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This study aimed to develop tannin-based non-isocyanate polyurethane (tannin-Bio-NIPU) and tannin-based polyurethane (tannin-Bio-PU) resins for the impregnation of ramie fibers ( Boehmeria nivea L.) and investigate their mechanical and thermal properties. The reaction between the tannin extract, dimethyl carbonate, and hexamethylene diamine produced the tannin-Bio-NIPU resin, while the tannin-Bio-PU was made with polymeric diphenylmethane diisocyanate (pMDI). Two types of ramie fiber were used: natural ramie without pre-treatment (RN) and with pre-treatment (RH). They were impregnated in a vacuum chamber with tannin-based Bio-PU resins for 60 min at 25 °C under 50 kPa. The yield of the tannin extract produced was 26.43 ± 1.36%. Fourier-transform infrared (FTIR) spectroscopy showed that both resin types produced urethane (-NCO) groups. The viscosity and cohesion strength of tannin-Bio-NIPU (20.35 mPa·s and 5.08 Pa) were lower than those of tannin-Bio-PU (42.70 mPa·s and 10.67 Pa). The RN fiber type (18.9% residue) was more thermally stable than RH (7.3% residue). The impregnation process with both resins could improve the ramie fibers' thermal stability and mechanical strength. The highest thermal stability was found in RN impregnated with the tannin-Bio-PU resin (30.5% residue). The highest tensile strength was determined in the tannin-Bio-NIPU RN of 451.3 MPa. The tannin-Bio-PU resin gave the highest MOE for both fiber types (RN of 13.5 GPa and RH of 11.7 GPa) compared to the tannin-Bio-NIPU resin.

Eco-Friendly Tannin-Based Non-Isocyanate Polyurethane Resins for the Modification of Ramie (Boehmeria nivea L.) Fibers