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Molecules 2020, 25, 1712 30 of 44 anhydrous application. Composite membranes with random and block polymers were made and characterised to understand their behaviour. The degradation onset temperature for all the membranes were 250 ◦C and above, this means that they are suitable for operating in higher temperature fuel cells. The authors stated that the distribution of the ionic groups and the flexibility of the sulfonic groups are important determinants in ion conduction. Fuel cell experiments at 120 ◦C and with no humidity showed that the random chain SPI and homopolymer SPI produced maximum power densities of 100 and 70 mW cm−2 respectively. Malik et al. [211] prepared a SPEEK/ethylene glycol/ionic liquid composite membrane for high temperature application. The ethylene glycol was added to use as a crosslinker to help alleviate the quantity of leaching. The composite membranes had a high thermal stability, with the sulphonic groups beginning to degrade at 240 ◦C. The composite membranes had a lower leaching weight loss in comparison to the non-crosslinked membranes, however the proton conductivity of the crosslinked membranes was lower. The authors explained that some of the sulphonic groups where used in the crosslinking resulting in lower conductivity. From the above analysis of the literature, it can be seen that membrane fillers are very versatile, in terms of chemical structure, size, dimensions, etc. Numerous different characteristics to adapt to specific application whether that is operating at high temperature, low relative humidity, increasing mechanical strength, preventing acid leaching, increasing proton conductivity, or producing self-humidifying membranes. On top of that they can also be functionalised to either boost these characteristics or provide a secondary functionality. The abovementioned studies indicate promising performance for composite membranes; however, highlight the need for further research to improve the lifetime and durability of these membranes. Table 3. summarises hydrogen PEM performance of composite polymer electrolyte membrane described in this review. Table 3. Summary of hydrogen PEMFC best performance using composite membranes. Membrane Nafion/Silica [144] Nafion/Silica particles [139] Nafion/Hafnium oxide [147] Nafion/Titanium oxide [152] Nafion/Titanium oxide nanotubes [156] Nafion/Zirconium oxide [141] Nafion/Sulphonated zirconium oxide [142] Nafion/mesoporous zirconium pshosphate [146] Nafion/ zirconium pshosphate [145] Nafion/GO [179] Nafion/SGO [180] Nafion/GO/TiO2 [183] Nafion/GO/Phosphotungstic acid [184] Nafion/Phosphotungstic acid [202] PBI [169] PBI/SiO2 [169] PBI/GO [190] PBI/SGO [191] SulfonatedPolysulfone [160] SPolysulfone/titanium oxide [160] SPEEK [164] SPEEK/GO [188] SPEEK/silica [164] SPI/ionic liquid [210] SPI/demaTfO [208] Power Density (mW cm−2) 350 380 336 514 1020 400 609 353 450 212 300 324 841 220 200240 388 600 160 240 179 378 246 100 100 Temperature (◦C) RH% 100 100 85 100 100 - 110 - 80 - 130 85 70 83 70 18 130 - 100 25 70 20 0 80 20 120 - 165165 - 165 0 175 0 85 - 85 - 120 - 80 30 120 - 120 0 80 0 Membranes with fillers that were functionalised (most commonly with sulphonic groups) displayed a better performance in terms of proton conductivity and cell polarisation at elevated temperatures. This is attributed to the water retaining capabilities of these functional groups. Different fillers demonstrated different performances, and this is because of their chemical structure in addition to theirPDF Image | Composite Polymers for Electrolyte Membrane Technologies
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