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Engineering and Functionalization of Hemicellulose Hydrogels
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology, Polymer Technology. College of Polymer Science & Engineering, Sichuan University.ORCID iD: 0000-0003-2689-0251
2015 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Hemicellulose is the second most abundant component in wood and is an important renewable resource  that is used in films, paper composites and biofuels.  Hemicelluloses  have  several  advantages,  including  their abundance,  degradability  and  renewability.  O-acetyl-galactoglucomannan (AcGGM) is a type of hemicellulose that is predominantly found in softwood specimens. In the recent drive to engineer functional hydrogels with stimuli-responsive  properties,  functional  AcGGM-derived  hydrogels  are  highly interesting alternatives. In  the  first  part  of  this  thesis,  a  combination  of  the  electro-activity  of conducting oligomers and AcGGM was used to design a robust pathway to generate  electrically  conductive  hemicellulose  hydrogels  (ECHHs)  using AcGGM  and  a  conductive  aniline  tetramer.  Subsequently,  in  order  to fabricate  ECHHs  using  a  greener  and  more  facile  approach,  a  one-pot reaction  was  performed  in  which  AcGGM  was  cross-linked  with epichlorohydrin in the presence of a conductive aniline pentamer in water at ambient  temperature.  To  impart  other  functionalities  to  the  hemicellulose hydrogels,  magnetic  field-responsive  hemicellulose  hydrogels  (MFRHHs) were  fabricated  by  simultaneous  in  situ  formation  of  magnetic  Fe 3 O 4   and cross-linking of AcGGM. These MFRHHs exhibited  a controlled release of the  protein  bovine  serum  albumin.  Finally,  a  facile,  fast  and  functional chemical  methodology  to  prepare  stimuli-responsive  hemicellulose  micro-gels was developed that offers the potential for fabricating hydrogels using a green  processing  technique.  The  micro-gels  were  shown  to  have  a  rapid response to electrochemical stimuli, pH alterations and a magnetic field, as well  as  good  blood  compatibility,  which  is  required  for  biomedical applications.  All  these  stimuli-responsive  hemicellulose  hydrogels  demonstrated controllable  aqueous  swelling  behavior  and  combine  the  renewability  of hemicellulose  and  stimuli-responsiveness  of  functional  molecules,  thereby opening new potential routes to fabricate biomaterials with a wide range of applications  (e.g.,  biosensors,  nerve  system  repair,  and  controlled  drug release).

Abstract [sv]

Hemicellulosa är den näst mest förekommande komponenten i ved och är en  viktig  förnybar  resurs  som  kan  användas  för  filmer,  papperstillverkning och biobränslen. Hemicellulosorna har flera fördelar, inklusive riklig tillgång, nedbrytbarhet  och  förnybarhet.  O-acetyl-galaktoglukomannan  (AcGGM)  är en typ av hemicellulosa som är dominerande i barrved. Ett stort intresse har nyligen  utvecklats  för  att  skapa  funktionella  hydrogeler  med  t.ex. stimulikänsliga  egenskaper,  vilket  har  gjort  funktionella  AcGGM-baserade hydrogeler till mycket intressanta materialalternativ. I den första delen av detta arbete kombineras elektroaktiviteten hos ledande oligomerer  med  AcGGM.  En  robust  syntesväg  till  elektriskt  ledande hemicellulosabaserade  hydrogeler  (ECHHs)  har  utvecklats  med  AcGGM och en ledande anilin tetramer som komponenter. För att tillverka ECHHs med en grönare syntes utvecklades därefter en enklare metod där AcGGM tvärbinds  med  epiklorhydrin  i  en  enstegsreaktion  i  närvaro  av  en  ledande anilinpentamer med vatten som lösningsmedel vid rumstemperatur. För att tillföra  andra  funktioner  till  de  hemicellulosabaserade  hydrogelerna  har magnetiska hemicellulosabaserade hydrogeler (MFRHHs) tillverkats genom att, in situ bilda magnetisk Fe 3 O 4  och samtidigt tvärbinda AcGGM. MFRHHs uppvisade även kontrollerad frisättning av proteinet bovint serumalbumin.  I den sista delen av avhandlingen, användes en enkel, snabb och funktionell metod för att tillverka stimuli-responsiva hemicellulosabaserade mikrogeler. Dessa geler är mycket intressanta då de både är responsiva och tillverkas med  en  miljövänlig  bearbetningsteknik.  Mikrogelerna  visade  sig  reagera snabbt  på  externa  stimuli:  pH-förändringar  elektriska  och  magnetiska  fält. De  hade  också  en  god  blodkompatibilitet,  vilket  krävs  för  biomedicinska tillämpningar. Alla dessa stimuli-responsiva hemicellulosabaserade hydrogeler visade sig ha  ett  kontrollerbart  svällningsbeteende  i  vatten.  Denna  egenskap, tillsammans med deras förnybarhet och förmåga att svara på externa stimuli öppnar  upp  nya  möjligheter  till  att  tillverka,  till  exempel,  biomaterial  för biosensorer, nervsystem och kontrollerad läkemedelsfrisättning.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2015. , 75 p.
Series
TRITA-CHE-Report, ISSN 1654-1081 ; 2015:61
Keyword [en]
Hemicellulose, O-acetyl-galactoglucomannan, hydrogels, stimuli-responsive, aniline tetramer, aniline pentamer, electro-active, conductivity, pH-sensitivity, magnetic field-responsive, micro-gels, swelling, drug delivery.
National Category
Engineering and Technology Natural Sciences
Research subject
Fibre and Polymer Science
Identifiers
URN: urn:nbn:se:kth:diva-176302ISBN: 978-91-7595-741-8 (print)OAI: oai:DiVA.org:kth-176302DiVA: diva2:866558
Public defence
2015-11-25, Kollgiesalen, Brinellvägen 8, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Funder
EU, European Research Council, Paradigm 246776
Note

QC 20151103

Available from: 2015-11-03 Created: 2015-11-03 Last updated: 2015-11-03Bibliographically approved
List of papers
1. A robust pathway to electrically conductive hemicellulose hydrogels with high and controllable swelling behavior
Open this publication in new window or tab >>A robust pathway to electrically conductive hemicellulose hydrogels with high and controllable swelling behavior
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2014 (English)In: Polymer, ISSN 0032-3861, E-ISSN 1873-2291, Vol. 55, no 13, 2967-2976 p.Article in journal (Refereed) Published
Abstract [en]

A robust pathway to synthesize electrically conductive hemicellulose hydrogels (ECHHs) based on O-acetylgalactoglucomannan (AcGGM) and conductive aniline tetramer (AT) is presented. These ECHHs were obtained by functionalizing carboxylated AcGGM with glycidyl methacrylate (GMA) and subsequently covalently immobilizing AT onto GMA. Hydrogel swelling ratios (SRs) were regulated by the degree of substitution (DS) of the carboxylated AcGGM, the maximum varied as follows: SRDS=1.14 < SRDS=0.60 < SRDS=0.24. The SR can also be tuned from 548% to 228% by changing the AT contents from 10% (w/w) to 40% (w/w) while simultaneously altering conductivities from 2.93 x 10(-8) to 1.12 x 10(-6) S/cm. Free-standing ECHHs with tunable conductivity and degree of swelling, as presented herein, have a broad potential for biomedical applications.

Keyword
Hydrogels, Hemicellulose, Electrically conductive
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-146864 (URN)10.1016/j.polymer.2014.05.003 (DOI)000337549000005 ()2-s2.0-84902104788 (Scopus ID)
Funder
EU, European Research Council, 246776
Note

QC 20140617

Available from: 2014-06-17 Created: 2014-06-17 Last updated: 2017-12-05Bibliographically approved
2. Facile and Green Approach towards Electrically Conductive Hemicellulose Hydrogels with Tunable Conductivity and Swelling Behavior
Open this publication in new window or tab >>Facile and Green Approach towards Electrically Conductive Hemicellulose Hydrogels with Tunable Conductivity and Swelling Behavior
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2014 (English)In: Chemistry of Materials, ISSN 0897-4756, E-ISSN 1520-5002, Vol. 26, no 14, 4265-4273 p.Article in journal (Refereed) Published
Abstract [en]

A one-pot reaction to synthesize electrically conductive hemicellulose hydrogels (ECHHs) is developed via a facile and green approach in water and at ambient temperature. ECHHs were achieved by cross-linking O-acetyl-galactoglucomannan (AcGGM) with epichlorohydrin in the presence of conductive aniline pentamer (AP) and were confirmed by infrared spectroscopy (IR) and elemental analysis. All hydrogels had macro-porous structures, and the thermal stability of ECHHs was improved by the addition of AP. Hydrogel equilibrium swelling ratios (ESRs) varied from 13.7 to 11.4 and were regulated by cross-linker concentration. The ESRs can also be tuned from 9.6 to 6.0 by changing the AP content level from 10 to 40% (w/w) while simultaneously altering conductivity from 9.05 x 10(-9) to 1.58 X 10(-6) S/cm. ECHHs with controllable conductivity, tunable swelling behavior, and acceptable mechanical properties have great potential for biomedical applications, such as biosensors, electronic devices, and tissue engineering.

Keyword
Biomedical Applications, Polysaccharide Hydrogels, In-Vitro, Thermoresponsive Hydrogels, Thermosensitive Hydrogels, Composite Hydrogels, Aniline Pentamer, Cross-Linking, Polymer, Epichlorohydrin
National Category
Polymer Chemistry
Identifiers
urn:nbn:se:kth:diva-146867 (URN)10.1021/cm501852w (DOI)000339471400030 ()2-s2.0-84904670901 (Scopus ID)
Funder
EU, European Research Council
Note

QC 20140822. Updated from manuscript to article in journal.

Available from: 2014-06-17 Created: 2014-06-17 Last updated: 2017-12-05Bibliographically approved
3. In Situ Synthesis of Magnetic Field-Responsive Hemicellulose Hydrogels for Drug Delivery
Open this publication in new window or tab >>In Situ Synthesis of Magnetic Field-Responsive Hemicellulose Hydrogels for Drug Delivery
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2015 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 16, no 8, 2522-2528 p.Article in journal (Refereed) Published
Abstract [en]

A one-pot synthetic methodology for fabricating stimuli-responsive hemicellulose-based hydrogels was developed that consists of the in situ formation of magnetic iron oxide (Fe3O4) nanoparticles during the covalent cross-linking of O-acetyl-galactoglucomannan (AcGGM). The Fe3O4 nanoparticle content controlled the thermal stability, macrostructure, swelling behavior, and magnetization of the hybrid hydrogels. In addition, the magnetic field-responsive hemicellulose hydrogels (MERHHs) exhibited excellent adsorption and controlled release profiles with bovine serum albumin (BSA) as the model drug. Therefore, the MFRHHs have great potential to be utilized in the biomedical field for tissue engineering applications, controlled drug delivery, and magnetically assisted bioseparation. Magnetic field-responsive hemicellulose hydrogels, prepared using a straightforward one-step process, expand the applications of biomass-derived polysaccharides by combining the renewability of hemicellulose and the magnetism of Fe3O4 nanoparticles.

National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-173274 (URN)10.1021/acs.biomac.5b00801 (DOI)000359499500030 ()26196600 (PubMedID)2-s2.0-84938940552 (Scopus ID)
Note

QC 20150911

Available from: 2015-09-11 Created: 2015-09-09 Last updated: 2017-12-04Bibliographically approved
4. In Situ Cross-Linking of Stimuli-Responsive Hemicellulose Microgels during Spray Drying
Open this publication in new window or tab >>In Situ Cross-Linking of Stimuli-Responsive Hemicellulose Microgels during Spray Drying
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2015 (English)In: ACS Applied Materials and Interfaces, ISSN 1944-8244, E-ISSN 1944-8252, Vol. 7, no 7, 4202-4215 p.Article in journal (Refereed) Published
Abstract [en]

Chemical cross-linking during spray drying offers the potential for green fabrication of microgels with a rapid stimuli response and good blood compatibility and provides a platform for stimuli-responsive hemicellulose microgels (SRHMGs). The cross-linking reaction occurs rapidly in situ at elevated temperature during spray drying, enabling the production of microgels in a large scale within a few minutes. The SRHMGs with an average size range of similar to 1-4 mu m contain O-acetyl-galactoglucomannan as a matrix and poly(acrylic acid), aniline pentamer (AP), and iron as functional additives, which are responsive to external changes in pH, electrochemical stimuli, magnetic field, or dual-stimuli. The surface morphologies, chemical compositions, charge, pH, and mechanical properties of these smart microgels were evaluated using scanning electron microscopy, IR, zeta potential measurements, pH evaluation, and quantitative nanomechanical mapping, respectively. Different oxidation states were observed when AP was introduced, as confirmed by UV spectroscopy and cyclic voltammetry. Systematic blood compatibility evaluations revealed that the SRHMGs have good blood compatibility. This bottom-up strategy to synthesize SRHMGs enables a new route to the production of smart microgels for biomedical applications.

Keyword
cross-linking, microgel, hemicellulose, stimuli-responsive, spray drying, polysaccharides
National Category
Polymer Technologies
Identifiers
urn:nbn:se:kth:diva-163470 (URN)10.1021/am5084732 (DOI)000350193000040 ()25630464 (PubMedID)2-s2.0-84923794901 (Scopus ID)
Funder
EU, European Research Council
Note

QC 20150408

Available from: 2015-04-08 Created: 2015-04-07 Last updated: 2017-12-04Bibliographically approved

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