Relating Redox Properties of Polyvinylamine-<i>g</i>-TEMPO/Laccase Hydrogel Complexes to Cellulose Oxidation
Bibliographic record
Abstract
The structure and electrochemical properties of adsorbed complexes based on mixtures of polyvinylamine- g -TEMPO (PVAm-T) and laccase were related to the ability of the adsorbed complexes to oxidize cellulose. PVAm-T10 with 10% of the amines bearing TEMPO moieties (i.e., DS = 10%), adsorbed onto gold sulfonate EQCM-D sensor surfaces giving a hydrogel film that was 7 nm thick, 89% water, and encasing laccase (200 mM) and TEMPO moieties (33 mM). For DS values >10%, all of the TEMPOs in the hydrogel film were redox-active in that they could be oxidized by the electrode. With hydrogel layers made with lower-DS PVAm-Ts, only about half of the TEMPOs were redox-active; 10% DS appears to be a percolation threshold for complete TEMPO-to-TEMPO electron transport. In parallel experiments with hydrogel complexes adsorbed onto regenerated cellulose films, the aldehyde concentrations increased monotonically with the density of redox-active TEMPO moieties in the adsorbed hydrogel. The maximum density of aldehydes was 0.24 μmol/m 2, about 10 times less than the theoretical concentration of primary hydroxyl groups exposed on crystalline cellulose surfaces. Previous work showed that PVAm-T/laccase complexes are effective adhesives between wet cellulose surfaces when the DS is >10%. This work supports the explanation that TEMPO-to-TEMPO electron transport is required for the generation of aldehydes necessary for wet adhesion to PVAm.
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How this classification was reachedexpand
Full frame machine prediction
Teacher imitationNot calibrated prevalence, not ground truth. Human validation pending. The Gemma side is a direct model label for every work in the frame, read from the title-only record. The Codex side is a classifier learned from the 10,348 direct Codex labels and calibrated to design-weighted sample rates; fields without enough sample support carry no Codex call. Candidate is the union of the two sides; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels.
Distilled classifier scores by category (both heads)
| Category | Codex | Gemma |
|---|---|---|
| Metaresearch | 0.000 | 0.001 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.000 | 0.000 |
| Bibliometrics | 0.000 | 0.000 |
| 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) | 0.001 | 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 source (direct Gemma or distilled Codex), 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".