Tuning the rheological properties of laccase-crosslinked arabinoxylan hydrogels by prior arabinofuranosidase treatments
Bibliographic record
Abstract
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. • Arabinoxylan hydrogels with tuned rheology prepared by enzyme engineering • Laccase crosslinking was influenced by prior arabinofuranosidase treatment • Arabinofuranosidase and freeze-drying altered the hydration and network structure • Covalent crosslinking and physical chain interactions influence hydrogel rheology • Enzyme technology as selective tool to design functional food hydrocolloids
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How this classification was reachedexpand
Full frame distilled prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.
Codex and Gemma teacher scores by category
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.001 |
| Science and technology studies | 0.000 | 0.000 |
| Scholarly communication | 0.000 | 0.000 |
| Open science | 0.000 | 0.000 |
| Research integrity | 0.000 | 0.000 |
| Insufficient payload (model declined to judge) | 0.000 | 0.000 |
Machine scores (provisional)
The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.
Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.
score_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from itClassification
machine, unvalidatedMachine predicted; a candidate call from one teacher head, not a consensus.
How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".