GSH-responsive polyurethane/PBAT blend films: degradation kinetics, ecotoxicity screening, and governance-carbon...

This study presents a transferable three-tier mapping framework translating laboratory degradation kinetics and ecotoxicity data of stimulus-responsive biodegradable materials into evolutionary game parameters and life cycle assessment (LCA) scenarios. Using glutathione (GSH)-responsive polyurethane (PUs)/poly(butylene adipate-co-terephthalate) (PBAT) blend films (20 : 80 w/w) as proof-of-concept, the films achieved 27.3 ± 1.8 MPa tensile strength with ∼90% disulfide embedding efficiency. An iso-crystallinity control (HDO-extended, disulfide-free, matched ∼20% crystallinity) confirmed >96% of acceleration derives from disulfide cleavage (99.2% vs. 19.5% mass loss at 498 h under 20 mM GSH, 313 K); 0.5 mM was the minimum effective GSH threshold (38.2% mass loss; 2.8-fold k-based acceleration). Arrhenius analysis yielded E _α,GSH = 45.2 ± 2.1 kJ mol^-1, 17.0 kJ mol^-1 below the hydrolysis pathway (P = < 0.01; ΔE _α 95% CI: 7.3-26.7 kJ mol^-1). Ecotoxicity screening confirmed no significant adverse effects; LC-MS identified sulfur-containing products below ecotoxicological thresholds. A three-dimensional scoring scheme maps material data into game parameters; structural decomposition revealed public participation sensitivity of 45% at R/C _eco = 1.2, with Monte Carlo validation (∼72% equilibrium survival). Functional coupling from game equilibria to disposal fractions (five-benchmark calibration; leave-one-out cross-validation: 2.8 pp) yielded carbon footprints of ∼550-1100 kg CO₂-eq per ton, with governance upgrading saving ∼540 kg CO₂-eq per ton-56% of the Scenario A reduction relative to PE.