A lung-inspired approach is employed to overcome reactant homogeneity issues in polymer electrolyte fuel cells. The fractal geometry of the lung is used as the model to design flow-fields of different branching generations, resulting in uniform reactant distribution across the electrodes and minimum entropy production of the whole system. 3D printed, lung-inspired flow field based PEFCs with N = 4 generations outperform the conventional serpentine flow field designs at 50% and 75% RH, exhibiting a B20% and B30% increase in performance (at current densities higher than 0.8 A cm Broader contextFlow-field design is crucial to fuel cell performance, since non-uniform transport of species to and from the membrane-electrode assembly results in significant power losses. The long channels of conventional, serpentine flow fields cause large pressure drops between inlets and outlets, thus large parasitic energy losses and low fuel cell performance. This issue is exacerbated for small, portable fuel cells, where the power required for fluid transport should be minimal. To ensure uniform distribution of reactants across the electrode and a low pressure drop, we use a nature-inspired design that is rooted in thermodynamic and mechanical fundamentals, rather than biomimicry in a narrow sense. Inspiration is derived from the structure of the human lung, which ensures uniform gas distribution via an optimized fractal structure linking bronchi to alveoli, and realizing a remarkable combination of minimal entropy production, low pressure drop, and scale-invariant operation. Our 3D-printed, conducting flow-field plates maintain these unique characteristics of the lung, resulting in improved fuel cell performance over conventional serpentine flow-field based fuel cells. Uniformity in reactant distribution and minimal pressure drop are retained during scale-up, demonstrating the robustness of the proposed nature-inspired approach across length scales.

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a Mass transport can significantly limit the rate of reaction and lead to concentration polarisation in electrochemical devices, especially under the conditions of high operating current density. In this study we investigate hierarchically structured micro-tubular solid oxide fuel cells (MT-SOFC) fabricated by a phase inversion technique and quantitatively assess the mass transport and electrochemical performance improvement compared to a conventional tubular SOFC. We present pioneering work to characterise the effective mass transport parameters for the hierarchically porous microstructures by an integrated computed fluid dynamics simulation, assisted by multi-length scale 3D X-ray tomography. This has been historically challenging because either imaging resolution or field of view has to be sacrificed to compensate for the wide pore size distribution, which supports different transport mechanisms, especially Knudsen flow. Results show that the incorporation of radially-grown micro-channels helps to decrease the tortuosity factor by approximately 50% compared to the conventional design consisting of a spongelike structure, and the permeability is also improved by two orders of magnitude. When accounting for the influence of Knudsen diffusion, the molecule/wall collisions yield an increase of the tortuosity factor from 11.5 (continuum flow) to 23.4 (Knudsen flow), but the addition of micro-channels helps to reduce it down to 5.3. Electrochemical performance simulations using the measured microstructural and mass transport parameters show good agreement with the experimental results at elevated temperatures. The MT-SOFC anode displays 70% lower concentration overpotential, 60% higher power density (0.98 vs. 0.61 W cm À2 ) and wider current density window for maximum power density than the conventional design. Broader contextHierarchical materials are a popular choice not only for electrochemical energy devices such as fuel cells and batteries, but also for a range of functional materials including catalysts, diffusion media and membranes for waste processing. This study qualitatively and quantitatively illustrates the effectiveness of hierarchically structured pores in reducing gas transport resistance, providing new insights into advanced microstructure optimisation. Moreover, it is a common mistake in the modelling of hierarchical materials to assume the flow to be governed by continuum physics irrespective of the length scale, whereas in the region of finest structure, the molecule/wall collisions become dominant, which cannot be addressed by continuum physics. It is also impossible to define a relevant average pore size to describe the mass transport in these materials due to the wide pore size distribution. The integrated computed fluid dynamics (I-CFD) technique proposed by us for the first time herein, aims to overcome this problem and accurately characterise the effective mass transport in these complex hierarchical structures. The concept and techniques used in this study are believed to be of wide inter...

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The porous transport layer (PTL) in polymer electrolyte membrane water electrolysers (PEMWEs) has the multiple roles of delivering water to the electro-catalyst, removal of product gas, and acts as a conduit for electronic and thermal transport. They are, thus, a critical component for optimized performance, especially at high current density operation. This study examines the relationship between the microstructure and corresponding electrochemical performance of commonly used titanium sinter PTLs. Four PTLs, with mean pore diameter (MPD) ranging from 16 µm to 90 μm, were characterized ex-situ using scanning electron microscopy and X-ray computed micro-tomography to determine key structural properties. The performance of these PTLs was studied operando using polarization and electrochemical impedance spectroscopy. Results showed that an increase in mean pore size of the PTLs correlates to an increase in the spread and multimodality of the pore size distribution and a reduction in homogeneity of porosity distribution. Electrochemical measurements reveal a strong correlation of mean pore size of the PTLs with performance. Smaller pore PTLs showed lower Ohmic resistance but higher mass transport resistance at high current density of 3.0 A cm-2. A non-monotonic trend of mass transport resistance was observed for different PTLs, which suggests an optimal pore size beyond which the advantageous influence of macroporosity for mass transport is diminished. The results indicate that maximizing contact points between the PTL and the catalyst layer is the overriding factor in determining the overall performance. These results guide PTL design and fabrication of PEMWEs.

In-depth understanding of the dynamics of water formation, accumulation and removal is important for flow-field design optimization to ensure robust performance and durability of polymer electrolyte fuel cells (PEFCs). Here, in-operando neutron radiography is used to display and quantify liquid water distribution across the entire active area of single-, double-and quad-channel serpentine flow-fields. The results revealed that the water management and performance of PEFCs is strongly affected by the number of serpentine channels in the cathode flow-field. The single-channel serpentine-based PEFC exhibits both a better cell performance and uniformity in the local water distribution. The quad-channel based PEFC exhibits the largest voltage fluctuations caused by severe water flooding in the gas channels. However, the single-channel design leads to significantly larger pressure drop than the multiple-channel counterparts, which requires much higher parasitic power to pressurize and recirculate the reactants. Three different regimes of operation can be defined based on the current density: gradually increasing hydration (< 400 mA cm-2), flooding (400 mA cm-2 ≤ j ≤ 600 mA cm-2) and drying out (>600 mA cm-2). The reduced overall quantity of water in the channels with an increase in current density can be attributed to faster gas velocity and higher cell temperature.

Water dynamics in the membrane electrode assembly (MEA) and flow channels of polymer electrolyte fuel cells (PEFCs) is governed by the complex interplay of many physical and operational factors. The chemical nature and structure of the gas diffusion layer (GDL) plays a large part in this and is affected by the extent to which is mechanically compressed. Here, X-ray computed tomography shows the effect of cell compression on the MEA, and how it differs under the land and channel regions. Multi-orientation neutron radiography reveals the effect of compression on the way in which water accumulates and is transported between land and channel and between cathode and anode. By performing neutron imaging in both the inplane and through-plane directions it is possible to determine what constitutes a given 'thickness' of water mapped across the extent of an MEA. Changing MEA compression from 25% to 35% has a significant effect on water distribution and dynamics in operational cells. The effect of compression on performance is most marked in the mass transport region and there are consequences for liquid accumulation in channels and back-diffusion of water from the cathode to the anode.

Metal foam flow-fields have shown great potential in improving the uniformity of reactant distribution in polymer electrolyte fuel cells (PEFCs) by eliminating the 'land/channel' geometry of conventional designs. However, a detailed understanding of the water management in operational metal foam flow-field based PEFCs is limited. This study aims to provide the first clear evidence of how and where water is generated, accumulated and removed in the metal foam flow-field based PEFCs using in-operando neutron radiography, and correlate the water 'maps' with electrochemical performance and durability. Results show that the metal foam flow-field based PEFC has greater tolerance to dehydration at 1000 mA cm -2 , exhibiting a ~50% increase in voltage, ∼127% increase in total water mass and ~38% decrease in high frequency resistance (HFR) than serpentine flow-field design. Additionally, the metal foam flow-field promotes more uniform water distribution where the standard deviation of the liquid water thickness distribution across the entire cell active area is almost half that of the serpentine. These superior characteristics of metal foam flow-field result in greater than twice the maximum power density over serpentine flow-field. Optimizing fuel cell operating condition and foam microstructure would partly mitigate flooding in the metal foam flow-field based PEFC, which will form the basis of future work.