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Fundamentals of Interactions between Cellulose Materials and its Implications on Properties of Fibrous Networks
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Fibre- and Polymer Technology, Fibre Technology.ORCID iD: 0000-0002-3184-3532
2024 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Fundamental research plays a pivotal role in the development of sustainable solutions that benefit both our environment and everyday lives. Cellulose, as an abundant and renewable resource, holds immense potential for sustainable applications. However, navigating the complexities of molecular and supramolecular structure of cellulose poses significant challenges in harnessing its full potential. By delving into fundamental research, we aim to uncover the underlying mechanisms governing cellulose interactions, paving the way for innovative advancements in sustainable material development.This thesis uncovers the intricate relationship between fundamental research and applied methodologies by showing how molecular contact and structure at the interface of cellulose-rich materials will control the development of the macroscopic mechanical properties of networks from cellulose-rich fibres. The study encompasses various facets, ranging from the development of model materials for studying interfacial interactions to the preparation of fibrous networks with tailored properties.In the initial part of the work the research delves into the development of model materials to investigate interactions at smooth interfaces of regenerated cellulose. The study reveals the crucial role of the making and breaking of cellulose interface, or sometimes interphase, in the development of adhesive joints. Experimental findings demonstrate how chemical additives influence the interactions between cellulose surfaces, thereby modulating the structural and adhesive properties at the interface. Furthermore, by utilizing model materials, insights are gained into fibre-fibre interactions and the influence of surface treatments on network formation and mechanical performance. Lastly, the research focused on investigating the preparation of fibrous networks at different densities and amount of adsorbed additives, providing a comprehensive understanding of how network density and composition affect mechanical properties of the networks.This work not only exemplifies a synergistic approach, where fundamental insights into molecular contacts and interface structures are translated into practical applications for enhancing macroscopic properties but also highlights the importance of integrating fundamental and applied methodologies in molecular engineering, offering novel strategies for advancing sustainable paper production practices and contributing to the attainment of sustainable development goals.

Abstract [sv]

Grundläggande forskning spelar naturligtvis en avgörande roll i utvecklingen av hållbara materiallösningar och processer som gynnar både vår miljö och vårt vardagsliv. Cellulosa, som är en förnyelsebar och rikligt tillgänglig råvara, har också en enorm användnings potential i olika typer av hållbara material. Cellulosan har dock en avancerad och komplicerad molekylär och över molekylärstruktur och det är därför svårt att till fullo utnyttja den inneboende potentialen hos denna fascinerande råvara. Genom att fördjupa oss i och klarlägga de molekylära mekanismer som ligger till grund för växelverkan mellan cellulosarika ytor har vi skapat en grundförutsättning för att kunna utnyttja cellulosans inneboende egenskaper i olika typer av fiberbaserade nätverk . Resultaten i avhandlingen understryker den komplicerade och användbara kopplingen som finns mellan grundläggande förståelse och praktiska tillämpningar genom att visa hur den molekylära kontakten och strukturen i gränsytan mellan två cellulosa-rika ytor kommer att kontrollera de makroskopiska egenskaperna hos nätverk ifrån cellulosa rika fibrer. Studierna i avhandlingen omfattar olika aspekter, allt ifrån utvecklingen av väldefinierade och nm-jämna modellmaterial, för att studera molekylära växelverkai gränsytan mellan två cellulosa ytor, till framställningen av fibrösa nätverk med skräddarsydda egenskaper.I den första delen av arbetet har fokus legat på att utveckla väl karakteriserade modellmaterial och väldefinierade metoder för att klarlägga växelverkan i gränsytan eller gränsfasen mellan två cellulosa ytor. Resultaten visar också hur tillsats kemikalier påverkar växelverkan mellan cellulosa ytor och hur valet av kemikalier kan användas för att styra de strukturella och adhesiva egenskaperna hos gränsytan. Genom att använda våra modellmaterial har det också varit möjligt att bättre förstå de grundläggande mekanismerna som kontrollerar fiber-fiberväxelverkningar och därigenom hur tillsatskemikalier eller fibermodifieringar påverkar bildandet av en fiber/fiberfog och hur det i sin tur kontrollerar de makroskopiska mekaniska egenskaperna hos fibernätverket. I den sista delen av arbetet undersöktes hur olika mängder av fysikaliskt adsorberade styrkekemikalier och nätverks densiteter påverkar slutegenskaperna hos fibernätverk ifrån olika typer av fibrer. Resultaten visar att tillsatskemikalierna fortfarande har relativt sett stor positiv påverkan på de mekaniska egenskaperna hos nätverken, trots höga densiteter, vilket igen understryker vikten att klarlägga molekylära växelverkningar i gränsytan mellan fibrerna i ett fibernätverk.Sammantaget visar detta arbete inte bara hur grundläggande insikter om molekylära växelverkningar och gränsytsstrukturer har direkta praktiska tillämpningar för att förbättra makroskopiska egenskaper hos fibernätverk, utan det betonar också vikten av att integrera grundläggande och tillämpade metoder för skapa nya eller förbättrade biobaserade och recirkulerbara material.

Place, publisher, year, edition, pages
KTH Royal Institute of Technology, 2024. , p. 59
Series
TRITA-CBH-FOU ; 2024:15
Keywords [en]
Cellulose interactions, model materials, adhesive properties, chemical additives, fibre network.
National Category
Paper, Pulp and Fiber Technology
Research subject
Fibre and Polymer Science
Identifiers
URN: urn:nbn:se:kth:diva-345069ISBN: 978-91-8040-900-1 (print)OAI: oai:DiVA.org:kth-345069DiVA, id: diva2:1849267
Public defence
2024-05-03, F3, Lindstedtsvägen 26 & 28, Stockholm, 09:00 (English)
Opponent
Supervisors
Note

QC 2024-04-08

Available from: 2024-04-08 Created: 2024-04-05 Last updated: 2025-02-06Bibliographically approved
List of papers
1. Structure Development of the Interphase between Drying Cellulose Materials Revealed by In Situ Grazing-Incidence Small-Angle X-ray Scattering
Open this publication in new window or tab >>Structure Development of the Interphase between Drying Cellulose Materials Revealed by In Situ Grazing-Incidence Small-Angle X-ray Scattering
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2021 (English)In: Biomacromolecules, ISSN 1525-7797, E-ISSN 1526-4602, Vol. 22, no 10, p. 4274-4283Article in journal (Refereed) Published
Abstract [en]

The nano- to microscale structures at the interface between materials can define the macroscopic material properties. These structures are extremely difficult to investigate for complex material systems, such as cellulose-rich materials. The development of new model cellulose materials and measuring techniques has opened new possibilities to resolve this problem. We present a straightforward approach combining micro-focusing grazing-incidence small-angle X-ray scattering and atomic force microscopy (AFM) to investigate the structural rearrangements of cellulose/cellulose interfaces in situ during drying. Based on the results, we propose that molecular interdiffusion and structural rearrangement play a major role in the development of the properties of the cellulose/cellulose interphase; this model is representative of the development of the properties of joint/contact points between macroscopic cellulose fibers.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2021
National Category
Materials Chemistry
Identifiers
urn:nbn:se:kth:diva-304560 (URN)10.1021/acs.biomac.1c00845 (DOI)000708389300020 ()34541856 (PubMedID)2-s2.0-85116551335 (Scopus ID)
Note

QC 20211108

Available from: 2021-11-08 Created: 2021-11-08 Last updated: 2024-04-05Bibliographically approved
2. Reevaluation of the adhesion between cellulose materials using macro spherical beads and flat model surfaces
Open this publication in new window or tab >>Reevaluation of the adhesion between cellulose materials using macro spherical beads and flat model surfaces
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2024 (English)In: Carbohydrate Polymers, ISSN 0144-8617, E-ISSN 1879-1344, Vol. 332, p. 121894-121894, article id 121894Article in journal (Refereed) Published
Abstract [en]

Interactions between dry cellulose were studied using model systems, cellulose beads, and cellulose films, usingcustom-built contact adhesion testing equipment. Depending on the configuration of the substrates in contact,Polydimethylsiloxane (PDMS) film, cellulose films spin-coated either on PDMS or glass, the interaction showsthree distinct processes. Firstly, molecular interlocking is formed between cellulose and cellulose when there is asoft PDMS thin film backing the cellulose film. Secondly, without backing, no initial attraction force between thesurfaces is observed. Thirdly, a significant force increase, ΔF, is observed during the retraction process for cel­lulose on glass, and there is a maximum in ΔF when the retraction rate is increased. This is due to the kinetics of acontacting process occurring in the interaction zone between the surfaces caused by an interdigitation of a finefibrillar structure at the nano-scale, whereas, for the spin-coated cellulose surfaces on the PDMS backing, there isa more direct adhesive failure. The results have generated understanding of the interaction between cellulose-rich materials, which helps design new, advanced cellulose-based materials. The results also show thecomplexity of the interaction between these surfaces and that earlier mechanisms, based on macroscopic materialtesting, are simply not adequate for molecular tailoring.

Place, publisher, year, edition, pages
Elsevier BV, 2024
Keywords
Interaction, Cellulose thin film, Cellulose bead, Contact adhesion testing
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-344920 (URN)10.1016/j.carbpol.2024.121894 (DOI)001183175200001 ()38431407 (PubMedID)2-s2.0-85184997085 (Scopus ID)
Funder
Knut and Alice Wallenberg Foundation
Note

QC 20240408

Available from: 2024-04-03 Created: 2024-04-03 Last updated: 2024-04-08
3. The Use of Model Cellulose Materials for Studying Molecular Interactions at Cellulose Interfaces
Open this publication in new window or tab >>The Use of Model Cellulose Materials for Studying Molecular Interactions at Cellulose Interfaces
2023 (English)In: ACS Macro Letters, E-ISSN 2161-1653, Vol. 12, no 11, p. 1530-1535Article in journal (Refereed) Published
Abstract [en]

Despite extensive research on biobased and fiber-basedmaterials, fundamental questions regarding the molecular processesgoverning fiber−fiber interactions remain unanswered. In this study, weintroduce a method to examine and clarify molecular interactions withinfiber−fiber joints using precisely characterized model materials, i.e.,regenerated cellulose gel beads with nanometer-smooth surfaces. Byphysically modifying these materials and drying them together to createmodel joints, we can investigate the mechanisms responsible for joiningcellulose surfaces and how this affects adhesion in both dry and wet statesthrough precise separation measurements. The findings reveal a subtlebalance in the joint formation, influencing the development ofnanometer-sized structures at the contact zone and likely inducingbuilt-in stresses in the interphase. This research illustrates how model materials can be tailored to control interactions betweencellulose-rich surfaces, laying the groundwork for future high-resolution studies aimed at creating stiff, ductile, and/or tough jointsbetween cellulose surfaces and to allow for the design of high-performance biobased materials.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2023
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-344919 (URN)10.1021/acsmacrolett.3c00578 (DOI)001096724800001 ()37910654 (PubMedID)2-s2.0-85178324088 (Scopus ID)
Funder
Knut and Alice Wallenberg FoundationStora Enso
Note

QC 20240404

Available from: 2024-04-03 Created: 2024-04-03 Last updated: 2024-04-05Bibliographically approved
4. Model Systems for Clarifying the Effects of Surface Modification on Fibre-Fibre Joint Strength and Paper Mechanical Properties
Open this publication in new window or tab >>Model Systems for Clarifying the Effects of Surface Modification on Fibre-Fibre Joint Strength and Paper Mechanical Properties
(English)Manuscript (preprint) (Other academic)
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-345067 (URN)
Note

QC 20240430

Available from: 2024-04-05 Created: 2024-04-05 Last updated: 2024-04-30Bibliographically approved
5. Influence of density and chemical additives on paper mechanical properties
Open this publication in new window or tab >>Influence of density and chemical additives on paper mechanical properties
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(English)Manuscript (preprint) (Other academic)
National Category
Paper, Pulp and Fiber Technology
Identifiers
urn:nbn:se:kth:diva-345068 (URN)
Note

QC 20240430

Available from: 2024-04-05 Created: 2024-04-05 Last updated: 2024-04-30Bibliographically approved

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