Clicking polyelectrolytes to form a crosslinked hydrogel [Elektronische Ressource] : their use for surface modification, electrospinning and preparation of nanoparticles / Miran Yu

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Informations

• Publié par: rheinisch-westfalischen_technischen_hochschule_-rwth-_aachen
• Publié le: 01 janvier 2011
• Nombre de lectures: 16
• Langue: English
• Poids de l'ouvrage: 14 Mo

Extrait

Clicking polyelectrolytes to form a crosslinked
hydrogel; their use for surface modification,
electrospinning and preparation of nanoparticles




Von der Fakultät für Mathematik, Informatik und Naturwissenschaften
der RWTH Aachen University zur Erlangung des akademischen Grades eines
Doktors der Naturwissenschaften genehmigte Dissertation

vorgelegt von

Master of Science
Miran Yu

aus Nonsan, Südkorea

Berichter: Universitätsprofessor Dr. rer. nat. Martin Möller
Universitätsprofessor Dr. rer. nat. Alexander Böker

Tag der mündlichen Prüfung: 18. Februar 2011

Diese Dissertation ist auf den Internetseiten der Hochschulbibliothek online verfügbar

















































시작과 끝을 함께 한










































사랑하는 나의 가족을 위해



TABLE OF CONTENTS
List of abbreviations vii
Summary ix
Zusammenfassung xi

Introduction CHAPTER 1 1
CHAPTER 2 Crosslinked self-assembled Poly(vinylamine) / Poly(amide 13
amine-epichlorohydrin) hydrogel films for silicon oxide
surface modification
CHAPTER 3 Azetidinium-amine coupling as “click” method for the 37
preparation of ultrathin hydrogel films on silicon oxide
CHAPTER 4 Ultrathin hydrogel coating to enhance shrinkproofing of 53
corona treated wool
CHAPTER 5 Aqueous electrospinning and stabilisation of PVAm 69
(polyvinylamine) based ultrathin nanofibers
CHAPTER 6 Polyelectrolyte crosslinked hydrogel nanofibers by 89
azetidinium-amine click reaction from aqueous gelating
solution
CHAPTER 7 Antimicrobial hydrogel nanofibers based on crosslinked 117
poly(vinylamine)
Synthesis of water swellable hybrid nanogels functionlized CHAPTER 8 137
by silver nanoparticles
CHAPTER 9 Antimicrobial surface modification onto fabrics using 163
polyamine nanogels functionalized by silver nanoparticles

Curriculum Vitae 185
List of publications 187
Acknowledgment 189
v




LIST OF ABBREVIATIONS
AAS atomic absorption spectroscopy
AFM atomforce microscopy
AOX absorbable organic chlorides
AgNO silver nitrate 3
B. sub Bacillus subtilis
Cryo cryogenics
CDOD methanol 4
DDS drug delivery system
D O deuterium oxide, heavy water 2
E. coli Escherichia coli
EDX energy disperive X-ray
FE SEM field emission scanning electron microscopy
FTIR fourier transform infrared
G ′ elastic moduli
G ″ viscous moduli
h hour(s)
HCl hydrogen chloride
HO water 2
IGAsorp isothermal gravimetric analyzer
LBL layer-by-layer
LD lethal dose 50
LDH lactate dehydrogenase
MEOH methanol
M weight average molecular weight w
NaBH sodium borohydride 4
NaC O H sodium citrate 6 7 5
NaOH hydroxide
NBF 4-chlor-7-nitrobenzofurazon
nm nanometer
NMR nuclear magnetic resonance
NVF N-vinylformamide
O oxygen 2
PAE poly(amideamine-epichlorohydrin)
vii

PECs polyelectrolyte complex
PEI poly(ethylene imine)
ppm part per million
PVAm poly(vinylamine)
R hydrodynamic radius h
SEM scanning electron microscopy
SFM force mi
TEM transmission electron microscope
Tg glass transition temperature
TGA thermogravimetric Analysis
TMS tetramethylsilane
®Triton X-100 octylphenoldecaethylenglycolether
UV ultraviolet
W/O water in oil
XPS X-ray photoelectron spectroscopy
°C degree Celsius
µm micrometer


















SUMMARY
This thesis presents the preparation and characterization of ultra-thin hydrogel films, ultra-
thin hydrogel nanofibers and silver nanoparticles functionalized nanogels based on
crosslinked polymers. The crosslinking was performed by “click” chemistry applying the
well-known azetidinium-amine coupling reaction. Hydrogel properties, such as water swelling
behavior, metal chelating ability, antimicrobial activity and cell toxicity, have been
investigated in detail.
This new type of hydrogel particles offers tunable material properties from macrostructure to
nanostructure. Furthermore, this approach offers the great opportunity to design functional
hybrid hydrogels by incorporation of inorganic nanoparticles, e.g. silver nanoparticles.
The polymer used in for the new approach is the commercially available poly(vinylamine)
(PVAm), which is a weak cationic polyelectrolyte bearing primary amine group among the
polymer backbone. PVAm is a useful material for coupling other molecules or chelating metal
ions due to the nucleophilic character of primary amines. Poly(amideamine-epichlorohydrin)
(PAE) is a reactive polymer resin and a weak cationic polyelectrolyte, which has a four-
membered 3-hydroxy-azetidinium ring among the polymer backbone.
The developed PVAm/PAE hydrogels could be successfully applied to a wide range of
applications ranging from surface modification of silicon oxide surface and wool fibers, to
electrospinning from aqueous gelating solution or to the fabrication of polymeric
nanoparticles as an antimicrobial coating on fabrics.
In summary, the developed PVAm/PAE hydrogels are a promising platform for various
applications. The systems can be easily modified to fulfill different tasks. The systems can be
easily adjusted to a specific application. To this respect, PVAm/PAE hydrogels will be
applied to surface coating of materials for further textile as well as biomedical applications.


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