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Molecules 2020, 25, 1712 10 of 44 The authors obtained the maximum power density of 62 mW cm−2 at 30 ◦C and 141 mW cm−2 at 70 ◦C after optimising the GO loading in the membrane (1% wt.) as depicted in Figure 2. Figure 2. Polarization curves of DMFC obtained for Nafion 112 and GO composite membranes at (a) 1M methanol at 30 ◦C and 70 ◦C and (b) 5M methanol at 30 ◦C; reproduced with permission from [98]. Moreover, at high methanol concentration, where methanol crossover becomes critical, benefits provided from the incorporation of graphene oxide were more evident: the composite membrane showed much higher power density, 3 times higher than Nafion (71 mW cm−2 vs 26 mW cm−2). Chien, et al. [99] prepared a composite membrane with sulphonated graphene oxide (SGO)/Nafion for DMFC to avoid the aggregation of GO in the polymer matrix. It was reported that proton conductivity increases with increasing amounts of SGO, as the SGO was distributed throughout the matrix and created more interconnected transfer channels. However, with further SGO amounts, aggregation began to predominate, thus reducing the conductivity of the composite membrane. Methanol permeability was shown to decrease in the presence of SGO as they block the methanol migration through the membrane. In DMFC test, the SGO/Nafion composite membrane exhibited higher current and power densities than commercial Nafion 115, for example; • in 1 M methanol solution, the current density and power density for the composite membrane at 0.4 V were 102.7 mA cm−2 and 42.9 mW cm−2, whereas the commercial Nafion 115 revealed only 78.6 mA cm−2 and 32.6 mW cm−2. • in 5 M methanol solution, the composite membrane showed values of 83.2 mA cm−2 (at 0.4 V) and 34.6 mW cm−2, which were better than the commercial membrane (54.1 mA cm−2 at 0.4 V and 22.1 mW cm−2). Additionally, the SGO/Nafion composite membrane had a lower catalyst activation loss than Nafion 115, which indicated that the composite membrane had lower methanol crossover and faster reaction kinetics. Yan et al. [100] proposed an innovative way to modify Nafion membrane by sandwiching a graphene oxide layer between two Nafion membranes. With the addition of a monolayer graphene film, methanol permeability decreased by 68.6% while observing only a marginal decrease in proton conductivity of 7% at 80 ◦C in comparison to pristine Nafion membrane. The authors tested the membrane in a DMFC varying methanol solution from 5 M to 15 M. Tests depicted that the graphene film allowed for a substantial performance improvement particularly when the passive DMFC was fed with high concentration methanol solutions enabling the passive DMFC to be operated at high concentrations. 2.2. Non-Perfluorinated Polymers Composite Membranes Non-fluorinated membranes seem to have a promising future for DMFCs as a replacement for the expensive fluorinated membranes that have high methanol and ruthenium crossover. Aromatic 1PDF Image | Composite Polymers for Electrolyte Membrane Technologies
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