kth.sePublications KTH
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Tuning the rheological properties of laccase-crosslinked arabinoxylan hydrogels by prior arabinofuranosidase treatments
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Glycoscience.ORCID iD: 0009-0004-0539-5918
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Glycoscience.ORCID iD: 0000-0003-1355-649x
Department of Chemistry and Chemical Engineering, Division of Applied Chemistry, Chalmers University of Technology, Göteborg, SE, 41296, Sweden.ORCID iD: 0009-0004-9247-6221
Department of Chemical Engineering and Applied Chemistry, University of Toronto, 200 College Street, Toronto, Ontario, M5S 3E5, Canada.ORCID iD: 0000-0002-4753-6975
Show others and affiliations
2026 (English)In: Food Hydrocolloids, ISSN 0268-005X, E-ISSN 1873-7137, Vol. 172, article id 112080Article in journal (Refereed) Published
Abstract [en]

Arabinoxylans are the most abundant polysaccharides in the bran from wheat and rye kernels. Ferulic acid moieties covalently bound to arabinosyl substitutions in arabinoxylans can be oxidised and crosslinked by laccase enzymes, forming xylan hydrogels stabilised by chemical and physical interactions. Here, we explore the use of α-L-arabinofuranosidases to tune the rheological properties of laccase-crosslinked feruloylated arabinoxylans from wheat (WAX) and rye (RAX) brans, proposed to be mediated via intermolecular backbone interactions. The effect of subsequent freeze-drying and regeneration of the hydrogels on their multiscale structure and viscoelastic properties was further evaluated by X-ray scattering, microscopy and rheology measurements. The combined use of α-L-arabinofuranosidases from glycosyl hydrolase (GH) families GH62 and GH43 with complementary specificity towards different substitution motifs in arabinoxylan resulted in synergistic arabinose removal with a 48 % and 33 % increase in arabinose removal in WAX and RAX respectively, while retaining the ferulic acid moieties in both WAX and RAX. The extent of ferulic acid oxidation in WAX and RAX seemed to be affected by substrate inaccessibility for the laccase and polysaccharide chain aggregation, which was further accentuated by enzymatic arabinose removal. Rheological investigations revealed that laccase-crosslinked WAX hydrogels pretreated with arabinofuranosidases showed a decrease of 65–95 % in the storage and loss moduli compared to the non-pretreated WAX hydrogels, whereas arabinose removal improved the viscoelastic properties of RAX hydrogels both before and after regeneration, with an increase of storage moduli of 72–100 %. Arabinofuranosidase treatments and freeze-drying/regeneration altered the hydration properties of the hydrogels and their network structure, promoting the occurrence of ordered domains. Our results show that the biophysical properties of the arabinoxylans in terms of aggregation and hydration largely influence substrate accessibility to laccase-mediated oxidation and the multiscale assembly of the hydrogels upon freeze drying and regeneration, thus impacting their overall rheological properties. These dietary fibre hydrogels from cereal side streams have large potential to be used as food hydrocolloids, contributing to the overall circularity of the food system.

Place, publisher, year, edition, pages
Elsevier BV , 2026. Vol. 172, article id 112080
Keywords [en]
Arabinoxylan, Crosslinking, Enzyme technology, Hydrogels, Rheological properties
National Category
Polymer Chemistry Food Science Materials Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-372350DOI: 10.1016/j.foodhyd.2025.112080ISI: 001593218000001Scopus ID: 2-s2.0-105017841035OAI: oai:DiVA.org:kth-372350DiVA, id: diva2:2011920
Note

QC 20251106

Available from: 2025-11-06 Created: 2025-11-06 Last updated: 2026-05-13Bibliographically approved
In thesis
1. Engineering of Dietary Fibres: From Cereal Sidestreams Towards Multifunctional Prebiotic Hydrogels
Open this publication in new window or tab >>Engineering of Dietary Fibres: From Cereal Sidestreams Towards Multifunctional Prebiotic Hydrogels
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The food industry is one of the largest in Sweden and through it, large side streams are being generated. One such is bran, derived from cereal grains, composed of extractable dietary fibres capable of becoming novel materials such as laccase-driven crosslinked hydrogels. This thesis will explore the valorisation of these fibres through enzymatic modifications, as novel delivery vessel and potential prebiotic properties in order to integrate significant food losses into a circular economy with added health benefits towards the populace.

Feruloylated arabinoxylans previously extracted from wheat (WAX) and rye (RAX)were treated with selective arabinofuranosidases to successfully remove arabinose substitutions not containing ferulic acid moieties, exposing the xylan backbone. This lead largely to a reduced degree of crosslinking in WAX and RAX hydrogels. Rheological and morphological features were affected by the removal with an increase in viscoelastic properties in RAX hydrogels and lead to a more ordered network structure while WAX hydrogels saw the opposite effect regarding both features.

Residual β-glucans in WAX and RAX extracts were investigated. Their molecular weight differed from commercially available β-glucans derived from cereal endosperm, but ratios of cellotriosyl and cellotetraosyl remained similar to previously reported β-glucans. Removal of β-glucans from WAX and RAX extracts using a lichenase prior to laccase-crosslinking resulted in lowered viscoelastic properties for WAX hydrogels and an increase for RAX hydrogels. The removal likely exposes the arabinoxylan backbone similarly to arabinose removal. Freeze-drying at lower temperatures prior to regeneration of hydrogels lead to decreased pore size in hydrogels but increased porosity in RAX hydrogels and decreased in WAX hydrogels,which in turn lead to a decrease in viscoelastic properties in WAX hydrogels but increased in RAX hydrogels. Difference in chemical and physical interactions between the arabinoxylan network between WAX and RAX is believed to be behind their different behaviours. WAX and RAX hydrogels successfully encapsulated and retained target biomolecules of varying sizes and properties as a proof of concept. Pore size and porosity did not severely affect retention of smaller molecules such asglucose and tryptophan but for larger proteins. Addition of a gut bacteria xylanase triggered release of encapsulated molecules.

The common gut bacteria Bacteroides ovatus was successfully grown on WAX, RAX and CAX (corn arabinoxylans) extracts and hydrogels, producing health beneficial short chain fatty acids as secondary metabolites, highlighting the potential prebiotic properties of the extracts and hydrogels. Structural and biochemical differences between carbon sources affected growth, metabolite production and expression levels for enzymes related to arabinoxylan degradation. This thesis has demonstrated that dietary fibres can be effectively valorised by tuning them for multifunctional hydrogels contributing to a circular economy and improved public health.

Abstract [sv]

Livsmedelsindustrin är en utav Sveriges största industrier och generar ett överflöd av sidoströmmar. En sådan är kli från sädesslag bestående utav extraherbara kostfibrer med möjligheten att omvandlas till nya material såsom korslänkade hydrogeler via lackas. Denna avhandling kommer att utforska valoriseringen utav dessa fiberhydrogeler genom enzymatisk modifiering, nya leveransapplikationer och potentiella prebiotiska egenskaper för att integrera påtagliga matförluster i en cirkulär ekonomi med fördelar för folkhälsan.

Feruloylerade arabinoxylaner tidigare extraherade ifrån vete (WAX) -och rågkli (RAX) behandlades med selektiva arabinofuranosidaser för lyckad borttagning av arabinossubstitutioner som saknar ferulsyra därmed blottar xylanstamnätet. Detta ledde till en minskning av korslänkningar i WAX och RAX-hydrogeler. Reologiska och morfologiska egenskaper påverkades av detta med ökad viskoelasticitet och nätverkstruktur för RAX-hydrogeler medan WAX-hydrogeler upplevde en motsatteffekt.

Överblivna β-glukaner i WAX och RAX-extrakt undersöktes. Deras molekylvikt skilde sig ifrån kommersiella β-glukaner från sädesfrövita men förhållanden mellan cellotriosyl och cellotetraosyl överensstämde med tidigare uppmätta β-glukaner. Borttagning av β-glukaner med ett lichenas innan korslänkning via lackas resulteradei minskade viskoelastiska egenskaper för WAX-hydrogeler och en ökning för RAX hydrogeler. Borttagningen av β-glukaner blottar troligen arabinoxylanerna likt borttagningen av arabinos. Frystorkning vid lägre temperaturer innan regenerering ledde till minskade porer hos hydrogelerna men ökad porositet hos RAX och minskad i WAX, vilket i sin tur ledde till en minskning av viskoelastiska egenskaper hos WAX hydrogeler och ökning hos RAX-hydrogeler. Skillnaderna mellan kemiska och fysiska interaktioner mellan arabinoxylannätverken hos WAX och RAX ligger troligen bakomderas skilda beteende. Hydrogeler från WAX och RAX lyckades inkapsla och behålla specifika biomolekyler av varierande storlek och egenskaper som ett koncepttest.Porstorlek och porositet påverkade inte kvarhållandet av mindre molekyler såsom glukos och tryptofan men gjorde det för större proteiner. Tillskott av xylanas från magtarmbakterie frigav de inkapslade molekylerna.

Den vanliga magtarmbakterien Bacteroides ovatus lyckades växa på extrakt och hydrogeler från WAX, RAX och CAX (arabinoxylan från majs) och producera kortkedjade fettsyror som sekundära metaboliter därmed betona potentiellt prebiotiska egenskaper hos extrakten och hydrogelerna. Strukturella och biokemiska skillnader sinsemellan kolkällorna påverkade tillväxt, metabolitproduktion samt enzymuttryck relaterat till nedbrytning utav arabinoxylaner. Denna avhandling har påvisat att kostfibrers värde kan på ett effektivt sätt höjas genom att modifiera dem mot mångsidiga hydrogeler som bidrar till en cirkulär ekonomi och förbättrad folkhälsa.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2026. p. 86
Series
TRITA-CBH-FOU ; 2026:27
Keywords
Arabinoxylan, hydrogel, arabinofuranosidase, β-glucan, freeze-drying, encapsulation, dietary fibre, prebiotic, Bacteroides ovatus, Arabinoxylan, hydrogel, arabinofuranosidase, β-glukaner, frystorkning, inkapsling, kostfiber, prebiotika, Bacteroides ovatus
National Category
Food Science Biochemistry Polymer Chemistry Microbiology
Research subject
Chemistry
Identifiers
urn:nbn:se:kth:diva-381142 (URN)978-91-8106-620-3 (ISBN)
Public defence
2026-06-11, F3 (Flodis), Lindstedtvägen 26, Stockholm, 09:00 (English)
Opponent
Supervisors
Note

QC 20260518

Available from: 2026-05-18 Created: 2026-05-13 Last updated: 2026-05-19Bibliographically approved

Open Access in DiVA

No full text in DiVA

Other links

Publisher's full textScopus

Authority records

Rämgård, CarlLadd-Parada, MarjorieMcKee, Lauren S.Vilaplana, Francisco

Search in DiVA

By author/editor
Rämgård, CarlLadd-Parada, MarjorieJanewithayapun, RatchawitVuong, Thu V.Ström, AnnaMcKee, Lauren S.Vilaplana, Francisco
By organisation
Glycoscience
In the same journal
Food Hydrocolloids
Polymer ChemistryFood ScienceMaterials Chemistry

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 83 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association-8th-edition
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf