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Molecules 2020, 25, 1712 23 of 44 the composite membranes did not perform as well as the baseline Nafion, with long term conductivity testing resulting in a continuous decrease in conductivity (80 ◦C, 70% RH for 4 days). The authors discovered that this is due to the excess acidity of the PFSA, humidification and gas flow reducing the cerium oxide into (III) which then binds to the sulphonic groups, inhibiting proton conduction. This was confirmed by reprotonation via sulphuric acid and the proton conductivity went back to its original value. Figure 6. Pre- and post 500 h test performance curves; reproduced with permission from [173]. Lee et al. [175] prepared cerium oxide impregnated sulfonated poly(arylene ether sulfone) (SPES, 50% degree of sulphonation) membranes aiming for improved fuel cell durability. The addition of cerium oxide led to a drop in water uptake, IEC and proton conductivity. With increasing loading resulting in lower water uptake, IEC and proton conductivity. However, the ex-situ Fenton reagent tests was performed to study the oxidative stability of the composite membranes. Introduction of the cerium oxide led to a decrease in degradation of the membrane. In addition, single cell accelerated OCV hold testing (90 ◦C, 30% RH, 0.5 bar) showed that the composite membrane with 2% cerium oxide was stable for up to 2200 h, compared to 670 h for the pristine SPES. Elakkiya et al. decided to enhance the proton conductivity of composite membranes by using sulphonated TiO2 coated in polyaniline within a SPES polymer matrix [176]. Water uptake and proton conductivity improved with the addition of the filler however, no in-situ testing was performed. It would be interesting to see what effect the polyaniline has on fuel cell performance, and if the sulphonated filler improves performance at elevated temperatures/reduced humilities. Lee et al. [177] synthesized sulphonated silicon dioxide within SPAEK. As expected, the addition of the filler improved fuel cell performance (at 60 ◦C and at both 100 and 70% RH) but the functionalised filler also outperformed the composite with non-functionalised silicon dioxide. This is due to the sulphonic groups retaining more water and allowing sufficient proton transport. 3.2. Carbon Nanomaterial Fillers In recent year carbon nanomaterials have become the go-to filler, particularly graphene oxide due to its abundance of oxygen containing functional groups [178]. These oxygen-containing functional groups attract water molecules and are able to retain higher levels of water in comparison to pristine Nafion. In addition, graphene oxide’s flat structure meansPDF Image | Composite Polymers for Electrolyte Membrane Technologies
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