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Article Dans Une Revue Macromolecules Année : 2022

Harnessing Catalysis Selectivity and Isophorone Diisocyanate Asymmetry for Tailored Polyurethane Prepolymers and Networks

Résumé

We synthesized polyurethane (PU) materials via a typical two-stage industrial process based on the synthesis of NCO-terminated prepolymers, followed by their crosslinking with polyols. We investigated the influence of metallic and organic catalysts on (i) polyaddition kinetics between a challenging monomer (aliphatic and asymmetric isophorone diisocyanates, a.k.a. IPDI) and polyols and (ii) the structure and properties of corresponding PU prepolymers and networks. Tin (Sn)-free catalysts (Ti- and Zn-based) and even metal-free catalysts (guanidines, amidines, and amines) are competitive alternatives to a standard Sn catalyst. Besides the activity criterion, appropriately choosing the catalyst allowed us to adjust the prepolymer structure relying on respective selectivities toward primary versus secondary isocyanate moieties as well as the propensity to favor functionalization over chain extension. By quantitative NMR spectroscopy, three different catalyst selectivities were pinpointed, which either favored the primary or secondary isocyanate functions or promoted their isoreactivity. These selectivities were harnessed at both the prepolymerization and crosslinking stages to significantly decrease the reaction time by judicious and innovative combinations of catalysts with opposite selectivities toward primary/secondary isocyanates. We eventually evidenced the efficiency of this methodology for tailored PU-based materials through in situ solid-state NMR monitoring of the crosslinking stage.
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Dates et versions

hal-03728235 , version 1 (20-07-2022)

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Priscilla Arnould, Frédéric Simon, Stéphane Fouquay, Francis Pardal, Guillaume Michaud, et al.. Harnessing Catalysis Selectivity and Isophorone Diisocyanate Asymmetry for Tailored Polyurethane Prepolymers and Networks. Macromolecules, 2022, 55 (8), pp.3344-3352. ⟨10.1021/acs.macromol.1c02491⟩. ⟨hal-03728235⟩
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