Email Alert  RSS
工艺探讨

植酸和唑类衍生物复合转化膜的制备及其机理研究

展开
  • 江南大学机械学院,江苏 无锡 214122
卞 达(1990-),副教授,博士,研究方向为表面工程,E-mail: biand@jiangnan.edu.cn

收稿日期: 2023-01-25

  修回日期: 2023-02-10

  录用日期: 2023-03-15

  网络出版日期: 2023-08-23

基金资助

国家自然科学基金(51675232);江苏省自然科学基金(BK20190611)资助

Preparation and Mechanism Study of Phytic Acid and Azole Derivatives Composite Conversion Film

Expand
  • School of Mechanical Engineering,Jiangnan University,Wuxi 214122,China

Received date: 2023-01-25

  Revised date: 2023-02-10

  Accepted date: 2023-03-15

  Online published: 2023-08-23

摘要

为改善植酸单独使用时难以在铜表面形成完整且致密转化膜的问题,采用浸渍法在铜表面制备含植酸(PA)和不同唑类衍生物的转化膜,利用接触角测试仪、电化学工作站、扫描电子显微镜(SEM)、能谱分析(EDS)表征了转化膜的疏水性、耐腐蚀性、表面形貌及成分,使用X 射线电子能谱仪(XPS)对耐蚀性能最佳的PA+BTA 转化膜的成膜机理进行分析。结果表明:加入不同唑类衍生物所形成的转化膜的耐腐蚀性提高,其中加入苯并三氮唑(BTA)和植酸的转化膜的接触角达到最大值(135.51°),腐蚀电流密度达到最小值(2.050×10-7 A/cm2),阻抗值超过90 kΩ;观察PA+BTA 转化膜的SEM 形貌发现,该转化膜在铜基底表面分布均匀且致密;对PA+BTA 转化膜进行XPS 谱分析,发现PA 和BTA 均参与了转化膜的形成,在铜基底表面生成了PA-Cu 和BTA-Cu 配合物,能有效保护铜基底。

本文引用格式

杨忠钰, 卞 达, 赵永武 . 植酸和唑类衍生物复合转化膜的制备及其机理研究[J]. 材料保护, 2023 , 56(7) : 119 -126 . DOI: 10.16577/j.issn.1001-1560.2023.0170

Abstract

To improve the problem of difficulty in forming a complete and dense conversion film on the copper surface when using phytic acid alone,the conversion films containing phytic acid (PA) and different azole derivatives were prepared on copper surface by impregnation method.The hydrophobicity,corrosion resistance and surface morphology of the conversion films were characterized by contact angle tester,electrochemical workstation,scanning electron microscope and energy dispersive spectroscopy (EDS).The film formation mechanism of PA+BTA conversion film with the best corrosion resistance was analyzed using X-ray electron spectroscopy (XPS).Results showed that the corrosion resistance of conversion films formed by adding different azole derivatives was improved.The contact angle of the conversion film with benzotriazole (BTA) and phytic acid reached maximum value (135.51 °),and the corrosion current density reached minimum value (2.050 × 10-7 A/cm2),while the impedance value exceeding 90 kΩ.By observing the SEM morphology of PA+BTA conversion film,it was found that the conversion film was evenly distributed and dense on the surface of copper substrate.XPS analysis of the PA+BTA conversion film showed that both PA and BTA were involved in the formation of the conversion film.PA-Cu and BTA-Cu complexes were formed on the surface of copper substrate,which could effectively protect the substrate.

参考文献

[1] 刘仁辉,刘斌斌,喻 玺,等.黄铜表面植酸钝化膜耐蚀性及其成膜机理[J].表面技术,2017,46(9):197-202.LIU R H,LIU B B,YU X,et al.Corrosion resistance and film formation mechanism of phytic acid passivation film on brass surface[J].Surface Technology,2017,46 (9):197-202.

[2] JHAN J J,WATAYA K,NISHIKAWA H,et al.Electrodeposition of nanocrystalline Cu for Cu-Cu direct bonding.Electrodeposition of nanocrystalline Cu for Cu - Cu direct bonding[J].Journal of the Taiwan Institute of Chemical Engineers,2022,132:104127.

[3] 卢 爽.铜表面自组装膜的制备及缓蚀性能研究[D].锦州:渤海大学,2021.LU S.Preparation and corrosion inhibition of self-assembled monolayers on copper surface [D].Jinzhou: Bohai University,2021.

[4] 印仁和,万宗跃,徐群杰,等.植酸自组装单分子膜对白铜B30 缓蚀作用的研究[J].功能材料,2007(4):562-564.YIN R H,WAN Z Y,XU Q J,et al.Study on the corrosion inhibition of phytic acid self-assembled monolayer on white copper B30 [J].Functional Materials,2007(4):562-564.

[5] 王 琳,祝群英,王健美.植酸铜配合物的合成与表征[J].吉林化工学院学报,2007(2):24-26.WANG L,ZHU Q Y,WANG J M.Synthesis and characterization of copper phytate complexes [J].Journal of Jilin Institute of Chemical Technology,2007 (2): 24-26.

[6] 贲建栋,鲁 钢,孙大东.植酸/硅烷复合钝化镀锌层的耐蚀性能[J].材料保护,2015,48(10): 13-15.BEN J D,LU G,SUN D D.Corrosion resistance of phytic acid/silane composite passivated zinc coating [J].Materials Protection,2015,48(10): 13-15.

[7] CUI X F,LI Y,LI Q F,et al.Influence of phytic acid concentration on performance of phytic acid conversion coatings on the AZ91D magnesium alloy [J].Materials Chemistry and Physics,2008,111: 503-507.

[8] POLING G W.Reflection infra-red studies of films formed by benzotriazole on Cu[J].Corrosion Science,1970,10(5): 359-370.

[9] ANDREA M,STEPHEN M.Effect of the pH in the growth of benzotriazole model layers at realistic environmental conditions[J].Corrosion Science,2018,143: 107-115.

[10] EL-SAYED M S,ERASMUS R M,COMINS J D.Effects of 3-amino-1,2,4-triazole on the inhibition of copper corrosion in acidic chloride solutions[J].Journal of Colloid and Interface Science,2007,311(1): 144-150.

[11] 王伟力,王桂清.植酸在金属缓蚀方面的应用[J].化工时刊,2012,26(3):47-50.WANG W L,WANG G Q.Application of phytic acid in metal corrosion inhibition [J].Chemical Engineering Journal,2012,26 (3): 47-50.

[12] LIU L,SU H Y,LI X,et al.Study on the preparation and corrosion inhibition of Schiff - base self - assembled membranes[J].Anti-Corrosion Methods & Materials,2019,66(2): 168-173.

[13] LIU L,LU S,WU Y Q,et al.Corrosion inhibition behavior of four benzimidazole derivatives and benzotriazole on copper surface[J].Anti-Corrosion Methods & Materials,2020,67(6): 565-574.

[14] 陈洪希.肌醇六磷酸脂在低温磷化液中的应用[J].四川化工与腐蚀控制,2000,3(4):7-11.CHEN H X.Application of inositol hexaphosphate in low temperature phosphating solution [J].Sichuan Chemical Industry and Corrosion Control,2000,3(4):7-11.

[15] 闫艳红.苯并三氮唑类化合物对典型金属合金的腐蚀抑制机制研究[D].沈阳:东北大学,2017.YAN Y H.Study on the corrosion inhibition mechanism of Benzotriazole Compounds on typical metal alloys [D].Shenyang: Northeast University,2017.

[16] YIN D,YANG L,TAN B M,et al.Theoretical and electrochemical analysis on inhibition effects of benzotriazole derivatives (un- and methyl) on copper surface[J].Journal of Molecular Structure,2021,1243: 130 871.

[17] SHEN S,DU J,GUO X Y,et al.Adsorption behavior of pH-dependent phytic acid micelles at the copper surface observed by Raman and electrochemistry[J].Applied Surface Science,2015,327(1): 116-121.

[18] WANG J Y,BIAN D,ZHAO Y W,et al.Effect of hybrid aluminum dihydrogen phosphate on the corrosion resistance of PTFE composite ceramic coatings[J].Materials and Corrosion,2021:1-11.

[19] BETHENCOURT M,BOTANA F J,CANO M J,et al.Using EIS to analyse samples of Al-Mg alloy AA5083 treated by thermal activation in cerium salt baths[J].Corrosion Science,2008,50(5): 1 376-1 384.

[20] LIU Y X,WANG Y G,BIAN D,et al.Impact of TiO nanoparticles and nanowires on corrosion protection performance of chemically bonded phosphate ceramic coatings[J].Ceramics International,2022,48(4): 5 091-5 099.

[21] KATYA B,MANUELE D,IRENE C,et al.Effect of HCl pre-treatment on corrosion resistance of cerium-based conversion coatings on magnesium and magnesium alloys[J].Corrosion Science,2005,47(4): 989-1 000.

[22] HUYNH N,BOTTLE S E,NOTOYA T,et al.Studies on alkyl esters of carboxybenzotriazole as inhibitors for copper corrosion[J].Corrosion Science,2002,44(6): 1 257-1 276.

[23] PAN F,YANG X,ZHANG D.Chemical nature of phytic acid conversion coatingon AZ61 magnesium alloy [J].Applied Surface Science,2009,255: 8 363-8 371.

[24] LI X H,DENG S D,HUI F.Synergistic inhibition effect of rare earth cerium(IV) ion and anionic surfactant on the corrosion of cold rolled steel in H2 SO4 solution[J].Corrosion Science,2008,50(9):2 635-2 645.

[25] 常钦鹏,陈友媛,安振东,等.B30 铜镍合金表面植酸转化膜的制备工艺研究[J].材料导报,2019,33(23):3 876-3 881.CHANG Q P,CHEN YY,AN Z D,et al.Study on the preparation process of phytic acid conversion film on B30 copper nickel alloy surface [J].Materials Reports,2019,33(23): 3 876-3 881.

[26] NANDINI S,RONALD N,ADIMULE S P,et al.Anticorrosive Effects of Derivatives of 4 - {[4 - (Dimethylamino)Benzylidene]amino}-1,2,4-Triazole on 316 Stainless Steel in HCl Medium: Experimental and Computational Study[J].Journal of Failure Analysis & Prevention,2021,21(3):1-20.

[27] HAO F,QING W,PEI Y L,et al.In-situ chemical conversion film for stabilizing zinc metal anodes[J].Journal of Energy Chemistry,2022,73(10):387-393.

[28] WANG X,MENG J P,LIN X G,et al.Stable Zinc Metal Anodes with Textured Crystal Faces and Functional Zinc Compound Coatings[J].Advanced Functional Materials,2021,31(48): 2106114.

[29] YIN D,YANG L,MA T D,et al.Synergistic effect of composite complex agent on BTA removal in post CMP cleaning of copper interconnection [J].Materials Chemistry and Physics,2020,252: 123230.

[30] LEBRINI M,Lagrenée M,TRAISNEL M,et al.Enhanced corrosion resistance of mild steel in normal sulfuric acid medium by 2,5-bis(n-thienyl)-1,3,4-thiadiazoles: Electrochemical,X-ray photoelectron spectroscopy and theoretical studies[J].Applied Surface Science,2007,253 (23):9 267-9 276.

[31] WENG L T,POLEUNIS C,BERTRAND P,et al.Sizing removal and functionalization of the carbon fiber surface studied by combined TOF SIMS and XPS[J].Journal of Adhesion Science & Technology,1995,9(7):859-871.

[32] OLIVARES O,LIKHANOVA N V,Gómez B,et al.Electrochemical and XPS studies of decylamides of α - amino acids adsorption on carbon steel in acidic environment[J].Applied Surface Science,2005,252(8): 2 894-2 909.

[33] ZARROK H,ZARROUK A,HAMMOUTI B,et al.Corrosion control of carbon steel in phosphoric acid by purpald -Weight loss,electrochemical and XPS studies[J].Corrosion Science,2012,64: 243-252.
文章导航

/