Polyelectrolyte Multilayer Films Based on Natural Polymers: From Fundamentals to Bio-Applications
<p>(<b>a</b>) Sequential deposition of polycations (PCs) and polyanions (PAs) during the LbL assembly leading to the buildup of a multilayer film; different layer-by-layer (LbL) deposition techniques can be employed for the buildup of multilayer films: (<b>b</b>) dipping; (<b>c</b>) spray; (<b>d</b>) spin coating; (<b>e</b>) brushing.</p> "> Figure 2
<p>(<b>a</b>) Schematic representation of the electrostatic interaction between the protonated amine groups of chitosan and carboxylate groups of alginate; (<b>b</b>) Thickness of CHI/ALG films built up by dipping and a cross-sectional image via SEM (Adapted and reprinted with permission from [<a href="#B47-polymers-13-02254" class="html-bibr">47</a>]; Copyright 2013 American Chemical Society); (<b>c</b>) Evolution of the thickness of (ALG/CHI)<sub>n</sub> films with different ALG concentrations: 1 mg/mL (■) and 2.5 mg/mL (●) measured by SEM. The inset of the figure is a representative SEM micrograph of a film’s cross-section (Reprinted with permission from [<a href="#B48-polymers-13-02254" class="html-bibr">48</a>]; Copyright 2016 American Chemical Society); (<b>d</b>) Growth thickness of CHI/ALG films assembled by brushing with a comparison of dipping and brushing methods in the inset and in the topographic AFM images (adapted and reprinted with permission from [<a href="#B33-polymers-13-02254" class="html-bibr">33</a>]. Copyright 2018, Kyungtae Park et al. Springer Nature).</p> "> Figure 3
<p>(<b>a</b>) Thickness of (CMCHI/CHI)<sub>n</sub> built-up by spray using LMW chitosan (blue curve) or MMW chitosan (red curve) and AFM topographic images of multilayer films with 20 layer pairs (Adapted and reprinted with permission from [<a href="#B45-polymers-13-02254" class="html-bibr">45</a>]; Copyright 2012 Maria A. Witt et al.); (<b>b</b>) Thickness, measured by surface plasmon resonance (SPR) and ellipsometry, of CHI-based films assembled in the presence of different polyanions (i.e., HA, CHS, and HEP) (Reprinted with permission from [<a href="#B51-polymers-13-02254" class="html-bibr">51</a>]; Copyright 2011 American Chemical Society); (<b>c</b>) Thickness of CHI/CHS films built up by simultaneous spraying at a fixed salt concentration of 150 mM NaCl at different pHs: 2 (○), 4 (△), and pH 6 (□) (Adapted and reprinted with permission from [<a href="#B52-polymers-13-02254" class="html-bibr">52</a>]; Copyright 2012 American Chemical Society); (<b>d</b>) Film thickness after sequential deposition of CHI and HEP at different ionic strengths and pHs: 150 mM NaCl and pH 5.8 (●), 150 mM NaCl and pH 4.2 (■), 30 mM NaCl and pH 5.8 (○), and 30 mM NaCl and pH 4.2 (□) (Adapted and reprinted with permission from [<a href="#B42-polymers-13-02254" class="html-bibr">42</a>]; Copyright 2011 American Chemical Society); (<b>e</b>) Differences in the QCM frequency shifts at 15 MHz for CHI/HA multilayer films at pH 5 and different NaCl concentrations (0.15 M, 10<sup>−2</sup> M, and 10<sup>−4</sup> M NaCl) (Reprinted with permission from [<a href="#B25-polymers-13-02254" class="html-bibr">25</a>]. Copyright 2004 American Chemical Society).</p> "> Figure 4
<p>(<b>a</b>) Schematic representation of different cross-linking mechanisms in LbL films made of chitosan and alginate or hyaluronic acid; (<b>b</b>) DAPI-phalloidin fluorescence assay at 1 day of HUVECs cell culture in multilayers with different cross-linking degrees (top) and cell density as a function of cross-linking degree (bottom). (Adapted and reprinted with permission from [<a href="#B75-polymers-13-02254" class="html-bibr">75</a>]; Copyright 2017 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.); (<b>c</b>) AFM images of (CHI/CHS)<sub>10</sub> and (CHI/HA)<sub>10</sub> films (top) and phalloidin-stained bovine chondrocytes cultured on (CHI/CHS)<sub>10</sub> and (CHI/HA)<sub>10</sub> films (bottom) (Adapted and reprinted with permission from Ref [<a href="#B44-polymers-13-02254" class="html-bibr">44</a>]. Copyright 2011 American Chemical Society).</p> "> Figure 5
<p>(<b>a</b>) NIH/3T3 fibroblasts after 1 day of contact with controls or LbL multilayer films (left), and surface cell density after 1 and 7 days (right) (Adapted and reprinted with permission from [<a href="#B84-polymers-13-02254" class="html-bibr">84</a>]; Copyright 2016 Elsevier Inc. All rights reserved); (<b>b</b>) Adapted and reprinted with permission from [<a href="#B90-polymers-13-02254" class="html-bibr">90</a>] Copyright 2010 Wiley Periodicals, Inc.; (<b>c</b>) Schematic representation of the electrostatic interaction between chitosan and hyaluronic acid (left). Adhesive properties of freestanding membranes CHI/HA and CHI/HA-DN (center). Osteopontin immunofluorescence images of MC3T3-EI cells on those membranes, and images of the adhesiveness potential of those freestanding membranes on a clean surface of porcine bone: before (right-top) and after applying a detachment force with tweezers (right) (Adapted and reprinted with permission from [<a href="#B91-polymers-13-02254" class="html-bibr">91</a>]. Copyright 2017 MDPI).</p> "> Figure 6
<p>(<b>a</b>) Normalized <span class="html-italic">S. aureus</span> growth after 24 h contact with (PAR/HA)<sub>24</sub> multilayer films composed of PAR with a variable number of residues per chain (left) and confocal images (67 × 67 μm<sup>2</sup>) of <span class="html-italic">S. aureus</span> after 24 h of incubation on glass substrates, (PAR/HA)<sub>24</sub> films built with PAR10, PAR30, PAR100, or PAR200 and on a glass slide with antibiotics (right). The green channel corresponds to SYTO 24 labeling all bacteria and the red channel only healthy bacteria through metabolism of CTC (5-cyano-2,3-ditolyl tetrazolium chloride) into an insoluble, red fluorescent formazan. (Reprinted with permission from [<a href="#B101-polymers-13-02254" class="html-bibr">101</a>]; Copyright 2016 American Chemical Society); (<b>b</b>) Cumulative release profiles of TA from TA/COL films in contact with PBS pH 7.4 at room temperature (left), CFU of <span class="html-italic">S. aureus</span> from the supernatant of TA/COL films after 24 and 48 h of contact (N.D. means not detected, no CFUs were observed; dashed line means CFUs were obtained from the bacterial supernatant in contact with an uncoated glass) (center), and schematic representation of TA release-killing toward bacteria (right) (Adapted and reprinted with permission from [<a href="#B103-polymers-13-02254" class="html-bibr">103</a>]. Copyright 2020 American Chemical Society).</p> "> Figure 7
<p>(<b>a</b>) Post-operative view of the implanted PLGA tube maintained by suture wires (top), CµCT reconstructions (center) taken at 8 weeks after implantation at different doses of BMP-2 (scale bar = 5 mm) (center) and bone volume ratio at 8 weeks (bottom) (Adapted and reprinted with permission from [<a href="#B106-polymers-13-02254" class="html-bibr">106</a>]; Copyright 2016 Michael Bouyer et al., Published by Elsevier Ltd.); (<b>b</b>) Schematic representation of bioinstructive (CHI/ALG-RGD)<sub>6</sub> multilayers over liquefied ALG microchannels embedded in photocross-linkable glycidyl methacrylated xanthan gum (XG-GMA) hydrogels (top). Fluorescence microscopy image of a 3D ALG sacrificial microfiber coated with (RITC-CHI/ALG)<sub>6</sub> multilayer film (bottom-left), and live/dead confocal micrographs of HUVECs seeded for 3 days in the microchannels (bottom-right) (Reprinted with permission from [<a href="#B113-polymers-13-02254" class="html-bibr">113</a>]; Copyright 2021 by Cristiana F. V. Sousa et al. Licensee MDPI); (<b>c</b>) PET ligament, surgical schematic diagram of an anterior cruciate ligament (ACL) reconstruction model, and gross graft sample observation 3 months after operation in a porcine model (left). Immunohistochemical staining for collagen type I and relative expression of collagen type I (right) (Adapted and reprinted with permission from [<a href="#B114-polymers-13-02254" class="html-bibr">114</a>]. Copyright 2012 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved).</p> "> Figure 8
<p>(<b>a</b>) Diffusion of FITC-dextran (FD) of different molecular weights (4, 40, and 70 kDa) through a (CHI/ALG)<sub>100</sub> film (left) and CLSM images (right) (Reprinted with permission from [<a href="#B47-polymers-13-02254" class="html-bibr">47</a>]; Copyright 2013 American Chemical Society); (<b>b</b>) Schematic representation of drug delivery from multilayer films and cumulative release profiles of tamoxifen (TMX) from (ALG/CHI)<sub>5</sub>TMX(CHI/ALG)<sub>m</sub> (m = 5 (■), 10 (●), and 20 (▲)) films, where the inset shows the fitting to the Ritger-Peppas model, (left) and percentage of MCF-7 cell viability after tamoxifen (TMX) release from these films comparing with control films without TMX (right) (Adapted and reprinted with permission from [<a href="#B120-polymers-13-02254" class="html-bibr">120</a>]; Copyright 2018 Elsevier Ltd.); (<b>c</b>) Release profiles of bFGF reservoirs assembled with 3LP or 6LP and from co-solutions with bFGF at 0.1 or 1 µg/mL (left) and NIH/3T3 fibroblasts proliferation on FGF reservoirs with 6LP (right) (Adapted and reprinted with permission from [<a href="#B126-polymers-13-02254" class="html-bibr">126</a>]; Copyright 2015 Elsevier B.V.); (<b>d</b>) Kinetic of IL-4 release from PLL/HA and PLL/HA-Ald films in PBS (left) and phase contrast images (right) of monocytes seeded on the films after 6 days in presence of IL-4. Scale bar = 100 μm. (Adapted and reprinted with permission from [<a href="#B128-polymers-13-02254" class="html-bibr">128</a>]. Copyright 2016 American Chemical Society).</p> "> Figure 9
<p>(<b>a</b>) Maximum temperature increase dependence on nominal laser power for a thermofilm TNF10x with the inset showing the TNF-mediated thermalization of chicken breast tissue upon laser irradiation. Cell viability assay: calcein and EthD-1, signal before and after laser exposure (λ = 785 nm, 50 mW, 150 s) of TNF10x in contact with human neuroblastoma cells (Adapted and reprinted with permission from [<a href="#B131-polymers-13-02254" class="html-bibr">131</a>]; Copyright 2014 American Chemical Society); (<b>b</b>) Determination of Fe<sub>3</sub>O<sub>4</sub> content and temperature increase as a function of the number of NP layers deposited in the presence of an alternating magnetic field (AMF) (left). (ALG/CHI)<sub>40</sub>(NPs/CHI)<sub>160</sub> films subjected to 0 cycles of MHT (control), 1 cycle of MHT (30 min), and 3 cycles of MHT (30 min, 5 h waiting time between cycles). Note that cells are labeled with calcein (live cells in green) and EthD-1 (dead cells in red). Determination of % cell viability obtained from the images corresponding to live cells stained in green (Adapted and reprinted with permission from [<a href="#B132-polymers-13-02254" class="html-bibr">132</a>]. Copyright 2017 The Royal Society of Chemistry).</p> ">
Abstract
:1. Introduction
2. Growth Mechanisms in LbL Assembly of Natural Polymers
3. Experimental Factors Influencing the Growth in LbL Assembly of Natural Polymers
3.1. Molecular Weight
3.2. Nature of the Charged Groups of the Polyanion
3.3. pH, Ionic Strength, and Solvent
4. Engineering of LbL Films for Biomedical Applications
4.1. Cross-Linking Degree
4.2. Structure and Nature of the Ending Layer
5. Overview of the Performance of Natural LbL Films in Selected Biomedical Applications
5.1. Multilayer Films as Bioactive Functional Coatings
5.1.1. Blood-Compatible Coatings for Cardiovascular Implants
5.1.2. Biocompatible Coatings for Dental and Orthopedic Implants
5.1.3. Antimicrobial Coatings
5.2. Platforms for Tissue Regeneration
5.3. Matrixes for Drug Delivery
5.4. LbL Nanocomposite Films as Platforms for Thermal Therapies
6. Conclusions and Future Perspectives
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
Abbreviations
aCNFs | Cellulose nanofibrils |
aFGFs | Acidic fibroblast growth factors |
AFM | Atomic force microscopy |
ALG | Alginate |
AMF | Alternating magnetic field |
α-MSH | Alpha-melanocyte stimulating hormone |
APTT | Activated partial thromboplastin time |
Au-NPs | Gold nanoparticles |
bFGF | Basic bifroblast growth factor |
BM-MSCs | Bone marrow-derived stromal cells |
BMP-2 | Bone morphogenetic protein |
BMP-2 | Human bone morphogenetic protein 2 |
BSA | Bovine serum albumin |
C2C12 | Myoblast cells |
CAT | Catestatin |
CCL18 | C-C Motif Chemokine Ligand 18 |
CFU | Colony-forming unit |
CHI | Chitosan |
CHS | Chondroitin sulphate |
CLSM | Confocal laser scanning microscopy |
CMCHI | Carboxymethylchitosan |
COL | Collagen |
CTC | 5-cyano- 2,3-ditolyl tetrazolium chloride |
DCM | N,N-dimethyl chitosan |
Dex | Dextran sulfate |
DPSCs | Dental pulp stromal cells |
E. Coli | Escherichia coli |
ECM | Extracellular matrix |
EDC | 1-ethyl-3-(3-(dimethylamino)-propyl) carbodiimide |
EDTA | Ethylenediaminetetraacetic acid |
EthD-1 | Ethidium homodimer-1 |
FD | FITC-dextran |
FT-SPR | Surface plasmon resonance |
GIS | Grazing incidence spraying |
GL | Gelatin |
HA | Hyaluronic acid |
HA-CTL | Cateslytin functionalized hyaluronic acid |
HA-DN | Hyaluronic acid modified with dopamine |
hASCs | Human adipose stem cells |
HDF | Human dermal fibroblast |
HEP | Heparin |
HT29 | Human colonic adenocarcinoma cells |
HUVECs | Human umbilical vein endothelial cells |
IL | Interleukin |
IL1-RA | Interleukin-1 receptor antagonist |
IL-1β | Interleukin-1 beta |
IOP | Intraocular pressure |
LbL | Layer-by-layer |
LMW | Low molecular weight |
L-S | Sulfated levan |
Mb | Myoglobin |
MC3T3-E1 | Murine calvarial cells |
MCF-7 | Human breast cancer cells |
mCHI | Mesyl-chitosan |
MHT | Magnetic Hyperthermia Therapy |
MMW | Medium molecular weight |
MSCs | Bone marrow-derived ovine cells |
NHS | N-hydroxy-sulfosuccinimide |
NIH 3T3 | Mouse embryonic fibroblast cells |
NPs | Nanoparticles |
NSPCs | Neural stem/progenitor cells |
P. aeruginosa | Pseudomonas aeruginosa |
PA | Polyanion |
PAR | Polyarginine |
PBS | Phosphate buffer saline |
PC | Polycation |
PECs | Polyelectrolyte complexes |
PEI | Poly(ethylene imine) |
PGA | Poly(g-glutamic acid) |
PLL | Poly(L-lysine) |
PT | Prothrombin time |
PU | Polyurethane |
Px | Piroxicam |
RGD | Arginine–glycine–aspartic acid |
Rq | Surface roughness |
S. aureus | Staphylococcus aureus |
SEM | Scanning electron microscopy |
SH-SY5Y | Human neuroblastoma cancer cells |
TA | Tannic acid |
TCM | N,N,N-trimethyl chitosan |
TGFb1 | Transforming growth factor beta 1 |
TMFs | Thermomagnetic films |
TMX | Tamoxifen |
TNF | Thermonanofilms |
TNF-α | Tumor necrosis factor-α |
WJ-SCs | Wharton’s jelly |
XG-GMA | Glycidyl methacrylated xanthan gum |
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Polycation | Polyanion | Biomedical Applications | References |
---|---|---|---|
PLL | ALG | Wound healing Bioactive coatings tissue engineering | [16] [95] |
HA | Cell adhesive membranes Tissue engineering membranes Antitumor pads Drug delivery Reservoirs for growth factors | [61,69,70,71,72,73,74,78] [104,105,106,111] [70] [4,128,129] [78,108,128,129,130] | |
CHS | Cell adhesive membranes Reservoirs for growth factors | [78] [78] | |
PGA | Cell adhesive membranes Tissue engineering membranes Drug delivery Reservoirs for growth factors | [40,83] [108,109,110,112] [108,109,110] [108] | |
CHI | HA | Cell adhesive membranes Bioactive coatings tissue engineering Tissue engineering membranes Wound healing Antimicrobial coatings Antitumor pads Drug delivery | [54,75,81] [81,94] [86,91] [107] [40,99,100] [70] [86,125] |
ALG | Cell adhesive membranes Bioactive coatings tissue engineering Tissue engineering membranes Sensitive immunosensors Antimicrobial coatings Thermal patches Drug delivery Antitumor pads | [47,58,70,76,77,79,82] [81,94] [113,117] [127] [96] [131,132] [47,123,124] [120,122] | |
HEP | Anticoagulant coatings Anti-inflammatory coatings Wound healing Bioactive coatings tissue engineering Antimicrobial coatings Drug delivery Reservoirs for growth factors | [8,24,85] [8,84] [8] [92,93] [97,98] [126] [126] | |
Dex | Anticoagulant coatings | [24] | |
CHS | Cell adhesive membranes | [65] | |
COL | HA | Cell adhesive membranes Bioactive coatings tissue engineering | [43] [115] |
HEP | Cell adhesive membranes Anticoagulant coatings Bioactive coatings tissue engineering | [44] [87,88,89] [90] | |
CHS | Cell adhesive membranes Bioactive coatings tissue engineering | [44] [116] | |
ALG | Cell adhesive membranes | [9] | |
TA | Antimicrobial coatings | [103] | |
GL | HA | Bioactive coatings tissue engineering | [114] |
CHS | Tissue engineering membranes | [118] |
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Criado-Gonzalez, M.; Mijangos, C.; Hernández, R. Polyelectrolyte Multilayer Films Based on Natural Polymers: From Fundamentals to Bio-Applications. Polymers 2021, 13, 2254. https://doi.org/10.3390/polym13142254
Criado-Gonzalez M, Mijangos C, Hernández R. Polyelectrolyte Multilayer Films Based on Natural Polymers: From Fundamentals to Bio-Applications. Polymers. 2021; 13(14):2254. https://doi.org/10.3390/polym13142254
Chicago/Turabian StyleCriado-Gonzalez, Miryam, Carmen Mijangos, and Rebeca Hernández. 2021. "Polyelectrolyte Multilayer Films Based on Natural Polymers: From Fundamentals to Bio-Applications" Polymers 13, no. 14: 2254. https://doi.org/10.3390/polym13142254