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Molecules 2020, 25, 1712 31 of 44 physical structure (nanoparticle, flat, nanotubes). Therefore, when selecting a filler material not only should the material itself and possible functionalising be considered, but also the shape of the filler itself. Another point of consideration is the polymer that the filler will be embedded in. As we have shown, composite membranes were made using different polymers such as Nafion, SPEEK and SPAES. However, only Nafion meets industry standards regarding lifetime and durability. This implies that composite membranes should use a Nafion matrix in addition to Nafion ionomer in the GDE. Overall, membrane performance has to be looked at from a variety of experiments, such as; cell polarisation and power, long term durability and ex-situ tests to name a few. A membrane that performs well in-situ might degrade quickly during thermal/humidity cycling and be unsuitable. Another point of consideration is the interaction between the composite membrane and the catalyst layer. Conventional Nafion membranes use gas diffusion electrodes that consist of Nafion ionomer binder. However the addition of a filler material could potentially affect this interaction between the membrane and catalyst layer, for example the filler is added to only improve the membrane performance but if some of the filler is dispersed closer to the edges of the membrane then this could interfere with the anode and cathode functions (hydrophilic fillers situated close to the cathode could cause flooding more easily). Also, the ionomer and membrane might not consist of the same material, further complicating this interaction, which would be exacerbated during manufacturing of MEAs with composite membranes and binders of different materials. To the authors knowledge, the use of composite ionomers in the catalyst layer is not studied and requires further research. Composite membranes are tested for their performance in-situ (fuel cell testing) and ex-situ (proton conductivity, water uptake etc.), however their durability during fuel cell testing is an area of research not fully explored. In order to be competitive with conventional Nafion membranes, the composite membrane must not only be able to perform better but also perform adequately over long periods. Composite membranes are developed aiming for harsher operating conditions (higher temperature and lower humidity) and therefore their durability must be investigated and demonstrated in-situ. It is also important to study the change in the membrane degradation mechanisms due to the presence of fillers, for instance; how does the filler affect the membrane mechanical properties due to the humidity cycling and what is the impact of the filler on the catalyst stability or dissolution into the membrane. 4. Composite Membranes for Electrolysers Composite membranes with metal oxides as fillers (SiO2, TiO2, or WO2) showed promising properties for high temperature operation of PEM water electrolysers allowing achieving high performance with respect to a commercial membrane. Baglio et al. [212] and Antonucci et al. [213] focused their work on Nafion-TiO2 and Nafion-SiO2 respectively, to allow efficient operation at high temperature, above 100 ◦C. Both works claimed that the high temperature operating conditions were allowed by the better water retention and more uniform distribution of water across the composite membrane due to the presence of inorganic hygroscopic fillers inside the polymeric matrix. This resulted in reduced ohmic resistance and therefore better electrolyser performance [214]. The performance of composite membranes was better than that of Nafion membrane under high temperature and high pressure so the application of this technology is very promising especially when high electrical efficiency is required. As evidence of this result, Figure 10 illustrates characteristics curve of cell equipped with commercial Nafion and composite Nafion-SiO2 membranes at high temperature and pressure. These alternative composite membranes also showed a decrease of the cross-over of the gases through the membrane. However, a slight decay of performance was observed during the experiment; thus, a further amelioration of membrane is necessary to improve the stability and lifetime. Another way to produce electrolyte membranes with high conductivity and durability for water electrolysers is using perfluorosulfonic acid with shorter and non-branched pendant side-chain with higher crystallinity than longer side-chain perfluorosulfonic acid. Aricò et al. [215] used the Aquivion short side chain perfluorosolfonic membrane using Nafion 111 for comparison. Authors claimed thatPDF Image | Composite Polymers for Electrolyte Membrane Technologies
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