Epoxy-based vitrimeric semi-interpenetrating network/MXene nanocomposites for hydrogen gas barrier applications†

Abstract

Herein, we report MXene-filled epoxy-based vitrimeric nanocomposites featuring a semi-interpenetrating network (S-IPN) to develop a hydrogen gas (H₂) barrier coating with self-healing characteristics for compressed H₂ storage applications. The reversible epoxy network was formed by synthesizing linear epoxy chains with pendent bis-hydroxyl groups using amino diol, which were then crosslinked with 1,4-benzenediboronic acid to generate dynamic boronic ester linkages. To achieve the S-IPN-type molecular arrangement, the epoxy chains were in situ crosslinked in the presence of poly(ethylene-co-vinyl alcohol) (EVOH), giving rise to a self-healing network (EEP) with a healing efficiency of 87%. Into the S-IPN vitrimer (EEP), a 2D platelet-type nanofiller MXene was incorporated to introduce a tortuous path for H₂ gas diffusion along with improved mechanical properties. The nanocomposite coating was applied to nylon 6 liner material, which is conventionally used in all-composite H₂ storage vessels. The application of a 2 wt% MXene/EEP nanocomposite coating showed a permeability coefficient of 0.062 cm³ mm m⁻² d⁻¹ atm⁻¹ exhibiting ∼96% reduction in gas permeability compared to uncoated nylon 6. The same nanocomposite exhibited a healing efficiency of 79%. Increasing the MXene loading to 10 wt% further reduced the permeability coefficient to 0.002 cm³ mm m⁻² d⁻¹ atm⁻¹; however, the healing efficiency decreased due to restricted chain mobility. In essence, the current work highlights the potential of vitrimeric S-IPN nanocomposite coatings for H₂ gas-barrier applications, enhancing safety and performance.