阳极氧化钽酸锂薄膜在NaOH溶液中的腐蚀行为研究
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摘要
通过阳极氧化法在高纯钽片表面制备了钽酸锂复合薄膜,采用浸泡失重法和电化学测试法考察了镀膜前后样品在10%(质量分数) NaOH溶液中的腐蚀行为。利用X射线衍射仪、扫描电子显微镜及能谱仪分别对薄膜的物相组成、表面及截面形貌、膜层厚度进行了测试分析。结果表明,阳极氧化后得到的复合薄膜由钽酸锂和氧化钽组成;该薄膜与基体之间结合良好,厚度约3μm;镀膜后样品的质量腐蚀速率至少减少了6倍,腐蚀电流密度下降了2个数量级,腐蚀96 h后样品表面没有明显变化。而对比的纯钽样品却发生了严重的腐蚀反应,生成了很多长条状和多棱柱状的腐蚀产物Na_3TaO_4、Na_2Ta_2O_6和Na_8Ta_6O_(19)。
Lithium tantalate(LiTaO_3) thin film was synthesized on high purity tantalum foil in molten LiNO_3 via anodic oxidation. Then corrosion behavior of the LiTaO_3 coated Ta foil was studied in 10%(mass fraction) NaOH solution by means of immersion corrosion test and electrochemical measurement. While the LiTaO_3 coated Ta foil before and after corrosion test was characterized with X-ray diffractometer(XRD), scanning electron microscopy(SEM) and energy dispersive spectrometer(EDS), respectively. Results showed that the anodic oxidation thin film consists of LiTaO_3 and tantalum oxides. The film was 3 μm in thickness and well bounded to the Ta matrix. The corrosion rate of the anodic oxidation thin film coated Ta foil was 1/6 that of the plain Ta foil, correspondingly, the corrosion current density of the former was two order magnitude lower than that of the later. Moreover, the morphology of the anodic oxidation thin film coated Ta foil remains unchanged even after 96 h immersion test. In contract, the plain Ta foil underwent severely corrosion with formation of rod-like and prism-like corrosion products of Na_3TaO_4, Na_2Ta_2O_6 and Na_8Ta_6O_(19).
Lithium tantalate(LiTaO_3) thin film was synthesized on high purity tantalum foil in molten LiNO_3 via anodic oxidation. Then corrosion behavior of the LiTaO_3 coated Ta foil was studied in 10%(mass fraction) NaOH solution by means of immersion corrosion test and electrochemical measurement. While the LiTaO_3 coated Ta foil before and after corrosion test was characterized with X-ray diffractometer(XRD), scanning electron microscopy(SEM) and energy dispersive spectrometer(EDS), respectively. Results showed that the anodic oxidation thin film consists of LiTaO_3 and tantalum oxides. The film was 3 μm in thickness and well bounded to the Ta matrix. The corrosion rate of the anodic oxidation thin film coated Ta foil was 1/6 that of the plain Ta foil, correspondingly, the corrosion current density of the former was two order magnitude lower than that of the later. Moreover, the morphology of the anodic oxidation thin film coated Ta foil remains unchanged even after 96 h immersion test. In contract, the plain Ta foil underwent severely corrosion with formation of rod-like and prism-like corrosion products of Na_3TaO_4, Na_2Ta_2O_6 and Na_8Ta_6O_(19).
引文
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[3]Hee A C,Zhao Y,Jamali S S,et al.Corrosion behaviour and microstructure of tantalum film on Ti6Al4V substrate by filtered cathodic vacuum arc deposition[J].Thin Solid Films,2017,636:54
[4]Wei D B,Chen X H,Zhang P Z,et al.Plasma surface tantalum alloying on titanium and its corrosion behavior in sulfuric acid and hydrochloric acid[J].Appl.Surf.Sci.,2018,441:448
[5]Yin W H,Tang H P.Downstream Processing Technology for Refractory Metals[M].Beijing:Chemical Industry Press,2015:30(殷为宏,汤慧萍.难熔金属材料深加工技术[M].北京:化学工业出版社,2015:30)
[6]Shi W,Wang Y.Handering treatment on tantalum surface[J].Heat Treat.Met.,2000,(5):27(石文,王煜.金属钽材表面强化处理[J].金属热处理,2000,(5):27)
[7]Zhang D Y,Xu L P,Luo W,et al.Corrosion behavior of tantalum and its nitride in alkali solution[J].Chin.J.Nonferrous Met.,2001,11(Suppl.2):277(张德元,许兰萍,罗文等.钽及表面离子渗氮层在碱液中的腐蚀行为[J].中国有色金属学报,2001,11(Suppl.2):277)
[8]Yao J Y,Wang Y C.The research of crystalline diamond films depositing on Ta spinneret[J].New Technol.New Proc.,2007,(2):74(姚锦元,王裕超.钽喷丝头表面覆加金刚石膜的研究[J].新技术新工艺,2007,(2):74)
[9]Liu Y Z.Process for providing lithium tantalum oxide coated tantalum articles with improved wear resistance[P].US,4678546,1987
[10]Zhang Y A,Xu H A,Guo T L.Fabrication and characterization of Ta2O5dielectric films by anodic oxidation[J].J.Funct.Mater.,2009,40:977(张永爱,许华安,郭太良.阳极氧化法制备Ta2O5绝缘膜及性能研究[J].功能材料,2009,40:977)
[11]Kolb E D,Laudise R A.The phase diagram,LiOH-Ta2O5-H2O and the hydrothermal synthesis of LiTaO3and LiNbO3[J].J.Cryst.Growth,1976,33:145
[12]Vogel U,Gemming T,Eckert J,et al.Analysis of the thermal and temporal stability of Ta and Ti thin films onto SAW-substrate materials(LiNbO3and LiTaO3)using AR-XPS[J].Surf.Interface Anal.,2016,48:570
[13]Yang X F,Zhang Z B,Sun H X,et al.Composition,surface morphology,optical properties and Ti profile characteristics of Ti-diffused LiTaO3strip waveguide[J].J.Alloy.Compd.,2017,695:2519
[14]Li Y H,Chen F,Gao G Y,et al.Ferroelectric,dielectric and leakage current properties of epitaxial(K,Na)NbO3-LiTaO3-CaZrO3thin films[J].J.Electroceram.,2015,34:249
[15]Gorelik V S,Sidorov N V,Vodchits A I.Optical properties of lithium niobate and lithium tantalate crystals with impurities and defects[J].Phys.Wave Phenom.,2017,25:10
[16]Wu Y S.Metallic Corrosion Research Method[M].Beijing:Metallurgical Industry Press,1993:48(吴荫顺.金属腐蚀研究方法[M].北京:冶金工业出版社,1993:48)
[17]Prabhu R A,Venkatesha T V,Shanbhag A V,et al.Inhibition effects of some Schiff's bases on the corrosion of mild steel in hydrochloric acid solution[J].Corros.Sci.,2008,50:3356
[18]Jak M J J,Konstapel C,Van Kreuningen A,et al.The influence of substrate defects on the growth rate of palladium nanoparticles on a TiO2(110)surface[J].Surf.Sci.,2001,474:28
[19]Robin A.Corrosion behaviour of tantalum in sodium hydroxide solutions[J].J.Appl.Electrochem.,2003,33:37
[20]Robin A.Corrosion behaviour of niobium in sodium hydroxide solutions[J].J.Appl.Electrochem.,2004,34:623