Stabilizing phosphotungstic acid in Nafion membrane via targeted silica fixation for high-temperature fuel cell application

With PWA as proton transfer and silica as water retainer, stable phosphotungstic acid/silica/Nafion (PWA/Si–N) composite membrane is non-destructively fabricated and exhibits excellent stability and high temperature proton conductivity. Compared with pristine Nafion, high temperature proton conductivity is significantly enhanced due to the collaboration between –SO₃H ionic clusters and the in-situ filled silica embedded PWA nanoparticles. PWA is stabilized in the ionic clusters via in-situ catalyzing the hydrolysis silica precursor targeted filled into the –SO₃H ionic clusters. Stable proton conductivity of the PWA/Si–N membrane at 110 °C and 60% RH is high to 0.058 S/cm, which is 2.4 folds of that of Nafion. At the same time, the composite membrane still maintains good mechanical and thermal stability. As a result, high temperature fuel cell performance of the composite membrane is improved by 41% compared with the pristine Nafion membrane. The in-situ coating method proved to be an effective method to solve the stability of PWA in Nafion membrane, especially the inorganic oxide with good hygroscopicity as the modifier.     

Nanofiber based hybrid sulfonated silica/P(VDF-TrFE) membranes for PEM fuel cells

In this study, novel nanofiber based-hybrid proton conducting membranes for polymer electrolyte membrane (PEM) fuel cells were fabricated via electrospinning method using sulfonated silica particles (S–SiO₂) as a functional additive. Here, poly(vinylidene fluoride-co-trifluoroethylene) (P(VDF-TrFE)) was used as the carrier polymer during electrospinning step for the fabrication of PEM fuel cell membrane structure for the first time in literature. The effect of electrospinning conditions, i.e. namely, solvent, carrier polymer, electrospinning voltage, relative humidity, and flow rate on the uniformity of the resultant electrospun mats, and the average fiber diameter, respectively, were investigated in detail. Furthermore, electrospinning was conducted with poly(vinylidene fluoride) (PVDF) as the carrier polymer to compare with (P(VDF-TrFE)) as well. S–SiO₂ particles were homogeneously distributed along the carrier polymer without any noticeable bead formation. After electrospinning, fiber mats were transformed into dense membranes via hot-pressing and subsequent Nafion® impregnation. After obtaining the densified membrane, proton conductivity, water uptake and mechanical strength of the hybrid membranes were examined and reported as well. Consequently, hybrid membrane with P(VDF-TrFE) carrier exhibited a superior proton conductivity (102 mS/cm) benchmarked with PVDF carrier polymer containing membrane (43 mS/cm) and solution casted Nafion® membrane (95 mS/cm) at the same conditions.     

The development of PTFE/Nafion/TEOS membranes for application in moderate and high temperature proton exchange membrane fuel cells

PTFE/Nafion (PN) and PTFE/Nafion/TEOS (PNS) membranes were fabricated for the application of moderate and high temperature proton exchange membrane fuel cells (PEMFCs), respectively. Membrane electrode assemblies (MEAs) were fabricated by PTFE/Nafion (and PTFE/Nafion/TEOS) membranes with commercially available low and high temperature gas diffusion electrodes (GDEs). The effects of relative humidity, operation temperature, and back pressure on the performance and durability test of the as-prepared MEAs were investigated. Incorporating TEOS into a PNS membrane and adding another layer of carbon onto a GDE would result in low membrane conductivity and low fuel cell performance respectively. However, in this work it is shown that HT-PNS MEAs demonstrate a higher performance than LT-PN MEAs in severe conditions - high temperature (118 °C) and low humidity (25% RH). The TEOS and additional carbon layer function as water retaining agents which are especially important for high temperature and low humidity conditions. The HT-PNS MEA showed good stability in a 50 h fuel cell test at high temperature, moderate relative humidity (50% RH) and back pressure of 14.7 psi.     

Experimental study on water transport in membrane humidifiers for polymer electrolyte membrane fuel cells

This paper presents an experimental setup for the measurement of water transfer in membrane humidifiers for automotive polymer electrolyte membrane (PEM) fuel cells at different process conditions. This setup was used to determine steady-state water permeation through perfluorinated sulfonic acid (PFSA)-based polymer membranes. The process conditions were varied within a relative humidity in the feed stream of RH = 30–90 %, absolute pressures of p = 1.25–2.5 bar, and temperatures of T = 320–360 K. The examined membranes are Nafion® membranes of different thicknesses (Nafion® 211, 212 and 115) and an experimental composite membrane manufactured by W. L. Gore & Associates. It was found that the overall water permeance is affected by both the mass transfer resistance of the membrane and the resistances in the boundary layers of the adjacent gas streams. The overall permeance is a strong function of water activity, with high levels of relative humidity showing the highest overall permeance. The absolute pressure only affects the overall permeance by affecting the diffusion in the boundary layers. Lower pressures are preferable for high overall water permeances. Increasing temperatures favor diffusion in the membrane and the boundary layers but lead to lower sorption into the membrane. The thicker Nafion® membranes show lower overall permeance at higher temperatures, while the overall permeance of the composite membrane shows no dependency on the temperature. Investigation of membrane humidifiers in counter-, co-, and cross-flow shows that the flow configuration in our setup has very little impact on the water flux in the humidifier.     

Fabrication and evaluation of Nafion nanocomposite membrane based on ZrO2–TiO2 binary nanoparticles as fuel cell MEA

Synthesis and characterization of nanocomposite membranes for proton exchange membrane fuel cell (PEMFC) operating at different temperatures and humidity were investigated in this study. Recast Nafion composite membrane with ZrO₂ and TiO₂ nanoparticles with 75 nm in mean size diameter, prepared for PEM fuel cells. Nafion/TiO₂ composite membranes have been also fabricated by in-situ sol–gel method. However, fine particles of the ZrO₂ were synthesized and Nafion/ZrO₂ composite membrane were produced by blending a 5% (w/w) Nafion-water dispersion with the inorganic compound. All nanocomposite membranes demonstrated higher water retention in comparison with unmodified membranes. Proton conductivity increased with increasing ZrO₂ content while TiO₂ additive (with mean size of 25 nm) enhanced water retention. Subsequently, structures of the membranes were investigated by Atomic Force Microscopy (AFM), Scanning Electron Microscopy (SEM) as well as X-Ray Diffraction (XRD). In addition, water uptake and proton conductivity of the modified membranes were also measured. The nanocomposite membrane was tested in a 25 cm² commercial single cell at the temperature range of 80–110 °C and in humidified H₂/O₂ under different relative humidity (RH) conditions. The membrane electrode assembly (MEA) prepared from Nafion/TiO₂, ZrO₂ presented highest PEM fuel cell performance in respect of I–V polarization under condition of 110 °C, 0.6 V and 30% RH and 1 atm.     

Sulfonated poly(arylene ether sulfone)s membranes with distinct microphase-separated morphology for PEMFCs

Copoly (arylene ether sulfone)s was employed for proton exchange membrane preparation via atom transfer radical polymerization followed by mild sulfonation, enhanced phase-separated morphology and favorable proton conductivity were achieved. The comprehensive ex-situ properties of a range of membranes with different ion exchange capacities were characterized alongside the fuel cell performances investigation. The membranes exhibit higher water uptake, which is beneficial to the proton conduction, compared to Nafion® 211 while maintaining similar swelling ratio. The prepared membranes exhibit reasonably high proton conductivity (0.16 S/cm at 85 °C) benefitting from the well-defined microstructure and high connectivity of the hydrophilic domains. Considering the comprehensive property, membrane with moderate ion exchange capacity (1.39 mmol/g) was employed to fabricate the membrane electrode assembly and peak power density of 0.65 W/cm² at 80 °C, 60% relative humidity was achieved for a H₂/O₂ fuel cell, these hydrocarbon membranes can therefore be implemented in PEMFCs.     

High-performance SO2-depolarized electrolysis cell using advanced polymer electrolyte membranes

Three different proton conducting polymeric membrane materials (Nafion® 115, Nafion® 212, and sulfonated Diels-Alder polyphenylene [SDAPP]) were evaluated for use in SO₂-depolarized electrolyzers for the production of hydrogen via the hybrid sulfur cycle. Their performance was measured using different water feed strategies to minimize overpotential losses while maintaining high product acid concentration. Both thin membranes (Nafion® 212 and SDAPP) showed performance superior to that of the thicker Nafion® 115. The SDAPP membrane electrode assembly (MEA) performed well at higher acid concentrations, maintaining low ohmic and kinetic overpotentials. Finally, short-term (100-h) stability tests under constant current conditions showed minimal degradation for the SDAPP and Nafion® 212 MEAs. SDAPP MEA performance approached the targets needed to make the hybrid sulfur cycle a competitive process for hydrogen production (product acid concentration ≥65 wt% H₂SO₄ at ≤ 0.6-V cell potential and ≥0.5 A-cm^?2 current density).     

Quantitative analysis of proton exchange membrane prepared by radiation-induced grafting on ultra-thin FEP film

Radiation-induced graft polymerization is introduced to effectively fabricate proton exchange membrane based on 12.5 μm fluorinated ethylene propylene (FEP) film. The graft side chains penetrate FEP film and distribute inside the bulk matrix evenly. The membranes exhibit hydrophilic/hydrophobic microphase-separated morphology as well as good thermal stability. The influences of irradiation parameters on the membrane property are investigated and the resulting membranes (named FEP-g-PSSA) exhibit excellent physicochemical properties. Membrane with 27.48% degree of graft and 130.1 mS cm^?1 proton conductivity is employed for fuel cell performance measurement. Under optimized operate conditions (80 °C, 75% relative humidity), the power density could reach up to 0.896 W cm^?2, inspiring for fuel cell application. The mass-transport-controlled polarization of membrane electrode assembly (MEA) based on FEP-g-PSSA membrane is higher than Nafion® 211 within the whole current density range and the gap is widening with increasing current density. At 2.0 A cm^?2, the mass transfer polarization of FEP-g-PSSA reaches up to 0.204 V, far higher than Nafion® 211 (0.084 V). By promoting the compatibility between the ionomer in the catalyst layer and FEP-g-PSSA membrane and optimizing the membrane/catalyst layer/gas diffusion layer interfaces, the fuel cell performance could be significantly enhanced, making the FEP-g-PSSA membranes promising in fuel cell application.     

Development of non-perfluorinated hybrid materials for single-cell proton exchange membrane fuel cells

Development of low temperature fuel cells that operate under 100 °C are needed to reduce the costs, to design a class of hybrid membranes and to construct various structures of membrane-electrode-assembles (MEAs) for proton exchange membrane fuel cells (PEMFC). In this work, PVA/PMA/SiO₂ hybrid composite membranes were synthesized and their conductivities were determined by impedance measurements. We found a maximum conductivity value of 4.2 × 10⁻³ S/cm at 80 °C and 100% relative humidity (RH). A fuel cell test evaluation for various MEAs was conducted by the potentiodynamic analysis and the current density values were determined from the current–voltage (I–V) curves. A maximum current density of 635 mA/cm² was obtained at 80 °C and 100% RH. To the best of our knowledge, this is the first time that a high current density of PVA-based electrolytes for PEMFCs operating at low temperature is reported. The structural characters were examined using of XRD and FTIR methods, and thermal properties were studied using DSC and TGA techniques and the results were discussed (cf. supplementation). The present study revealed that the single cell performance depends mainly on the temperature, relative humidity and chemical compositions of the membranes.     

Preparation and performance of nano silica/Nafion composite membrane for proton exchange membrane fuel cells

Composite membranes made from Nafion ionomer with nano phosphonic acid-functionalised silica and colloidal silica were prepared and evaluated for proton exchange membrane fuel cells (PEMFCs) operating at elevated temperature and low relative humidity (RH). The phosphonic acid-functionalised silica additive obtained from a sol–gel process was well incorporated into Nafion membrane. The particle size determined using transmission electron microscope (TEM) had a narrow distribution with an average value of approximately 11 nm and a standard deviation of ±4 nm. The phosphonic acid-functionalised silica additive enhanced proton conductivity and water retention by introducing both acidic groups and porous silica. The proton conductivity of the composite membrane with the acid-functionalised silica was 0.026 S cm⁻¹, 24% higher than that of the unmodified Nafion membrane at 85 °C and 50% RH. Compared with the Nafion membrane, the phosphonic acid-functionalised silica (10% loading level) composite membrane exhibited 60 mV higher fuel cell performance at 1 A cm⁻², 95 °C and 35% RH, and 80 mV higher at 0.8 A cm⁻², 120 °C and 35% RH. The fuel cell performance of composite membrane made with 6% colloidal silica without acidic group was also higher than unmodified Nafion membrane, however, its performance was lower than the acid-functionalised silica additive composite membrane.     

Understanding of temperature-dependent performance of short-side-chain perfluorosulfonic acid electrolyte and reinforced composite membrane

The short-side-chain (SSC) perfluorosulfonic acid (PFSA) membranes are important candidates as membrane electrolytes applied for high temperature or low relative humidity (RH) proton exchange membrane fuel cells. In this paper, the fuel cell performance, proton conductivity, proton mobility, and water vapor absorption of SSC PFSA electrolytes and the reinforced SSC PFSA/PTFE composite membrane are investigated with respect to temperature. The pristine SSC PFSA membrane and reinforced SSC composite membrane show better fuel cell performance and proton conductivity, especially at high temperature and low relative humidity conditions, compared to the long-side-chain (LSC) Nafion membrane. Under the same condition, the proton mobility of SSC PFSA membranes is lower than that of the LSC PFSA membrane. The water vapor uptake values for Nafion 211 membrane, pristine SSC PFSA membrane and SSC PFSA/PTFE composite membrane are 9.62, 11.13, and 11.53 respectively at 40 °C and they increase to 9.89, 12.55 and 13.09 respectively at 120 °C. The high water content of SSC PFSA membrane makes it maintain high performance even at elevated temperatures.     

Proton conductivity and performance in fuel cells of grafted membranes based on polymethylpentene with radiation-grafted crosslinked sulfonated polystyrene

In this work, a comparative study was carried out of the transport properties and performance in a hydrogen-air fuel cell of the membranes based on polymethylpentene (PMP) with grafted sulfonated polystyrene and the standard Nafion® 212 membrane. Grafted cation-exchange membranes (GCM) were obtained by radiation graft post-polymerization of styrene onto UV-exposed PMP film followed by sulfonation with chlorosulfonic acid. The proton-conductivity of the GCM membrane with an ion-exchange capacity of 2.9 ± 0.1 meq/g reaches 21 ± 1 mS cm^?1 at room temperature and 95% relative humidity, which is twice higher the conductivity of the Nafion® under the same conditions. The GCM-1 H₂-permeability of 2.06?10^?7 cm² s^?1 even slightly lower than that of the Nafion® 212 (2.14?10^?7 cm² s^?1). A comparison of these membranes in the membrane electrode assemblies (MEA) of hydrogen-air fuel cells (FC) shows that the use of the grafted membranes with the high ion-exchange capacity is highly promising. The maximum performance of FC with grafted and Nafion® 212 membrane are both close to 180 mW/cm² at the current density of 400 mA/cm². At the same time, the high degree of crosslinking of sulfonated polystyrene leads to a decrease in conductivity and does not give an advantage in gas permeability.     

Effects of inlet relative humidity (RH) on the performance of a high temperature-proton exchange membrane fuel cell (HT-PEMFC)

A high temperature-proton exchange membrane fuel cells (HT-PEMFC) based on phosphoric acid (PA)-doped polybenzimidazole (PBI) membrane is able to operate at elevated temperature ranging from 100 to 200 °C. Therefore, it is evident that the relative humidity (RH) of gases within a HT-PEMFC must be minimal owing to its high operating temperature range. However, it has been continuously reported in the literature that a HT-PEMFC performs better under higher inlet RH conditions. In this study, inlet RH dependence on the performance of a HT-PEMFC is precisely studied by numerical HT-PEMFC simulations. Assuming phase equilibrium between membrane and gas phases, we newly develop a membrane water transport model for HT-PEMFCs and incorporate it into a three-dimensional (3-D) HT-PEMFC model developed in our previous study. The water diffusion coefficient in the membrane is considered as an adjustable parameter to fit the experimental water transport data. In addition, the expression of proton conductivity for PA-doped PBI membranes given in the literature is modified to be suitable for commercial PBI membranes with high PA doping levels such as those used in Celtec^® MEAs. Although the comparison between simulations and experiments shows a lack of agreement quantitatively, the model successfully captures the experimental trends, showing quantitative influence of inlet RH on membrane water flux, ohmic resistance, and cell performance during various HT-PEMFC operations.     

Proton exchange membrane water electrolysis at high current densities: Investigation of thermal limitations

In this work the thermal limitations of high current density proton exchange membrane water electrolysis are investigated by the use of a one dimensional model. The model encompasses in-cell heat transport from the membrane electrode assembly to the flow field channels. It is validated by in-situ temperature measurements using thin bare wire thermocouples integrated into the membrane electrode assemblies based on Nafion® 117 membranes in a 5 cm² cell setup. Heat conductivities of the porous transport layers, titanium sinter metal and carbon paper, between membrane electrode assembly and flow fields are measured in the relevant operating temperature range of 40 °C – 90 °C for application in the model. Additionally, high current density experiments up to 25 A/cm² are conducted with Nafion® 117, Nafion® 212 and Nafion® XL based membrane electrode assemblies. Experimental results are in agreement with the heat transport model. It is shown that for anode-only water circulation, water flows around 25 ml/(min cm²) are necessary for an effective heat removal in steady state operation at 10 A/cm², 80 °C water inlet temperature and 90 °C maximum membrane electrode assembly temperature. The measured cell voltage at this current density is 2,05 V which corresponds to a cell efficiency of 61 % based on lower heating value. Operation at these high current densities results in three to ten-fold higher power density compared to current state of the art proton exchange membrane water electrolysers. This would drastically lower the material usage and the capital expenditures for the electrolysis cell stack.     

Multi-functionalized acid-base double-shell nanotubes are incorporated into the proton exchange membrane to cope with low humidity conditions

Proton exchange membranes (PEM) with high proton conductivity and water retention are critical to the commercial application of proton exchange membrane fuel cells (PEMFC). In this study, acid-base double-shell nanotubes with carboxylate inner shell and an imidazole outer shell (DSNT-A@B) are synthesized via continuous distillation-precipitation polymerization using halloysite nanotubes (HNTs) as seeds. Then, it is incorporated into sulfonated poly (ether ether ketone) matrix to prepare composite membranes. The carboxylic inner shell can increase the content of combined water, thereby giving the composite membrane higher water retention. The imidazole shell acts as basic shell to create acid-base pairs with the membrane and inner shell to promote proton conductivity following the Grotthuss mechanism. The results show that when the blending amount is 5 wt%, the proton conductivity of the composite membrane reaches 0.336 S/cm at 80 °C and 100% relative humidity (RH), which is twice as high as that of the original membrane. In particular, the water loss of SPEEK/DSNT-A@B-10 composite membrane is only 54.55% at 40 °C and 20% RH, which is 32.77% lower than the SPEEK membrane. Therefore, this DSNT-A@B/SPEEK composite membrane can be used as a potential candidate for high temperature and low humidity fuel cells.     

Molecular sieve as an effective barrier for methanol crossover in direct methanol fuel cells

Methanol crossover is still a significant barrier to the commercialization of direct methanol fuel cells with wide-used Nafion® membrane. Herein, molecular sieve is introduced into the design of polymer electrolyte membrane to alleviate methanol crossover. The UZM-9 zeolite with an intermediate window size of 0.42 nm can effectively separate hydrated methanol (ca. 1.10 nm) and hydrated proton (ca. 0.23 nm). The methanol diffusion rate through the membrane is effectively suppressed after modified with UZM-9, which is about four times lower than the origin Nafion® membrane. The resulted peak power density reached 80 mW cm⁻² with 2 mol L⁻¹ methanol solution feed, which is 2.5-fold higher than that of direct methanol fuel cell with commercial Nafion® membrane. These results open a promising route to alleviate methanol crossover in direct methanol fuel cells.     

SCTF nanosheets@sulfonated poly (p-phenylene-co-aryl ether ketone) composite proton exchange membranes for passive direct methanol fuel cells

The development of a simple and efficient methanol-resistant membrane strategy is of great significance for improvement of the performance of fuel cells, making it an attractive and challenging topic. In this work, sulfonated covalent triazine framework (SCTF) nanosheets are prepared by a micro-interface method and post-sulfonation, which show excellent dispersion in polar solutions, such as water and N, N-Dimethylacetamide (DMAc). Then a series of composite proton exchange membranes (SCTF-x@SPP-co-PAEKs) are prepared by blending these SCTF nanosheets with sulfonated micro-block copolymers (SPP-co-PAEKs) resin. The results show that the appropriate addition of SCTF can significantly improve the proton conductivity (PC), methanol resistance and fuel cell performance of the prepared composite membrane, which can be attributed to the good interfacial compatibility between the SCTF nanosheets and the sulfonated micro-block copolymer matrix. The passive direct methanol fuel cells (DMFCs) with SCTF-x@SPP-3 membrane exhibit power density in the range of 28.0–33.3 mW cm⁻² at 25 °C, which is superior to the related values of the pristine membrane and the commercial Nafion® series membranes.     

Macromolecule sulfonated Poly(ether ether ketone) crosslinked poly(4,4′-diphenylether-5,5′-bibenzimidazole) proton exchange membranes: Broaden the temperature application range and enhanced mechanical properties

Proton exchange membranes with a wide application temperature range were fabricated to start high-temperature fuel cells under room temperature. The volume swelling stability, oxidative stability as well as mechanical properties of crosslinked membranes have been improved for covalently crosslinking poly(4,4′-diphenylether-5,5′-bibenzimidazole) (OPBI) with fluorine-terminated sulfonated poly(ether ether ketone) (F-SPEEK) via N-substitution reactions. High proton conductivity was simultaneously realized at both high (80–160 °C) and low (40–80 °C) temperatures by crosslinking and jointly constructing hydrophilic-hydrophobic channels. The crosslinked membranes exhibited the highest proton conductivity of 191 mS cm⁻¹ at 80 °C under 98% relative humidity (RH) and 38 mS cm⁻¹ at 160 °C under anhydrous, respectively. Compared with OPBI membrane, the fuel cell performance of the crosslinked membranes showed higher peak power density at full temperature range (40–160 °C).     

Empirical correlations for the performance of a PEFC considering relative humidity of fuel and oxidant gases

The growing energy demand and the impact of polluting gases lead to the necessity of alternative energy sources and conversion energy devices. Fuel cells (FCs) appears as a suitable solution for facing the mentioned issues. Predicting the behavior of a polymer electrolyte fuel cell (PEFC) under different conditions represents a proper initial step to solve the several issues, e.g., aging water balance problems, which occur inside the cell during the energy conversion process. Understanding microstructural impacts of the diffusion media, water management issues of FCs or the impacts of the inlet reactant gases to the cell represent some of the processes that have to be analyzed to improve the efficiency and behavior of FCs.The current study aims, based on experimentally collected data, to propose empirical correlations that describe and predict the performance of a PEFC. The single cell considered in this study corresponds to a single PEFC with a Nafion® 112 membrane as electrolyte and with an effective area of 25 cm². Relative humidity as a function of the reactive inlet gas temperature, as well as the power and the current density as a function of the cell/reactant gas temperature gradient are analyzed. In addition, correlations for power and current density as a function of the relative humidity (RH) have been proposed. Our correlations are obtained for an operating voltage of 0.6 V. It was shown a strong correlation between the power and current densities with the RH since the membrane conductivity depends mainly on the water content. The PEFC behavior was evaluated at different RHs. The results show big losses of operating power and current densities, as well as an increment of the resistance of the membrane when it operates at low RH.     

Enhanced transport properties of graphene‐based,thin Nafion® membrane for polymer electrolyte membrane fuel cells

A polymer electrolyte membrane fuel cell (PEMFC) is one of the promising renewable energy conversion systems; however, its performance is considerably limited by the sluggish transport properties and/or reaction kinetics of the catalyst layers, especially at a high current density. In this study, graphene‐based, thin Nafion® membranes are prepared using 0 to 4 wt% of graphene nanoflakes, and the effects of the graphene are examined for enhanced transport properties. The electrical conductivity and dielectric constant are drastically enhanced to 0.4 mS/cm and 26 at 4 wt% of graphene nanoflakes, respectively, while the thermal conductivity linearly increases to 3 W/m‐K. The proton conductivity also significantly increases with the aid of graphene nanoflakes at >2 wt% of graphene nanoflakes, and the enhancement doubles compared with those of the carbon‐black (CB)‐based and carbon nanotube (CNT)‐based, thin Nafion® membranes, perhaps due to unique graphene structures. Additionally, the quasi‐steady‐state water contact angle increases from 113° to ~130° with the addition of graphene nanoflakes, showing that a hydrophobic‐like water wetting change may be related to the significant proton conductivity enhancement. This work provides an optimal material design guideline for the transport‐enhanced cathode catalyst layer using graphene‐based materials for polymer electrolyte membrane fuel cell applications.