Skip to main content

Advertisement

SpringerLink
Log in

Fabrication of polyelectrolyte/amine-modified silica composite thin film by coupling of layer-by-layer assembly and sol–gel techniques

  • Original Paper
  • Published:
Journal of Polymer Research Aims and scope Submit manuscript

Abstract

This study focuses on a facile approach to create polyelectrolyte/SiO2 composite thin films. The film was fabricated by alternate deposition of N-[3-(trimethoxysilyl)propyl]diethylenetriamine (C10H27N3O3Si, TPDT in short) and poly(acrylic acid) (PAA). The layer-by-layer assembly process was accompanied by sol–gel transition of TPDT. The resultant films were investigated in detail by Fourier transform infrared spectroscopy (FT-IR), UV-Visible spectroscopy (UV–vis), ellipsometry, thermogravimetric analysis (TGA), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The results indicated that the films grew exponentially with increasing bilayer number. During deposition, hydrolysis and condensation of silanol groups in the film resulted in the formation of a Si-O-Si network embedded into the framework of the polymer. The obtained free-standing films had high transparency even with a high content of silica, and showed good mechanical properties with a tensile strength of 32.8 MPa at break.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  1. Decher G (1997) Fuzzy nanoassemblies: toward layered polymeric multicomposites. Science 277(5330):1232–1237

    Article  CAS  Google Scholar 

  2. Ariga K, Hill JP, Ji Q (2007) Layer-by-layer assembly as a versatile bottom-up nanofabrication technique for exploratory research and realistic application. PCCP 9(19):2319–2340

    Article  CAS  Google Scholar 

  3. Yang J, Cao S, Xin J, Chen X, Wu W, Li J (2013) Calcium carbonate deposition on layer-by-layer systems assembled from star polymers. J Polym Res 20(6):1–10

    Google Scholar 

  4. Ding C, Xu S, Wang J, Liu Y, Hu X, Chen P, Feng S (2012) Controlled loading and release of methylene blue from LbL polyurethane/poly (acrylic acid) film. Polym Adv Technol 23(9):1283–1286

    Article  CAS  Google Scholar 

  5. Mamedov AA, Kotov NA, Prato M, Guldi DM, Wicksted JP, Hirsch A (2002) Molecular design of strong single-wall carbon nanotube/polyelectrolyte multilayer composites. Nat Mater 1(3):190–194

    Article  CAS  Google Scholar 

  6. Wang Y, Angelatos AS, Caruso F (2007) Template synthesis of nanostructured materials via layer-by-layer assembly. Chem Mater 20(3):848–858

    Article  Google Scholar 

  7. Srivastava S, Kotov NA (2008) Composite layer-by-layer (LBL) assembly with inorganic nanoparticles and nanowires. Acc Chem Res 41(12):1831–1841

    Article  CAS  Google Scholar 

  8. Zhao Y, Xu Z, Wang X, Lin T (2012) Photoreactive azido-containing silica nanoparticle/polycation multilayers: durable superhydrophobic coating on cotton fabrics. Langmuir 28(15):6328–6335

    Article  CAS  Google Scholar 

  9. Laufer G, Carosio F, Martinez R, Camino G, Grunlan JC (2011) Growth and fire resistance of colloidal silica-polyelectrolyte thin film assemblies. J Colloid Interface Sci 356(1):69–77

    Article  CAS  Google Scholar 

  10. Wang J, Cheng Q, Tang Z (2012) Layered nanocomposites inspired by the structure and mechanical properties of nacre. Chem Soc Rev 41(3):1111–1129

    Article  Google Scholar 

  11. Yao H-B, Fang H-Y, Wang X-H, Yu S-H (2011) Hierarchical assembly of micro-/nano-building blocks: bio-inspired rigid structural functional materials. Chem Soc Rev 40(7):3764–3785

    Article  CAS  Google Scholar 

  12. Podsiadlo P, Michel M, Lee J, Verploegen E, Wong Shi Kam N, Ball V, Lee J, Qi Y, Hart AJ, Hammond PT (2008) Exponential growth of LBL films with incorporated inorganic sheets. Nano Lett 8(6):1762–1770

    Article  CAS  Google Scholar 

  13. Vendamme R, Ohzono T, Nakao A, Shimomura M, Kunitake T (2007) Synthesis and micromechanical properties of flexible, self-supporting polymer-SiO2 nanofilms. Langmuir 23(5):2792–2799

    Article  CAS  Google Scholar 

  14. Podsiadlo P, Kaushik AK, Arruda EM, Waas AM, Shim BS, Xu J, Nandivada H, Pumplin BG, Lahann J, Ramamoorthy A (2007) Ultrastrong and stiff layered polymer nanocomposites. Science 318(5847):80–83

    Article  CAS  Google Scholar 

  15. Podsiadlo P, Michel M, Critchley K, Srivastava S, Qin M, Lee JW, Verploegen E, Hart AJ, Qi Y, Kotov NA (2009) Diffusional self-organization in exponential layer-by-layer films with micro- and nanoscale periodicity. Angew Chem 121(38):7207–7211

    Article  Google Scholar 

  16. Lutkenhaus JL, Hrabak KD, McEnnis K, Hammond PT (2005) Elastomeric flexible free-standing hydrogen-bonded nanoscale assemblies. J Amer Chem Soc 127(49):17228–17234

    Article  CAS  Google Scholar 

  17. Podsiadlo P, Arruda EM, Kheng E, Waas AM, Lee J, Critchley K, Qin M, Chuang E, Kaushik AK, Kim H-S (2009) LBL assembled laminates with hierarchical organization from nano-to microscale: high-toughness nanomaterials and deformation imaging. Acs Nano 3(6):1564–1572

    Article  CAS  Google Scholar 

  18. Ding C, Xu S, Lin J, Hu X, Jian W, Wang J, Ma J, Feng S (2012) Controlled loading and release of methylene blue for hydrogen-bonded LbL poly (vinyl pyrrolidone)/poly (acrylic acid) film. J Polym Res 19(2):1–5

    Article  CAS  Google Scholar 

  19. Lavalle P, Gergely C, Cuisinier F, Decher G, Schaaf P, Voegel J, Picart C (2002) Comparison of the structure of polyelectrolyte multilayer films exhibiting a linear and an exponential growth regime: an in situ atomic force microscopy study. Macromolecules 35(11):4458–4465

    Article  CAS  Google Scholar 

  20. Richert L, Lavalle P, Payan E, Shu XZ, Prestwich GD, Stoltz J-F, Schaaf P, Voegel J-C, Picart C (2004) Layer by layer buildup of polysaccharide films: physical chemistry and cellular adhesion aspects. Langmuir 20(2):448–458

    Article  CAS  Google Scholar 

  21. Picart C, Mutterer J, Richert L, Luo Y, Prestwich G, Schaaf P, Voegel J-C, Lavalle P (2002) Molecular basis for the explanation of the exponential growth of polyelectrolyte multilayers. PNAS 99(20):12531–12535

    Article  CAS  Google Scholar 

  22. Gui Z, Qian J, An Q, Zhao Q, Jin H, Du B (2010) Layer-by-layer self-assembly, controllable disintegration of polycarboxybetaine multilayers and preparation of free-standing films at physiological conditions. J Mater Chem 20(8):1467–1474

    Article  CAS  Google Scholar 

  23. George A, Knez M, Hlawacek G, Dl H, Verputten HH, van Gastel R, ten Elshof JE (2012) Nanoscale patterning of organosilane molecular thin films from the gas phase and its applications: fabrication of multifunctional surfaces and large area molecular templates for site-selective material deposition. Langmuir 28(5):3045–3052

    Article  CAS  Google Scholar 

  24. Chan CC, Choudhury NR, Majewski P (2011) Fabrication and characterisation of self-assembled monolayers of N-[3-(trimethoxysilyl)propyl]diethylenetriamine on silica particles. Colloids Surf, A: Physicochem Eng Aspects 377(1):20–27

    Article  CAS  Google Scholar 

  25. Ulman A (1996) Formation and structure of self-assembled monolayers. Chem Rev 96(4):1533–1554

    Article  CAS  Google Scholar 

  26. Silberzan P, Leger L, Ausserre D, Benattar J (1991) Silanation of silica surfaces. A new method of constructing pure or mixed monolayers. Langmuir 7(8):1647–1651

    Article  CAS  Google Scholar 

  27. Demirel G, Çağlayan MO, Garipcan B, Duman M, Pişkin E (2007) Formation and organization of amino terminated self-assembled layers on Si (001) surface. Nanoscale Res Lett 2(7):350–354

    Article  CAS  Google Scholar 

  28. Liu D, Liu H, Hu N (2010) pH-controllable bioelectrocatalysis of glucose by glucose oxidase loaded in weak polyelectrolyte layer-by-layer films with ferrocene derivative as mediator. Electrochim Acta 55(22):6426–6432

    Article  CAS  Google Scholar 

  29. Sung MM, Kluth GJ, Yauw OW, Maboudian R (1997) Thermal behavior of alkyl monolayers on silicon surfaces. Langmuir 13(23):6164–6168

    Article  CAS  Google Scholar 

  30. Mauritz KA, Mountz D, Reuschle D, Blackwell R (2004) Self-assembled organic/inorganic hybrids as membrane materials. Electrochim Acta 50(2):565–569

    Article  CAS  Google Scholar 

Download references

Acknowledgements

This work was supported by the National Natural Science Foundation of China (51163015) and the Program for New Century Excellent Talents in University (NCET-11-1072).

Author information

Authors and Affiliations

  1. Key Laboratory of Oil and Gas Fine Chemicals, Ministry of Education and Xinjiang Uyghur Autonomous Region, College of Chemistry and Chemical Engineering, Xinjiang University, Urumqi, Xinjiang, 830046, People’s Republic of China

    Huanhuan Liu, Ronglan Wu, Juan Du, Xudong Nie, Shimei Xu & Jide Wang

Authors
  1. Huanhuan Liu
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Ronglan Wu
    View author publications

    You can also search for this author in PubMed Google Scholar

  3. Juan Du
    View author publications

    You can also search for this author in PubMed Google Scholar

  4. Xudong Nie
    View author publications

    You can also search for this author in PubMed Google Scholar

  5. Shimei Xu
    View author publications

    You can also search for this author in PubMed Google Scholar

  6. Jide Wang
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Shimei Xu.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Liu, H., Wu, R., Du, J. et al. Fabrication of polyelectrolyte/amine-modified silica composite thin film by coupling of layer-by-layer assembly and sol–gel techniques. J Polym Res 21, 328 (2014). https://doi.org/10.1007/s10965-013-0328-9

Download citation

  • Received:

  • Accepted:

  • Published:

  • DOI: https://doi.org/10.1007/s10965-013-0328-9

Keywords

Search

Navigation