Vitrification: Versatile Method To Modulate Properties of Myrcene-Based Rubbers
Why this work is in the frame
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Bibliographic record
Abstract
We report bio-derived vitrimeric rubbers with weldability and excellent reprocessability. Reversible-deactivation radical copolymerization of the commercially available terpene-based β-myrcene with 10 to 30 mol % (2-acetoacetoxy)ethyl methacrylate (AAEMA) afforded linear prepolymers, which were cross-linked in a single step treatment with difunctional amine, the vegetable oil-derived Priamine 1075, or trifunctional amine tris(2-aminoethyl)amine (TREN). Decoupling the networks’ backbone structure and cross-linkers led to high tunability of the vitrimers’ final mechanical and rheological properties using prepolymer composition, molecular weight, nature and concentration of cross-linker, and cross-linking density. Glass transition temperature ( T g ) of the vitrimers ranged between −49 and −5 °C, while the average elongation and stress at break ranged from ∼83% and 0.18 MPa to ∼30% and 1.68 MPa, respectively from the lowest, 0.12 mol/L, to the highest, 0.98 mol/L, cross-linking densities. The characteristic features of dynamic vinylogous urethane-vitrimers were confirmed over at least three reprocessing cycles by grounding and hot-pressing at 110 °C. No appreciable changes in the ATR-FTIR spectra, T g, decomposition temperatures, tensile properties, and storage modulus were observed due to reprocessing. Furthermore, the incorporation of 5 mol % epoxy-based glycidyl methacrylate into the prepolymer led to the formation of a network with dual static and dynamic cross-links. Compared to the counterpart network with solely dynamic cross-links, the addition of static cross-links decreased creep by 75% and imparted shape memory effects. This work shows that combining vitrimer chemistry with myrcene is a facile and inexpensive, yet highly versatile method to not only modulate and compensate for the poorer mechanical properties of brush-like terpene-based elastomers but also provides a potential platform for recyclable biobased rubbers with more sophisticated functionalities.
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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 | 0.001 | 0.000 |
| Meta-epidemiology (narrow) | 0.000 | 0.000 |
| Meta-epidemiology (broad) | 0.001 | 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 | 0.001 |
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 it