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The layer-by-layer (LbL) deposition technique is a versatile approach for preparing nanoscale multimaterial films: the fabrication of multicomposite films by the LbL procedure allows the combination of literally hundreds of different materials with nanometer thickness in a single device to obtain novel or superior performance. In the last 15 years the LbL technique has seen considerable developments and has now reached a point where it is beginning to find applications in bioengineering and biomedical engineering. The book gives a thorough overview of applications of the LbL technique in the context of bioengineering and biomedical engineering where the last years have witnessed tremendous progress. The first part familiarizes the reader with the specifics of cell-film interactions that need to be taken into account for successful application of the LbL method in biological environments. The second part focuses on LbL-derived small drug delivery systems and antibacterial agents, and the third part covers nano- and microcapsules as drug carriers and biosensors. The fourth and last part focuses on larger-scale biomedical applications of the LbL method such as engineered tissues and implant coatings.
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Cover
Related Titles
Title Page
Copyright
Foreword
Preface
About the Editors
List of Contributors
Part I: Control of Cell/Film Interactions
Chapter 1: Controlling Cell Adhesion Using pH-Modified Polyelectrolyte Multilayer Films
1.1 Introduction
1.2 Influence of pH-Modified PEM Films on Cell Adhesion and Growth
1.3 Summary and Outlook
Acknowledgments
References
Chapter 2: The Interplay of Surface and Bulk Properties of Polyelectrolyte Multilayers in Determining Cell Adhesion
2.1 Surface Properties
2.2 Bulk Modulus
References
Chapter 3: Photocrosslinked Polyelectrolyte Films of Controlled Stiffness to Direct Cell Behavior
3.1 Introduction
3.2 Elaboration of Homogeneous Films of Varying Rigidity
3.3 Elaboration of Rigidity Patterns
3.4 Behavior of Mammalian Cells on Homogeneous and Photopatterned Films
3.5 Influence of Film Rigidity on Bacterial Behavior
3.6 Conclusion
Acknowledgments
References
Chapter 4: Nanofilm Biomaterials: Dual Control of Mechanical and Bioactive Properties
4.1 Introduction
4.2 Surface Cross-Linking
4.3 NP Templating
4.4 Discussion
4.5 Conclusions
Acknowledgments
References
Chapter 5: Bioactive and Spatially Organized LbL Films
5.1 Introduction
5.2 Role of Chemical Properties
5.3 Role of Physical Properties
5.4 Spatially Organized PEMs
5.5 Conclusions and Future Perspectives
Acknowledgments
References
Chapter 6: Controlling Stem Cell Adhesion, Proliferation, and Differentiation with Layer-by-Layer Films
6.1 Introduction
6.2 Mesenchymal Stem Cells and Layer-by-Layer Films
6.3 Pluripotent Stem Cells and Layer-by-Layer Films
6.4 Future Directions and Trends
References
Part II: Delivery of Small Drugs, DNA and siRNA
Chapter 7: Engineering Layer-by-Layer Thin Films for Multiscale and Multidrug Delivery Applications
7.1 Introduction
7.2 Engineering LbL Release Mechanisms – from Fast to Slow Release
7.3 LbL Biologic Release for Directing Cell Behavior
7.4 Moving LbL Release Technologies to the Nanoscale: LbL Nanoparticles
7.5 Conclusions and Perspective on Future Directions
Acknowledgments
References
Chapter 8: Polyelectrolyte Multilayer Coatings for the Release and Transfer of Plasmid DNA
8.1 Introduction
8.2 Fabrication of Multilayers Using Plasmid DNA and Hydrolytically Degradable Polyamines
8.3 Toward Therapeutic Applications
In vivo
Contact-Mediated Approaches to Vascular Gene Delivery
8.4 Exerting Temporal Control over the Release of DNA
8.5 Concluding Remarks
Acknowledgments
References
Chapter 9: LbL-Based Gene Delivery: Challenges and Promises
9.1 LbL-DNA Delivery
9.2 LbL-siRNA Delivery
9.3 Concluding Remarks
References
Chapter 10: Subcompartmentalized Surface-Adhering Polymer Thin Films Toward Drug Delivery Applications
10.1 Introduction
10.2 Cyclodextrin (CD)-Containing LbL Films
10.3 Block Copolymer Micelle (BCM)-Containing LbL Films
10.4 Liposome-Containing LbL Films
10.5 LbL Films Containing Miscellaneous Drug Deposits
10.6 Conclusion/Outlook
References
Part III: Nano- and Microcapsules as Drug Carriers
Chapter 11: Multilayer Capsules for In vivo Biomedical Applications
11.1 Introduction
11.2 A Rationale for Functionally Engineered Multilayer Capsules
11.3
In vivo
Fate of Multilayer Capsules
11.4 Vaccine Delivery via Multilayer Capsules
11.5 Tumor Targeting via Multilayer Capsules
11.6 Concluding Remarks
References
Chapter 12: Light-Addressable Microcapsules
12.1 Introduction
12.2 Light-Responsive Components
12.3 Capsule Synthesis and Loading
12.4 Gold-Modified Layer-by-Layer Capsules
12.5 Morphological Changes of Capsules and Nanoparticles
12.6 Bubble Formation
12.7 Cytosolic Release
12.8 Triggering Cytosolic Reactions
12.9 Conclusions and Perspectives
Acknowledgments
References
Chapter 13: Nanoparticle Functionalized Surfaces
13.1 Introduction
13.2 Nanoparticles on Polyelectrolyte Multilayer LbL Capsules
13.3 Nanoparticles on Polyelectrolyte LbL Films
13.4 Conclusions
References
Chapter 14: Layer-by-Layer Microcapsules Based on Functional Polysaccharides
14.1 Introduction
14.2 Fabrication of Polysaccharide Capsules by the LbL Technique
14.3 Biomedical Applications
14.4 Interactions with Living Cells
14.5 Conclusion
References
Chapter 15: Nanoengineered Polymer Capsules: Moving into the Biological Realm
15.1 Introduction
15.2 Capsule Design and Assembly
15.3 Capsules at the Biological Interface
15.4 Biological Applications
15.5 Conclusion and Outlook
References
Chapter 16: Biocompatible and Biogenic Microcapsules
16.1 Introduction
16.2 LbL Assembly of Biocompatible and Biogenic Microcapsules
16.3 Applications
16.4 Conclusions and Perspectives
Acknowledgments
References
Chapter 17: Three-Dimensional Multilayered Devices for Biomedical Applications
17.1 Introduction
17.2 Freestanding Multilayer Films
17.3 Tubular Structures
17.4 Spherical Coated Shapes
17.5 Complex LbL Devices with Compartmentalization and Hierarchical Components
17.6 Porous Structures
17.7 Conclusions
Acknowledgments
References
Part IV: Engineered Tissues and Coatings of Implants
Chapter 18: Polyelectrolyte Multilayer Film – A Smart Polymer for Vascular Tissue Engineering
18.1 Layer by Layer Coating
18.2 Anti-Adhesive Properties of PEMs
18.3 Adhesion Properties of PEMs and Their Use in Vascular Tissue Engineering
18.4 Polyelectrolyte Multilayer Films and Stem Cell Behavior
18.5 PEM Coating of Vascular Prosthesis
18.6 Functional PEMs Mimicking Endothelial Cell Function
18.7 Conclusion
References
Chapter 19: Polyelectrolyte Multilayers as Robust Coating for Cardiovascular Biomaterials
19.1 Introduction
19.2 The Basement Membrane: The Bioinspired Cue for Cardiovascular Regeneration
19.3 PEMs as a Feasible Method for Immobilization: From Antithrombosis to theSynergistic Interaction
19.4 Controlled Delivery from PEMs: From Small Molecule Drugs and BioactiveMolecules to Genes
19.5 Effects of Mechanical Properties of PEMs on Cellular Events
19.6 PEM as a Coating for Cardiovascular Device: From
In vitro
to
In vivo
19.7 Conclusion and Perspectives
References
Chapter 20: LbL Nanofilms Through Biological Recognition for 3D Tissue Engineering
20.1 Introduction
20.2 A Bottom-Up Approach for 3D Tissue Construction
20.3 Conclusions
Acknowledgments
References
Chapter 21: Matrix-Bound Presentation of Bone Morphogenetic Protein 2 by Multilayer Films: Fundamental Studies and Applications to Orthopedics
21.1 Introduction
21.2 BMP-2 Loading: Physico-Chemistry and Secondary Structure
21.3 Osteoinductive Properties of Matrix-Bound BMP-2
In vitro
21.4 Early Cytoskeletal Effects of BMP-2
21.5 Toward
In vivo
Applications for Bone Repair
21.6 Toward Spatial Control of Differentiation
21.7 Conclusions
Acknowledgments
List of Abbreviations
References
Chapter 22: Polyelectrolyte Multilayers for Applications in Hepatic Tissue Engineering
22.1 Introduction
22.2 PEMs for 2D Hepatic Cell Cultures
22.3 PEMs for 3D Hepatic Cell Cultures
22.4 Conclusions
Acknowledgments
References
Chapter 23: Polyelectrolyte Multilayer Film for the Regulation of Stem Cells in Orthopedic Field
23.1 Introduction
23.2 Layer-by-Layer Assembly and Classification
23.3 Classic Polyelectrolyte Multilayer Films (Intermediate Layer)
23.4 Hybrid Polyelectrolyte Multilayer Film
23.5 “Protecting” Polyelectrolyte Multilayer Film (Cover Layer)
23.6 Conclusion and Perspective
References
Chapter 24: Axonal Regeneration and Myelination: Applicability of the Layer-by-Layer Technology
24.1 Current Challenges of Spinal Cord Injury: Inflammation, AxonalRegeneration, and Remyelination
24.2 PEM Film–Cell Interactions and Adhesion
24.3 Controlled Drug Delivery for Nerve Regeneration
24.4 Future Perspective
Acknowledgments
References
Index
End User License Agreement
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Cover
Table of Contents
Foreword
Preface
Part I: Control of Cell/Film Interactions
Chapter 1: Controlling Cell Adhesion Using pH-Modified Polyelectrolyte Multilayer Films
Figure 1.1
Figure 1.2
Figure 1.3
Figure 1.4
Figure 1.5
Figure 1.6
Figure 1.7
Figure 1.8
Figure 1.9
Figure 1.10
Figure 1.11
Figure 1.12
Figure 1.13
Figure 1.14
Figure 2.1
Figure 2.2
Figure 2.3
Figure 2.4
Figure 2.5
Figure 2.6
Figure 2.7
Figure 2.8
Figure 2.9
Figure 2.10
Figure 2.11
Scheme 3.1
Figure 3.1
Figure 3.2
Figure 3.3
Scheme 3.2
Figure 3.4
Figure 3.5
Figure 3.6
Figure 3.7
Figure 3.8
Figure 3.9
Figure 4.1
Figure 4.2
Figure 4.3
Figure 4.4
Figure 4.5
Figure 4.6
Figure 5.1
Figure 5.2
Figure 5.3
Figure 5.4
Figure 5.5
Figure 6.1
Figure 6.2
Figure 6.3
Figure 6.4
Figure 7.1
Figure 7.2
Figure 7.3
Figure 7.4
Figure 7.5
Figure 7.6
Figure 7.7
Figure 7.8
Figure 7.9
Figure 7.10
Figure 7.11
Figure 7.12
Figure 7.13
Figure 8.1
Figure 8.2
Figure 8.3
Figure 8.4
Figure 8.5
Figure 9.1
Figure 9.2
Figure 9.3
Scheme 10.1
Figure 10.1
Figure 10.2
Figure 10.3
Figure 10.4
Figure 10.5
Figure 11.1
Figure 11.2
Figure 11.3
Figure 11.4
Figure 11.5
Figure 11.6
Figure 11.7
Figure 11.8
Figure 11.9
Figure 11.10
Figure 11.11
Figure 12.1
Figure 12.2
Figure 12.3
Figure 12.4
Figure 12.5
Figure 12.6
Figure 12.7
Figure 12.8
Figure 12.9
Figure 12.10
Figure 12.11
Figure 12.12
Figure 13.1
Figure 13.2
Figure 13.3
Figure 13.4
Figure 13.5
Figure 13.6
Figure 13.7
Figure 13.8
Figure 14.1
Figure 14.2
Figure 14.3
Figure 14.4
Figure 14.5
Figure 15.1
Figure 15.2
Figure 15.3
Figure 15.4
Figure 15.5
Figure 15.6
Figure 15.7
Figure 15.8
Figure 15.9
Figure 15.10
Figure 15.11
Figure 15.12
Figure 15.13
Figure 15.14
Figure 15.15
Figure 16.1
Figure 16.2
Figure 16.3
Figure 16.4
Figure 16.5
Figure 16.6
Figure 17.1
Figure 17.2
Figure 17.3
Figure 17.4
Figure 17.5
Figure 19.1
Figure 19.2
Figure 19.3
Figure 19.4
Figure 19.5
Figure 19.6
Figure 19.7
Figure 19.8
Figure 20.1
Figure 20.2
Figure 20.3
Figure 20.4
Figure 20.5
Figure 20.6
Figure 20.7
Figure 20.8
Figure 20.9
Figure 20.10
Figure 20.11
Figure 21.1
Figure 21.2
Figure 21.3
Figure 21.4
Figure 21.5
Figure 21.6
Figure 21.7
Figure 21.8
Figure 21.9
Figure 21.10
Figure 22.1
Figure 22.2
Figure 22.3
Figure 22.4
Figure 22.5
Figure 22.6
Figure 23.1
Figure 23.2
Figure 23.3
Figure 23.4
Figure 23.5
Figure 23.6
Figure 24.1
Figure 24.2
Figure 24.3
Figure 24.4
Table 2.1
Table 2.2
Table 2.3
Table 4.1
Table 6.1
Table 9.1
Table 12.1
Table 14.1
Table 14.2
Table 15.1
Table 20.1
Table 21.1
Table 21.2
Table 24.1
Table 24.2
Decher, G., Schlenoff, J.B. (eds.)
Multilayer Thin Films
Sequential Assembly of Nanocomposite Materials
2nd Edition
2012
Print ISBN: 978-3-527-31648-9; also available in digital formats
Knoll, W., Advincula, R.C. (eds.)
Functional Polymer Films
2 Volume Set
2011
Print ISBN: 978-3-527-32190-2; also available in digital formats
Chujo, Y. (ed.)
Conjugated Polymer Synthesis
Methods and Reactions
2011
Print ISBN: 978-3-527-32267-1; also available in digital formats
Leclerc, M., Morin, J. (eds.)
Design and Synthesis of Conjugated Polymers
2010
Print ISBN: 978-3-527-32474-3; also available in digital formats
Ariga, K. (ed.)
Organized Organic Ultrathin Films
Fundamentals and Applications
2013
Print ISBN: 978-3-527-32733-1; also available in digital formats
Pacchioni, G., Valeri, S. (eds.)
Oxide Ultrathin Films
Science and Technology
2012
Print ISBN: 978-3-527-33016-4; also available in digital formats
Lyon, L.A., Serpe, M.J. (eds.)
Hydrogel Micro and Nanoparticles
2012
Print ISBN: 978-3-527-33033-1; also available in digital formats
Ruiz-Molina, D., Novio, F., Roscini, C. (eds.)
Bio- and Bioinspired Nanomaterials
2014
Print ISBN: 978-3-527-33581-7; also available in digital formats
Li, F., Nathan, A., Wu, Y., Ong, B.S.
Organic Thin Film Transistor Integration
A Hybrid Approach
2011
Print ISBN: 978-3-527-40959-4; also available in digital formats
Edited by Catherine Picart, Frank Caruso, and Jean-Claude Voegel
The Editors
Prof. Catherine Picart
University of Grenoble Alpes
Grenoble Institute of Technology
Department of Bioengineering
3 parvis Louis Néel
38016 Grenoble
France
Prof. Frank Caruso
The University of Melbourne
Chemical & Biomolecular Engineering
Victoria
3010 Parkville
Australia
Prof. Jean-Claude Voegel
The University de Strasbourg/INSERM
Biomaterials and Tissue Engineering
11 rue Humann
67085 Strasbourg
France
All books published by Wiley-VCH are carefully produced. Nevertheless, authors, editors, and publisher do not warrant the information contained in these books, including this book, to be free of errors. Readers are advised to keep in mind that statements, data, illustrations, procedural details or other items may inadvertently be inaccurate.
Library of Congress Card No.: applied for
British Library Cataloguing-in-Publication Data
A catalogue record for this book is available from the British Library.
Bibliographic information published by the Deutsche Nationalbibliothek
The Deutsche Nationalbibliothek lists this publication in the Deutsche Nationalbibliografie; detailed bibliographic data are available on the Internet at <http://dnb.d-nb.de>.
© 2015 Wiley-VCH Verlag GmbH & Co. KGaA, Boschstr. 12, 69469 Weinheim, Germany
All rights reserved (including those of translation into other languages). No part of this book may be reproduced in any form – by photoprinting, microfilm, or any other means – nor transmitted or translated into a machine language without written permission from the publishers. Registered names, trademarks, etc. used in this book, even when not specifically marked as such, are not to be considered unprotected by law.
Print ISBN: 978-3-527-33589-3
ePDF ISBN: 978-3-527-67589-0
ePub ISBN: 978-3-527-67588-3
Mobi ISBN: 978-3-527-67587-6
oBook ISBN: 978-3-527-67586-9
It is an honor and a great pleasure to address my colleagues in the fields of biomedicine and of nanocomposite coatings by introducing Layer-by-Layer (LbL) assembly as a tool for preparing some of next generation's smart biomaterials. In less than 25 years since its introduction by our team, LbL assembly has developed from an academic curiosity into a technology that is already beginning to change industry. It was very exciting for me to recently learn that several major industrial players, including for example 3M, are currently implementing LbL assembly as a platform technology. What if LbL assembly were today in a situation similar to the one physical and chemical vapor deposition techniques were in around the middle of the last century? Certainly, LbL assembly can be employed with even more classes of components than CVD or PVD, especially with respect to biological or bioactive materials.
With this book, LbL technology is now taking its next step into the field of biomedicine. According to the definition of the European Society for Biomaterials, “biomaterials are any substance, other than a drug, or combination of substances, synthetic or natural in origin, which can be used for any period of time, as a whole or as a part of a system which treats, augments, or replaces any tissue, organ, or function of the body.”
So why will LbL assembly be an exciting method for making new biomaterials or biomedical devices? Living matter, which biomaterials are supposed to help heal or to replace, is composed of thousands of different components whereas common composite materials are rarely composed of more than a handful of different constituents. If we accept that each component and its spatiotemporal arrangement contributes to the complex properties that need to be engineered into the materials for this field, then there is a huge interest to combine a large number of different components in future biomedical materials or devices. Given the very strength of LbL assembly, namely to control the co-assembly of hundreds of different components including proteins, DNA, RNA, or even living cells, it becomes evident why it has such a huge potential for developing even entirely new classes of biomaterials including, for example, multicompartment biomaterials or tissues. With the option to prepare multicomponent nano- or microparticles or capsules, to (bio-)functionalize or coat almost any surface including living cells, and to create reservoirs and barrier layers with tailored properties, with its potential for tissue engineering or for combining several of the above, there are tremendous opportunities for addressing the challenges of assembling those future biomaterials that we can only dream about today.
Gero Decher
Université de Strasbourg, France
The layer-by-layer field has been exponentially growing since its beginning in the early 1990s as judged by the number of publications, communications at international conferences, and groups from around the world who are now contributing to developments in the field. Thanks to the enthusiasm and energy of Gero Decher and Joe Schlenoff, a first book on Multilayer Thin Films: Sequential Assembly of Composite Materials was published in 2006. In view of the great success of this book, the second edition of the book was edited in 2011, with a revision and extension to two volumes. As described in the online version, this book is “a comprehensive summary of layer-by-layer assembled, truly hybrid nanomaterials and thin films, covering organic, inorganic, colloidal, macromolecular, and biological components, as well as the assembly of nanoscale films derived from them on surfaces.” Today, the layer-by-layer field has spread to a large number of subfields, from the fundamental understanding of film growth and properties to applications in specific areas such as energy, functional coatings, and liquid and gas filtration. The idea for a complementary book specifically focused on biomedical applications arose in 2010, after several important developments in films, capsules, and free-standing membranes in relation to bioactive molecules, drug delivery, and tissue engineering. Several successful reviews were published during this period, which highlighted the possibilities of layer-by-layer films for biomedical applications.
In March 2011, a layer-by-layer symposium organized by Gero Decher and colleagues was held in Strasbourg, France, where it was highlighted that the biological applications of layer-by-layer materials were rapidly growing. In June 2014, a new symposium organized by Svetlana Sukhisvili and Mike Rubner gathered the community in Hoboken near New York. This meeting again highlighted the important developments in the biomedical field.
In this book, our aim is to show the wide potential of multilayers in the biomedical field and also to promote the potential of the technology among biomedical students, teachers, and researchers. We believe that this book may become a textbook for biomedical students and attract new groups to work in the field and to develop the field further. Future advancements in this area are to develop multilayers that can be effectively translated into the clinic and ultimately used to treat patients.
We are pleased to have edited this book. We are honored that so many contributors from all over the world have accepted our invitation and took time to write significant contributions.
We look forward to future exciting and fruitful developments of layer-by-layer assembled materials in the biomedical fields. We also believe that layer-by-layer assembly will complement the range of model materials for fundamental studies on cellular processes and will provide new and well-defined systems to contribute to the development of new therapeutic and imaging systems.
Catherine Picart
Grenoble Institute of Technology, France
Frank Caruso
The University of Melbourne, Australia
Jean-Claude Voegel
University of Strasbourg/INSERM, France
Catherine Picartis full Professor of Bioengineering and Biomaterials at the Grenoble Institute of Technology, France, and former junior member of the Institut Universitaire de France (2006– 2011). She obtained her PhD in Biomedical Engineering from the University Joseph Fourier, Grenoble, and did post-doctoral research at the University of Pennsylvania, USA. Afterwards she joined the University Louis Pasteur, Strasbourg, as Assistant Professor and later the Department of Biology and Health at the University of Montpellier 2 as Associate Professor. Catherine Picart's research focuses on the assembly of biopolymers, protein/lipid interactions, and musculo-skeletal tissue engineering. She has authored more than 90 original articles and 6 reviews in international peer-reviewed journals. She received two ERC Grants from the European Research Council: a starting grant at the consolidator stage in 2010 and a Proof of Concept in 2012 to further develop osteoinductive layer-by-layer films for orthopedic and dental clinical applications. In 2013, she was nominated “Chevalier de l'ordre National du Merite” by the French Ministery of Research.
Frank Caruso is a Professor in the Department of Chemical and Biomolecular Engineering at the University of Melbourne, Australia. He was awarded an Australian Research Council Australian Laureate Fellowship in 2012 for recognition of his significant leadership and mentoring role in building Australia's internationally competitive research capacity. He has published over 350 peer-reviewed papers and is on ISI's most highly cited list, ranking in the top 20 worldwide in materials science in 2011. Frank Caruso is also included in Thomson Reuters' 2014 World's most influential scientific minds. He was elected a Fellow of the Australian Academy of Science in 2009. Prof. Caruso is also the recipient of the inaugural 2012 ACS Nano Lectureship Award (Asia/Pacific) from the American Chemical Society for global impact in nanoscience and nanotechnology, the 2013 Australian Museum CSIRO Eureka Prize for Scientific Leadership, and the 2014 Victoria Prize for Science and Innovation. His research interests focus on developing advanced nano- and biomaterials for biotechnology and medicine.
Jean-Claude Voegel was until end of 2012 head of the INSERM (French National Institute for Health and Medical Research) research unit “Biomaterials and Tissue Engineering” at the University of Strasbourg, France. His scientific activities were based on a research project going from fundamental developments to clinical applications, the preparation of materials and modification of biomaterial surfaces using functionalized architectures mainly prepared with the aid of polyelectrolyte multilayers obtained by the LbL technology. Jean-Claude Voegel published more than 130 papers in high-impact factor journals in the last decade around these projects and belongs to the top scientists in chemistry and materials science in terms of citations in this field.
List of Contributors
Jorge Almodovar
Centre National de la Recherche Scientifique, UMR 5628
3, Parvis Louis Néel
Grenoble
France
and
University of Grenoble Alpes
Grenoble Institute of Technology
Department of Bioengineering
3, Parvis Louis Néel
Grenoble
France
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