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Nanostructured biocomposites based on bacterial cellulosic nanofibers compartmentalized by a soft hydroxyethylcellulose matrix coating
KTH, School of Chemical Science and Engineering (CHE), Fibre and Polymer Technology. KTH, School of Biotechnology (BIO), Glycoscience.ORCID iD: 0000-0001-9832-027X
KTH, School of Biotechnology (BIO), Glycoscience.
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2009 (English)In: Soft Matter, ISSN 1744-683X, Vol. 5, no 21, 4124-4130 p.Article in journal (Refereed) Published
Abstract [en]

Biomimetic approaches involving environmentally-friendly synthetic pathways provide an opportunity to elaborate novel high-performance biocomposites. Here we have developed a low-energy biosynthetic system for the production of a high-strength composite material consisting of self-assembled and nanostructured cellulosic nanofibers. This biocomposite is analogous to natural composite materials with high strength and hierarchical organization such as wood or tendon. It was generated by growing the bacterium Acetobacter, which naturally produces cellulosic nanofibers, in the presence of hydroxyethylcellulose (HEC). Individual cellulose fibrils were coated by HEC and exhibited a smaller lateral dimension than pure bacterial cellulose (BC) fibrils. They self-assembled to form compartmentalized nanofibers and larger cellulose fibril aggregates compared to pure BC. The tensile strength of nanocomposite films prepared from the compartmentalized cellulosic nanofibers was 20% higher than that of pure BC sheets and wood cellulose nanopapers, and 60% higher than that of conventional BC/HEC blends, while no strain-to-failure decrease was observed. The thin nanoscale coating consisting of hydrated HEC significantly increased the mechanical performance of the nanocomposite films by provoking compartmentalization of individual fibrils.

Place, publisher, year, edition, pages
2009. Vol. 5, no 21, 4124-4130 p.
Keyword [en]
cp/mas c-13 nmr, different polymeric additives, cell-wall, polysaccharides, in-situ crystallization, acetobacter-xylinum, native, cellulose, mechanical-properties, composites, microfibrils, spectroscopy
National Category
Chemical Sciences
Identifiers
URN: urn:nbn:se:kth:diva-18869DOI: 10.1039/b907838jISI: 000270837900008Scopus ID: 2-s2.0-70350117835OAI: oai:DiVA.org:kth-18869DiVA: diva2:336916
Note

QC 20100525

Available from: 2010-08-05 Created: 2010-08-05 Last updated: 2015-05-26Bibliographically approved
In thesis
1. Structural changes during cellulose composite processing
Open this publication in new window or tab >>Structural changes during cellulose composite processing
2012 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Two approaches for creating a new all-cellulose composite material have been studied: the biosynthesis of compartmentalised bacterial cellulose fibril aggregates and the compression moulding of commercial chemical wood pulps processed with only water. The objective was to study the structural changes during processing and the complexity of relating the mechanical properties of the final biocomposites to the nanoscale structure was highlighted.

Solid-state CP/MAS 13C NMR spectroscopy was utilised to determine both the fibril aggregate width and the content of the different crystalline cellulose forms, cellulose I and cellulose II. Using this method, the quantities of hemicellulose present inside the fibre wall and localised at the fibre surfaces could be determined.

The formation of cellulose fibrils was affected by the addition of hydroxyethylcellulose (HEC) to a culture medium of Acetobacter aceti, and the fibrils were coated with a thin layer of HEC, which resulted in loose bundles of fibril aggregates. The HEC coating, improved the fibril dispersion in the films and prevented fractures, resulting in a biocomposite with remarkable mechanical properties including improved strength (289 MPa), modulus (12.5 GPa) and toughness (6%).

The effect of press temperature was studied during compression moulding of sulphite dissolving-grade pulps at 45 MPa. A higher press temperature yielded increases in the fibril aggregation, water resistance (measured as the water retention value) and Young’s modulus (12 GPa) in the final biocomposite. The high pressure was important for fibril aggregation, possibly including cellulose-cellulose fusion bonds, i.e., fibril aggregation in the fibre-fibre bond region. The optimal press temperature was found to be 170°C because cellulose undergoes thermal degradation at higher temperatures.

The effect of hemicellulose was studied by comparing a softwood kraft paper-grade pulp with a softwood sulphite paper and a softwood sulphite dissolving-grade pulp. A significant fibril aggregation of the sulphite pulps suggested that the content and distribution of hemicellulose affected the fibril aggregation. In addition, the hemicellulose structure could influence the ability of the hemicellulose to co-aggregate with cellulose fibrils. Both sulphite pulp biocomposites exhibited Young’s moduli of approximately 12 GPa, whereas that of the kraft pulp was approximately half that value at 6 GPa. This result can be explained by a higher sensitivity to beating in the sulphite pulps.

The effect of mercerisation, which introduces disordered cellulose, on the softwood sulphite dissolving-grade pulp was also studied under compression moulding at 170°C and 45 MPa. The mechanisms causing an incomplete transformation of cellulose I to II in a 12 wt% NaOH solution were discussed. The lower modulus of cellulose II and/or the higher quantity of disordered cellulose likely account for the decrease in Young’s modulus in the mercerised biocomposites (6.0 versus 3.9 GPa).

Abstract [sv]

Två metoder för att skapa ett nytt kompositmaterial baserat på enbart cellulosa har studerats, biosyntes av fibrillaggregat bestående av bakteriecellulosa och varmpressning av kommersiella träfiberbaserade massor med vatten som den enda processkemikalien. Målet var att studera de strukturella förändringarna som sker under tillverkningsprocessen. Även komplexiteten i att relatera strukturen på nanonivå till de mekaniska egenskaperna hos de slutliga biokompositerna belystes.

Med fastfas CP/MAS 13C NMR-spektroskopi var det möjligt att bestämma både fibrillaggregattjockleken och mängden av cellulosakristallformerna; cellulosa I och cellulosa II. Det var också möjligt att bestämma mängden hemicellulosa dels närvarande inuti fiberväggen och dels mängden lokaliserad på fiberytor.

Tillsats av hydroxyetylcellulosa (HEC) i odlingsmediet för Acetobacter aceti påverkade bildandet av cellulosafibriller som blev belagda med ett tunt skikt av HEC, vilket också resulterade i löst bundna fibrillaggregat. HEC-beläggningen förbättrade fibrilldispersionen i filmerna och minskade sprickbildningen, vilket gav en biokomposit med mycket goda mekaniska egenskaper med kombinerad hög styrka (289 MPa), styvhet (12.5 GPa) och seghet (6%).

Effekten av presstemperatur vid varmpressning (45 MPa tryck) studerades på sulfit dissolvingmassor. Högre presstemperatur gav ökad fibrillaggregering, ökat vattenmotstånd (mätt som vattenretentionsvärde) och högre styvhet (12 GPa) för biokompositen. Det höga trycket var också viktigt för fibrillaggregeringen, som troligen omfattar cellulosa-cellulosa samkristallisation dvs. fibrillaggregering i fiber-fiber-bindningsregionen. Den optimala presstemperaturen föreslogs vara 170° C pga. termisk nedbrytning av cellulosa vid högre temperaturer.

Effekten av hemicellulosa studerades genom att jämföra sulfat pappersmassa med sulfit pappersmassa och sulfit dissolvingmassa. Mängden och fördelningen av hemicellulosa föreslogs ligga till grund för skillnaden i fibrillaggregering, som var mera uttalad i sulfitmassorna. Även hemicellulosans struktur kan påverka förmågan hos hemicellulosa att sam-aggregera med cellulosafibriller. Biokompositerna baserade på sulfitmassorna hade en styvhet på ca. 12 GPa, medan sulfatmassan bara hade hälften av den nivån ca. 6 GPa, vilket förklarades av sulfitmassornas högre känslighet för malning.

Även effekten av mercerisering av sulfit dissolvingmassa varmpressad vid 170° C och 45 MPa studerades. Mercerisering introducerar oordnad cellulosa och mekanismerna som endast ger en partiell omvandling av cellulosa I till II i en 12 vikt% NaOH-lösning diskuterades. Den sämre styvheten hos den merceriserade biokompositen (6.0 resp. 3.9 GPa) förklaras troligen genom cellulosa II kristallens lägre styvhet och/eller den högre mängden av oordnad cellulosa.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2012. xi, 48 p.
Series
Trita-CHE-Report, ISSN 1654-1081 ; 2012:46
Keyword
CP/MAS 13C NMR, cellulose, fibril aggregation, biocomposite, compression moulding, supramolecular structure
National Category
Chemical Sciences Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-104568 (URN)978-91-7501-518-7 (ISBN)
Public defence
2012-11-30, K1, Teknikringen 56, KTH, Stockholm, 10:00 (English)
Opponent
Supervisors
Projects
Wallenberg Wood Science CenterBiomime
Funder
Knut and Alice Wallenberg Foundation
Note

QC 20121106

Available from: 2012-11-06 Created: 2012-11-06 Last updated: 2012-11-09Bibliographically approved
2. Analyzing the properties and biosynthesis of β-glucans from Gluconacetobacter and poplar
Open this publication in new window or tab >>Analyzing the properties and biosynthesis of β-glucans from Gluconacetobacter and poplar
2014 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Glucans are polysaccharides integral to many materials and biological functions. Under the umbrella of Biomime, the Swedish Center for Biomimetic Fiber Engineering, this work has aimed to improve basic understanding of the biosynthesis of such glucans. This has been achieved through direct investigation of cellulose structure, and by developing the tools to analyze glucan biosynthesis. Notably we have identified a novel chemical effector of glucan synthesis processes and developed a proteomic toolkit useful for analyzing membrane-bound glycosyltransferases, the enzyme group responsible for glucan biosynthesis. During this work, glucan synthesis has been studied using both Gluconacetobacter and Populus cell suspension cultures.

Publication I. Gluconacetobacter cellulose (BC) was used as a base to create a novel and well characterized nano-material with improved mechanical properties. This novel composite of BC and hydroxyethylcellulose (HEC) had improved tensile strength compared to pure BC. Through thorough study utilizing dispersion measurements, electron microscopy, nuclear magnetic resonance and X-ray diffraction it was shown that the improved properties derived from a layer of HEC coating each fibril.

Publication II. Bacterial cellulose was labeled in specific positions with 13C (C4 and C6). These samples were analyzed by CP/MAS NMR along with cellulose samples from cotton and Halocynthia sp. For each sample spectral fitting was performed and general properties of crystal allomorph composition and fibril widths were determined. Calculations were also made for water accessible surfaces of the fibrils. The results showed that water accessible C4 surface signals are reflective of the allomorph composition of the sample, along with a distorted signal that derives due to fibril imperfections. Water accessible surface signals from the C6 region are instead derived from rotamer conformations of the C6 hydroxymethyl groupsfrom glucose residues.

In Publication III, a high-throughput screen was used to identify an inhibitor of Golgi-derived glycosyltransferase activity, termed chemical A. The structural basis for inhibition was determined and in vitro assays of callose synthesis were performed. The in vitro assays revealed chemical A to also be an activator of callose synthesis. To understand this activation kinetic studies were performed, showing that chemical A is a mixed type of activator, which can bind either the free enzyme or the enzyme-substrate complex. Chemical A has uses in chemical genetics for dissecting processes involving callose synthesis, such as stress response and cell-plate formation.

In publication IV, we present an in-house developed platform for proteomics with a distributed processing model. This in-house system has been central to many proteomics tasks, including for those presented in publication V, and is being distributed as the Automated Proteomics Pipeline (APP).

In publication V, conditions for enrichment of Detergent-Resistant Microdomains (DRM) have been optimized for Populus trichocarpa cell cultures. The proteins enriched in DRM were identified using mass spectrometry based proteomics, and a functional model for DRM was proposed. This model involves proteins specialized in stress response, including callose synthase, and cell signaling. This further strengthens the arguments for DRMs as sites of specific cellular functions and confirms they play a role in glucan synthesis.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2014. 66 p.
Series
TRITA-BIO-Report, ISSN 1654-2312 ; 2014:8
Keyword
Cellulose synthesis, Bioinformatics, Proteomics, Cell wall
National Category
Biological Sciences Bioinformatics and Systems Biology
Identifiers
urn:nbn:se:kth:diva-147932 (URN)978-91-7595-184-3 (ISBN)
Public defence
2014-09-05, FR4, AlbaNova, Roslagstullsbacken 21, Stockholm, 13:00 (English)
Opponent
Supervisors
Note

QC 20140710

Available from: 2014-07-10 Created: 2014-07-09 Last updated: 2014-07-10Bibliographically approved

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