This is a comparative study to clarify the effect of the introduction of layered double hydroxide (LDH) into various polymer matrices. One perfluorosulfonic acid polymer, i.e., Nafion, and two polyaromatic polymers such as sulfonated polyether ether ketone (sPEEK) and sulfonated polysulfone (sPSU), were used for the preparation of nanocomposite membranes at 3 wt.% of LDH loading. Thereafter, the PEMs were characterized by X-ray diffraction (XRD) and dynamic mechanical analysis (DMA) for their microstructural and thermomechanical features, whereas water dynamics and proton conductivity were investigated by nuclear magnetic resonance (PFG and T1) and EIS spectroscopies, respectively. Depending on the hosting matrix, the LDHs can simply provide additional hydrophilic sites or act as physical crosslinkers. In the latter case, an impressive enhancement of both dimensional stability and electrochemical performance was observed. While pristine sPSU exhibited the lowest proton conductivity, the sPSU/LDH nanocomposite was able to compete with Nafion, yielding a conductivity of 122 mS cm-1 at 120 °C and 90% RH with an activation energy of only 8.7 kJ mol-1. The outcome must be ascribed to the mutual and beneficial interaction of the LDH nanoplatelets with the functional groups of sPSU, therefore the choice of the appropriate filler is pivotal for the preparation of highly-performing composites.
Keywords: PFG-NMR; dynamic mechanical analysis; layered double hydroxides; nanocomposite membranes; proton conductivity; proton exchange membrane fuel cells; proton exchange membranes; swelling tests.