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Nafion based proton exchange membrane (PEM) has long been used as conventional PEM in direct methanol fuel cell (DMFC) industry. However, the high cost of Nafion membrane and other drawbacks like high methanol crossover hinder the advancement of this industry. This study aims to develop a low cost membrane using sulfonated poly ether ether ketone (SPEEK) polymer. Silica and silicotungstic acid (SiWA) were incorporated into the membrane matrix using solution casting method. The optimum loading of the additives was tuned and it is discovered that the SPEEK membrane containing 10 wt% of silica and 5 wt% of SiWA has the best performance due to its high proton conductivity and moderately low methanol permeability. The performance of the membrane can further be enhanced by adding (3-aminopropyl)triethoxysilane (APTES) and carbonyldiimidazole (CDI) as coupling agents. Inclusion of APTES and CDI in SPEEK could not only improve the compatibility between organic SPEEK and inorganic additives, but also improve the homogeneity and dispersity of the additives. As a result, the resultant membrane with a better dimensional stability achieves high selectivity (10.60 × 104 S.s/cm3) up to 6.5 times more than pristine SPEEK membrane and 1.3 times higher than the commercial Nafion 117 membrane. • SPEEK/SiO 2 -SiWA was produced with APTES as coupling agent and CDI as promoter. • SPEEK1-AC achieved selectivity of 6.5 times higher than pristine SPEEK. • Silica-supported SiWA increased the proton conductivity of SPEEK membrane. • Improvement in homogeneity between organic SPEEK and inorganic additives. [ABSTRACT FROM AUTHOR]

Nafion, a perfluorosulfonic acid polymer, has been the standard membrane material for direct methanol fuel cells (DMFCs) due to its proton-carrying capabilities, despite its shortcomings as a methanol barrier. To attain self-healing and methanol-blocking properties, the incorporation of poly(vinyl alcohol) (PVA) polymer into Nafion was pursued. However, this strategy resulted in low proton conductivity. Thus, acid functional groups were added to a secondary modifier to boost proton conductivity. In this work, sulfonated graphene oxide (SGO) was assembled with Nafion and PVA through a simple freezing-thawing method to demonstrate a self-healable proton exchange membrane (PEM) without compromising the proton conductivity of Nafion. The synergistic effect of SGO in methanol-blocking and proton transport successfully strode over recast Nafion by hampering 33.2 % of methanol permeation and increasing 19.5 % of proton conductivity. As a result, the selectivity of the best hybrid PEM (N/PVA/SGO1.0) was increased by 1.8 times in comparison to recast Nafion. A single cell passive DMFC made using the novel hybrid membrane exhibited a power density of 6.07 mW cm−2 at a current density of 26.48 mA cm−2, and an open circuit voltage of 0.55 V at room temperature using 4 M methanol. This performance was essentially higher than that achieved by recast Nafion and commercial Nafion 117. The N/PVA/SGO1.0 hybrid membrane also showed remarkable self-healing properties, with 89 % recovery of methanol blocking function through reversible hydrogen bonding, illustrating its tremendous sustainable potential for use in DMFCs. [Display omitted] • Freeze-thaw process induces reversible physical crosslinking in N/PVA/SGO. • N/PVA/SGO achieves 28 % better DMFC performance than N117. • N/PVA/SGO demonstrates multiple times of self-healing. [ABSTRACT FROM AUTHOR]