结构成功地诱导薄膜获得了优异的强韧化行为和摩擦学性能。显然,固态去润湿法是构建有序核-壳结构TMC(N)@TM的有效途径,也是优化TMC(N)基薄膜综合性能的新策略。具体的实验结论为:具有核-壳结构的TaC@Ta纳米复合薄膜(lTa1.5 nm)同时实现了硬度、韧性、耐摩擦、抗磨损以及耐腐蚀等综合性能的改善。经深入分析发现,硬度的增强主要受Orowan强化机制的作用,韧性的提高主要归因于压痕诱导的相转变,即Ta相从面心立方的c-Ta转变为体心立方的?-Ta。CoF的降低主要由于较薄的赝晶Ta层(?1.5 nm)能够诱导磨损表面自发氧化而形成润滑Magnéli相?TaOx。同时实现的高硬度和高韧性也明显改善了薄膜的抗磨损能力。此外,耐腐蚀性能的优化则是因为有序共格的核-壳结构可以有效地抑制柱状晶的生长,并阻碍腐蚀液的扩散。显然,通过以上三种策略可以实现对TMC(N)基薄膜综合性能的改善,这将为薄膜的强韧化设计及其摩擦磨损行为的深入探究提供新思路,使该薄膜体系在机械、生物、航空、航天及军工等尖端技术领域表现出巨大的应用潜力。
Abstract
guo du zu jin shu tan (dan )hua wu ji bao mo de jiang ren hua she ji ji ji ma ca xue xing neng yan jiu guo du zu jin shu tan (dan )hua wu (TMC(N))bao mo you yu ji gao ying du 、gao rong dian ji gao hua xue duo xing de te dian bei ren wei shi yi chong fei chang chong yao de biao mian fang hu yong cai liao ,ke yong yu fang zhi ge chong ling bu jian biao mian de hua ca 、mo sun he fu shi ,zai jing mi ji xie 、sheng wu zhi ru 、jiao tong yun shu 、dao ju 、hang kong gong ye he de zhi kan tan deng ling yu biao xian chu ju da de ying yong qian li 。sui zhao gong ye ji shu de fei su fa zhan ,fu za de shi yong huan jing dui bao mo cai liao de ying du di chu le geng gao de xu qiu ,tong guo jiang hua TMC(N)ji bao mo lai ta kuan ji ying yong ling yu yi cheng wei dang qian de yan jiu re dian 。ran er ,ying du yu ren xing tong chang ci xiao bi chang ,ying du de zeng jiang wang wang yi xi sheng ren xing wei dai jia 。xian ran ,dui yu TMC(N)bao mo lai shui ,zhui qiu geng gao de ying du bing gai shan ji ren xing reng ran shi yi ge chong yao de tiao zhan 。ci wai ,zai gai shan TMC(N)bao mo ying du he ren xing de tong shi ,di ma ca ji shu (CoF)he di mo sun lv dui di gao ji nai jiu xing he fu yi shou ming ye zhi guan chong yao 。yin ci ,zai she ji he shua qu jiang ren hua fang an shi ,jiang di CoFhe gai shan bao mo de kang mo sun xing neng ye bei shi wei chong yao de ping jia biao zhun 。ji yu yi shang fen xi ,wo men cai yong san chong bu tong de ce lve lai shi xian TMC(N)ji bao mo de jiang ren hua she ji bing guan cha ji dui ma ca xue xing neng de ying xiang :(1)tong guo Agge jin hua de fang shi lai diao kong ji dian zi jie gou ,jin er you hua bao mo de ying du 、ren xing he ma ca mo sun hang wei ;(2)cha ru ruan zhi yan xing jin shu Agceng yi gou jian na mi duo ceng mo ,bing tan jiu yan xing ceng de che du xiao ying dui ji jiang ren hua hang wei he ma ca xue xing neng de ying xiang ;(3)yin ru gao rong dian de ren xing jin shu Taceng yi xing cheng you xu bao guo de na mi fu ge jie gou ,jie zhu you xu de bao guo jie gou wei gai shan bao mo de zeng ge xing neng di gong xin de ke neng 。(1)chuan tong guan nian yi zhi ren wei ruan zhi gui jin shu (Au、Ag、Cudeng )hui yi na mi li zi de xing shi cun zai yu TMC(N)de jing jie zhong ,er wo men fa xian ju you gao jia dian zi nong du (VEC)de gui jin shu Agzai han liang jiao di shi neng gou yu TMNjin hang ge jin hua bing gu rong jin ji jing ge zhong 。ju yin ru wei liang gu rong Agyuan zi bian ke yi shi xian TMNbao mo zeng ge xing neng de xian zhe gai shan ,zhu yao bao gua :ying du 、ren xing 、ma ca 、mo sun 、shu shui yi ji yi jun deng xing neng 。ju ti de shi yan fang an wei :tong guo gong jian she de fang fa jiang wei liang de gu rong Agyin ru dao NbNya jing ge zhong yi huo de Nb-Ag-Nna mi gu rong bao mo ,bing tan jiu gu rong Agyuan zi de han liang dui ji jiang ren hua hang wei he ma ca xue xing neng de ying xiang ;yan jiu fa xian wei liang gu rong Agyuan zi (1.5 at.%)de yin ru bu jin di gao le bao mo de ying du 、ren xing he kang mo sun neng li ,bing ju xian zhe jiang di le CoF。tong guo li lun ji suan jin yi bu que ren le gu rong Agyuan zi dao zhi de ying du zeng jiang zhu yao lai yuan yu Ag 5s、4dhe N pdian zi gui dao zhi jian de jiang za hua ,er ren xing de di gao zhu yao gui yin yu Ag egtai de chu xian 。chu le guan cha dao gao ying du he gao ren xing ke yi xian zhe jiang di mo sun lv wai ,hai que ren le CoFjian xiao de zhu yao yuan yin shi gu rong Agyuan zi tong guo ji huo ma ca hua xue fan ying er cu jin xing cheng le zi run hua xiang ?ni suan yin (AgNbO3)。ci wai ,gu rong Agyuan zi ke yi you xiao de jian cai bao mo biao mian de hua xue jian tai ,jia su xing cheng Ag2Oshu shui ji tuan ,shi bao mo cheng xian chu gao shu shui xing 。zui hou wo men yan zheng le gai fang an de pu kuo xing ,jie guo biao ming shou gu rong Agyuan zi de you dao ,Hf-Ag-N、Ta-Ag-Nna mi gu rong bao mo jun huo de le you yi de jiang ren hua hang wei ji ma ca xue xing neng 。te bie shi ,Hf-Ag-Nbao mo zhong wei liang de gu rong Agyuan zi (1.48 at.%)zai you run hua xia neng gou cui hua hua dong jie mian chu de ji chu you (PAO 10),shi ji yuan wei zi zu zhuang xing cheng run hua de xiang cong tan zhuai yi mo ,cong er xian zhe gai shan ji chu you de run hua xing neng 。geng you qu de shi ,Ta-Ag-Nbao mo zhong shao liang de gu rong Agyuan zi (3.08at.%)dui da chang gan jun you jiang lie de yi zhi zuo yong ,jin er shi bao mo cheng xian chu you yi de yi jun huo xing 。(2)zai TM-Ag-Ngu rong bao mo yan jiu de ji chu shang ,tong guo cha ru ruan zhi yan xing jin shu Agceng lai tan jiu na mi Agceng de che du xiao ying dui Ag/TMCna mi duo ceng mo de jiang ren hua hang wei he ma ca hua xue fan ying de ying xiang 。dang yan xing jin shu Agceng jiao bao shi ,suo xing cheng de bu lian xu na mi duo ceng jie gou neng gou xian zhe di gao bao mo de ying du he ren xing ,bing jiang di bao mo de CoFhe mo sun lv ;er dang Agceng jiao hou shi ,lian xu Agceng de chu xian dao zhi bao mo de ying du 、ren xing he kang mo sun xing neng jun chu xian da fu du de jiang di 。yin ci ,xiang TMC(N)zhong yin ru jiao bao de Agceng yi gou jian bu lian xu de na mi duo ceng jie gou ke neng hui cheng wei yi chong you xiao ce lve lai di gao bao mo de jiang ren hua hang wei bing gai shan ji ma ca xue xing neng 。ju ti de shi yan fang an wei :cai qu ci kong jian she de fang fa zhi bei ju you bu tong Agceng hou du (lAg,2 nm14 nm)de Ag/TaCna mi duo ceng mo ,bing jin yi bu yan jiu shou lAgzuo yong de bao mo sheng chang 、jiang ren hua hang wei ji ma ca hua xue fan ying 。jie guo xian shi ,dang lAg=2 nmshi ,shou gu tai qu run shi zuo yong er xing cheng de bu lian xu na mi duo ceng jie gou ke shi bao mo shi xian chao ying du 、gao ren xing ji you yi de nai ma ca he kang mo sun xing neng 。ji zhong ,CoFde jiang di (0.227)zhu yao gui yin yu ma ca chan wu —run hua Agna mi tuan cu he tan suan yin (AgTaO3)de xie tong zuo yong 。ran er ,dang lAgjiao hou shi (lAg?7nm),yi hua yi lian xu Agceng de xing cheng dao zhi bao mo de ying du 、ren xing he kang mo sun neng li jun fa sheng ming xian jiang di 。(3)chu gou jian na mi duo ceng jie gou wai ,xing cheng you ren xing jin shu ceng bao guo de he -ke na mi jie gou ye shi shi xian TMC(N)ji bao mo jiang ren hua de you xiao fang shi 。ran er ,mu qian reng ran que fa you xiao de zhi bei tu jing lai huo de gai you xu jie gou ,te bie dui yu shi xian TMC(N)yu “gao rong dian TM”zhi jian (yi hun rong ti ji )de fu ge geng shi cun zai ju da de tiao zhan 。wei ci ,wo men di chu yi chong xin ce lve :zai ci kong jian she fen ceng chen ji guo cheng zhong tong guo ji huo gu tai qu run shi (solid-state dewetting)guo cheng er zhi bei chu you xu gong ge de he -ke jie gou TMC(N)@TMna mi fu ge bao mo ,ji jiao bao Ta-ke (lTa1.5 nm)zai TaC-he de mo ban xiao ying xia gong ge sheng chang cheng yan jing c-Ta。zhe ge te shu de he -ke jie gou cheng gong de you dao bao mo huo de le you yi de jiang ren hua hang wei he ma ca xue xing neng 。xian ran ,gu tai qu run shi fa shi gou jian you xu he -ke jie gou TMC(N)@TMde you xiao tu jing ,ye shi you hua TMC(N)ji bao mo zeng ge xing neng de xin ce lve 。ju ti de shi yan jie lun wei :ju you he -ke jie gou de TaC@Tana mi fu ge bao mo (lTa1.5 nm)tong shi shi xian le ying du 、ren xing 、nai ma ca 、kang mo sun yi ji nai fu shi deng zeng ge xing neng de gai shan 。jing shen ru fen xi fa xian ,ying du de zeng jiang zhu yao shou Orowanjiang hua ji zhi de zuo yong ,ren xing de di gao zhu yao gui yin yu ya hen you dao de xiang zhuai bian ,ji Taxiang cong mian xin li fang de c-Tazhuai bian wei ti xin li fang de ?-Ta。CoFde jiang di zhu yao you yu jiao bao de yan jing Taceng (?1.5 nm)neng gou you dao mo sun biao mian zi fa yang hua er xing cheng run hua Magnélixiang ?TaOx。tong shi shi xian de gao ying du he gao ren xing ye ming xian gai shan le bao mo de kang mo sun neng li 。ci wai ,nai fu shi xing neng de you hua ze shi yin wei you xu gong ge de he -ke jie gou ke yi you xiao de yi zhi zhu zhuang jing de sheng chang ,bing zu ai fu shi ye de kuo san 。xian ran ,tong guo yi shang san chong ce lve ke yi shi xian dui TMC(N)ji bao mo zeng ge xing neng de gai shan ,zhe jiang wei bao mo de jiang ren hua she ji ji ji ma ca mo sun hang wei de shen ru tan jiu di gong xin sai lu ,shi gai bao mo ti ji zai ji xie 、sheng wu 、hang kong 、hang tian ji jun gong deng jian duan ji shu ling yu biao xian chu ju da de ying yong qian li 。
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标签:过渡族金属碳氮化物薄膜论文; 纳米多层膜论文; 核壳纳米结构论文; 强韧化论文; 摩擦论文; 磨损论文; 吉林大学2019-06-25论文;