Ionically Paired Layer-by-Layer Hydrogels: Water and Polyelectrolyte Uptake Controlled by Deposition Time

Selin, Victor; Ankner, John Francis; Sukhishvili, Svetlana

doi:10.3390/gels4010007

Title: Ionically Paired Layer-by-Layer Hydrogels: Water and Polyelectrolyte Uptake Controlled by Deposition Time

Journal Article · Thu Jan 11 00:00:00 EST 2018 · Gels

DOI:https://doi.org/10.3390/gels4010007· OSTI ID:1426564

Selin, Victor ^[1];

^[2]; Sukhishvili, Svetlana ^[1]

Texas A & M Univ., College Station, TX (United States). Dept. of Materials Science & Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)

Despite intense recent interest in weakly bound nonlinear (“exponential”) multilayers, the underlying structure-property relationships of these films are still poorly understood. This study explores the effect of time used for deposition of individual layers of nonlinearly growing layer-by-layer (LbL) films composed of poly(methacrylic acid) (PMAA) and quaternized poly-2-(dimethylamino)ethyl methacrylate (QPC) on film internal structure, swelling, and stability in salt solution, as well as the rate of penetration of invading polyelectrolyte chains. Thicknesses of dry and swollen films were measured by spectroscopic ellipsometry, film internal structure—by neutron reflectometry (NR), and degree of PMAA ionization—by Fourier-transform infrared spectroscopy (FTIR). The results suggest that longer deposition times resulted in thicker films with higher degrees of swelling (up to swelling ratio as high as 4 compared to dry film thickness) and stronger film intermixing. The stronger intermixed films were more swollen in water, exhibited lower stability in salt solutions, and supported a faster penetration rate of invading polyelectrolyte chains. These results can be useful in designing polyelectrolyte nanoassemblies for biomedical applications, such as drug delivery coatings for medical implants or tissue engineering matrices.

View Accepted Manuscript (DOE)

Cite

Export

Save

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1426564

Journal Information:: Gels, Vol. 4, Issue 1; ISSN 2310-2861

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

References (48)

Diffusion of Sites versus Polymers in Polyelectrolyte Complexes and Multilayers Fares, Hadi M.; Schlenoff, Joseph B. Journal of the American Chemical Society, Vol. 139, Issue 41 https://doi.org/10.1021/jacs.7b07905	journal	October 2017
Neutron reflectivity analysis of self-assembled film superlattices with alternate layers of deuterated and hydrogenated polysterenesulfonate and polyallylamine Korneev, D.; Lvov, Y.; Decher, G. Physica B: Condensed Matter, Vol. 213-214 https://doi.org/10.1016/0921-4526(95)00333-5	journal	August 1995
Modeling the Buildup of Polyelectrolyte Multilayer Films Having Exponential Growth ^✗ Lavalle, Philippe; Picart, Catherine; Mutterer, Jérome The Journal of Physical Chemistry B, Vol. 108, Issue 2 https://doi.org/10.1021/jp035740j	journal	January 2004
Nonlinear Layer-by-Layer Films: Effects of Chain Diffusivity on Film Structure and Swelling Selin, Victor; Ankner, John F.; Sukhishvili, Svetlana A. Macromolecules, Vol. 50, Issue 16 https://doi.org/10.1021/acs.macromol.7b01218	journal	August 2017
Steric Effects in Ionic Pairing and Polyelectrolyte Interdiffusion within Multilayered Films: A Neutron Reflectometry Study Xu, Li; Ankner, John F.; Sukhishvili, Svetlana A. Macromolecules, Vol. 44, Issue 16 https://doi.org/10.1021/ma200986d	journal	August 2011
Influence of the Polyelectrolyte Molecular Weight on Exponentially Growing Multilayer Films in the Linear Regime Porcel, C.; Lavalle, Ph.; Decher, G. Langmuir, Vol. 23, Issue 4 https://doi.org/10.1021/la062728k	journal	February 2007
Alginate-based hydrogels functionalised at the nanoscale using layer-by-layer assembly for potential cartilage repair Gentile, P.; Ghione, C.; Ferreira, A. M. Biomaterials Science, Vol. 5, Issue 9 https://doi.org/10.1039/C7BM00525C	journal	January 2017
Swelling and Smoothing of Polyelectrolyte Multilayers by Salt Dubas, Stephan T.; Schlenoff, Joseph B. Langmuir, Vol. 17, Issue 25 https://doi.org/10.1021/la0112099	journal	December 2001
Anisotropic Diffusion of Polyelectrolyte Chains within Multilayer Films Xu, Li; Kozlovskaya, Veronika; Kharlampieva, Eugenia ACS Macro Letters, Vol. 1, Issue 1 https://doi.org/10.1021/mz200075x	journal	November 2011
Deposition and properties of polyelectrolyte multilayers studied by ATR-FTIR spectroscopy Müller, M.; Briššová, M.; Rieser, T. Materials Science and Engineering: C, Vol. 8-9 https://doi.org/10.1016/S0928-4931(99)00033-8	journal	December 1999
Influence of the degree of ionization on the growth mechanism of poly(diallyldimethylammonium)/poly(acrylic acid) multilayers Bütergerds, Dörte; Kateloe, Christian; Cramer, Cornelia Journal of Polymer Science Part B: Polymer Physics, Vol. 55, Issue 5 https://doi.org/10.1002/polb.24283	journal	January 2017
Kinetics of Salt-Induced Annealing of a Polyelectrolyte Multilayer Film Morphology McAloney, Richard A.; Dudnik, Vyacheslav; Goh, M. Cynthia Langmuir, Vol. 19, Issue 9 https://doi.org/10.1021/la026882s	journal	April 2003
Layer-by-layer structured polysaccharides-based multilayers on cellulose acetate membrane: Towards better hemocompatibility, antibacterial and antioxidant activities Peng, Lincai; Li, Hui; Meng, Yahong Applied Surface Science, Vol. 401 https://doi.org/10.1016/j.apsusc.2016.12.235	journal	April 2017
Next generation, sequentially assembled ultrathin films: beyond electrostatics Quinn, John F.; Johnston, Angus P. R.; Such, Georgina K. Chemical Society Reviews, Vol. 36, Issue 5 https://doi.org/10.1039/b610778h	journal	January 2007
Polyelectrolytes I: Polyanion/Polycation Multilayers at the Air/Monolayer/Water Interface as Elements for Quantitative Polymer Adsorption Studies and Preparation of Hetero-superlattices on Solid Surfaces ^† Ruths, J.; Essler, F.; Decher, G. Langmuir, Vol. 16, Issue 23 https://doi.org/10.1021/la000257a	journal	November 2000
Study of the multilayer assembly and complex formation of poly(diallyldimethylammonium chloride) (PDADMAC) and poly(acrylic acid) (PAA) as a function of pH Alonso, T.; Irigoyen, J.; Iturri, J. J. Soft Matter, Vol. 9, Issue 6 https://doi.org/10.1039/C2SM26884A	journal	January 2013
Ionization and pH Stability of Multilayers Formed by Self-Assembly of Weak Polyelectrolytes Kharlampieva, Eugenia; Sukhishvili, Svetlana A. Langmuir, Vol. 19, Issue 4 https://doi.org/10.1021/la026546b	journal	February 2003
Influence of Polymer Molecular Weight on the Parabolic and Linear Growth Regime of PDADMAC/PSS Multilayers Nestler, Peter; Paßvogel, Malte; Helm, Christiane A. Macromolecules, Vol. 46, Issue 14 https://doi.org/10.1021/ma400333f	journal	July 2013
Polymer assemblies for controlled delivery of bioactive molecules from surfaces Pavlukhina, Svetlana; Sukhishvili, Svetlana Advanced Drug Delivery Reviews, Vol. 63, Issue 9 https://doi.org/10.1016/j.addr.2011.03.017	journal	August 2011
Comparison of the Structure of Polyelectrolyte Multilayer Films Exhibiting a Linear and an Exponential Growth Regime: An in Situ Atomic Force Microscopy Study Lavalle, Ph.; Gergely, C.; Cuisinier, F. J. G. Macromolecules, Vol. 35, Issue 11 https://doi.org/10.1021/ma0119833	journal	May 2002
Detailed Structure of Molecularly Thin Polyelectrolyte Multilayer Films on Solid Substrates as Revealed by Neutron Reflectometry Lösche, Mathias; Schmitt, Johannes; Decher, Gero Macromolecules, Vol. 31, Issue 25 https://doi.org/10.1021/ma980910p	journal	December 1998
Cooperative colloidal self-assembly of metal-protein superlattice wires Liljeström, Ville; Ora, Ari; Hassinen, Jukka Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/s41467-017-00697-z	journal	September 2017
Molecular Weight Dependence of Polymer Chain Mobility within Multilayer Films Xu, Li; Selin, Victor; Zhuk, Aliaksandr ACS Macro Letters, Vol. 2, Issue 10 https://doi.org/10.1021/mz400413v	journal	September 2013
Influence of the Degree of Ionization on Weak Polyelectrolyte Multilayer Assembly Choi, Jeeyoung; Rubner, Michael F. Macromolecules, Vol. 38, Issue 1 https://doi.org/10.1021/ma048596o	journal	January 2005
Acid−Base Equilibria of Weak Polyelectrolytes in Multilayer Thin Films Burke, Susan E.; Barrett, Christopher J. Langmuir, Vol. 19, Issue 8 https://doi.org/10.1021/la026500i	journal	April 2003
Advances in cellular and tissue engineering using layer-by-layer assembly Shukla, Anita; Almeida, Bethany Wiley Interdisciplinary Reviews: Nanomedicine and Nanobiotechnology, Vol. 6, Issue 5 https://doi.org/10.1002/wnan.1269	journal	April 2014
From Exponential to Linear Growth in Polyelectrolyte Multilayers Porcel, Claudine; Lavalle, Philippe; Ball, Vincent Langmuir, Vol. 22, Issue 9 https://doi.org/10.1021/la053218d	journal	April 2006
Factors Controlling the Growth of Polyelectrolyte Multilayers Dubas, Stephan T.; Schlenoff, Joseph B. Macromolecules, Vol. 32, Issue 24 https://doi.org/10.1021/ma981927a	journal	November 1999
Robust and Flexible Aramid Nanofiber/Graphene Layer-by-Layer Electrodes Kwon, Se Ra; Elinski, Meagan B.; Batteas, James D. ACS Applied Materials & Interfaces, Vol. 9, Issue 20 https://doi.org/10.1021/acsami.7b03449	journal	May 2017
Layer-by-layer self-assembled multilayers on PEEK implants improve osseointegration in an osteoporosis rabbit model Liu, Xilin; Han, Fei; Zhao, Peng Nanomedicine: Nanotechnology, Biology and Medicine, Vol. 13, Issue 4 https://doi.org/10.1016/j.nano.2017.01.011	journal	May 2017
Investigation of the Influence of Polyelectrolyte Charge Density on the Growth of Multilayer Thin Films Prepared by the Layer-by-Layer Technique Schoeler, Bjoern; Kumaraswamy, Guruswamy; Caruso, Frank Macromolecules, Vol. 35, Issue 3 https://doi.org/10.1021/ma011349p	journal	January 2002
Salt-induced changes in the growth of polyelectrolyte layers of poly(diallyl-dimethylammonium chloride) and poly(4-styrene sulfonate of sodium) Guzmán, Eduardo; Ritacco, Hernán; Rubio, José E. F. Soft Matter, Vol. 5, Issue 10 https://doi.org/10.1039/b901193e	journal	January 2009
Buildup Mechanism for Poly( l -lysine)/Hyaluronic Acid Films onto a Solid Surface Picart, C.; Lavalle, Ph.; Hubert, P. Langmuir, Vol. 17, Issue 23 https://doi.org/10.1021/la010848g	journal	November 2001
Dynamics of Layer-by-Layer Growth of a Polyelectrolyte Multilayer Studied in Situ Using Attenuated Total Reflectance Infrared Spectroscopy Owusu-Nkwantabisah, Silas; Gammana, Madhira; Tripp, Carl P. Langmuir, Vol. 30, Issue 39 https://doi.org/10.1021/la5031558	journal	September 2014
Hydrogen-Bonded Polymer Multilayers Probed by Neutron Reflectivity Kharlampieva, Eugenia; Kozlovskaya, Veronika; Ankner, John F. Langmuir, Vol. 24, Issue 20 https://doi.org/10.1021/la802502c	journal	October 2008
Layered, Erasable Polymer Multilayers Formed by Hydrogen-Bonded Sequential Self-Assembly Sukhishvili, Svetlana A.; Granick, Steve Macromolecules, Vol. 35, Issue 1 https://doi.org/10.1021/ma011346c	journal	January 2002
Linear versus Exponential Growth of Weak Polyelectrolyte Multilayers: Correlation with Polyelectrolyte Complexes Xu, Li; Pristinski, Denis; Zhuk, Aliaksandr Macromolecules, Vol. 45, Issue 9 https://doi.org/10.1021/ma300157p	journal	April 2012
Layer-by-Layer Hydrogen-Bonded Polymer Films: From Fundamentals to Applications Kharlampieva, Eugenia; Kozlovskaya, Veronika; Sukhishvili, Svetlana A. Advanced Materials, Vol. 21, Issue 30 https://doi.org/10.1002/adma.200803653	journal	August 2009
“In and Out Diffusion” Hypothesis of Exponential Multilayer Film Buildup Revisited Haynie, Donald T.; Cho, Eunhee; Waduge, Pradeep Langmuir, Vol. 27, Issue 9 https://doi.org/10.1021/la104516a	journal	May 2011
Thin Polymer Layers Formed by Polyelectrolyte Multilayer Techniques on Biological Surfaces Elbert, Donald L.; Herbert, Curtis B.; Hubbell, Jeffrey A. Langmuir, Vol. 15, Issue 16 https://doi.org/10.1021/la9815749	journal	August 1999
Polyelectrolyte Multilayers Containing a Weak Polyacid: Construction and Deconstruction Dubas, Stephan T.; Schlenoff, Joseph B. Macromolecules, Vol. 34, Issue 11 https://doi.org/10.1021/ma001720t	journal	May 2001
Molecular basis for the explanation of the exponential growth of polyelectrolyte multilayers Picart, C.; Mutterer, J.; Richert, L. Proceedings of the National Academy of Sciences, Vol. 99, Issue 20 https://doi.org/10.1073/pnas.202486099	journal	September 2002
Molecular Interactions Driving the Layer-by-Layer Assembly of Multilayers Borges, João; Mano, João F. Chemical Reviews, Vol. 114, Issue 18 https://doi.org/10.1021/cr400531v	journal	August 2014
Multilayer Nanoscale Encapsulation of Biofunctional Peptides to Enhance Bone Tissue Regeneration In Vivo Gentile, Piergiorgio; Ferreira, Ana Marina; Callaghan, Jill T. Advanced Healthcare Materials, Vol. 6, Issue 8 https://doi.org/10.1002/adhm.201601182	journal	February 2017
Chain Conformation and Dynamics in Spin-Assisted Weak Polyelectrolyte Multilayers Zhuk, Aliaksandr; Selin, Victor; Zhuk, Iryna Langmuir, Vol. 31, Issue 13 https://doi.org/10.1021/acs.langmuir.5b00401	journal	March 2015
Diffusional Response of Layer-by-Layer Assembled Polyelectrolyte Chains to Salt Annealing Selin, Victor; Ankner, John F.; Sukhishvili, Svetlana A. Macromolecules, Vol. 48, Issue 12 https://doi.org/10.1021/acs.macromol.5b00361	journal	June 2015
Next Generation, Sequentially Assembled Ultrathin Films: Beyond Electrostatics Quinn, John F.; Johnston, Angus P. R.; Such, Georgina K. ChemInform, Vol. 38, Issue 31 https://doi.org/10.1002/chin.200731267	journal	July 2007
An in-situ ATR-FTIR study on polyelectrolyte multilayer assemblies on solid surfaces and their susceptibility to fouling Müller, Martin; Rieser, Theresia; Lunkwitz, Klaus Macromolecular Rapid Communications, Vol. 19, Issue 7 https://doi.org/10.1002/marc.1998.030190701	journal	July 1998

Cited By (1)

Influence of poly‐ l ‐lysine molecular weight on antibacterial efficacy in polymer multilayer films Alkekhia, Dahlia; Shukla, Anita Journal of Biomedical Materials Research Part A, Vol. 107, Issue 6 https://doi.org/10.1002/jbm.a.36645	journal	February 2019

Similar Records

Nonlinear Layer-by-Layer Films: Effects of Chain Diffusivity on Film Structure and Swelling

Journal Article · Wed Aug 09 00:00:00 EDT 2017 · Macromolecules · OSTI ID:1426564

Selin, Victor; Ankner, John F.; Sukhishvili, Svetlana A.

Diffusional Response of Layer-by-Layer Assembled Polyelectrolyte Chains to Salt Annealing

Journal Article · Tue Jun 02 00:00:00 EDT 2015 · Macromolecules · OSTI ID:1426564

Selin, Victor; Ankner, John F.; Sukhishvili, Svetlana A.

Steric Effects in Ionic Pairing and Polyelectrolyte Interdiffusion within Multilayered Films: A Neutron Reflectometry Study

Journal Article · Sat Jan 01 00:00:00 EST 2011 · Macromolecules · OSTI ID:1426564

Xu, Li; Ankner, John Francis; Sukhishvili, Prof. Svetlana A.

Related Subjects

36 MATERIALS SCIENCE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
polyelectrolytes
layer-by-layer
multilayers
neutron reflectometry
exponential growth

Title: Ionically Paired Layer-by-Layer Hydrogels: Water and Polyelectrolyte Uptake Controlled by Deposition Time

Citation Formats

References (48)

Cited By (1)

Similar Records

Related Subjects