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Abstract Wide–scale commercialisation of proton exchange membrane fuel cell (PEMFC) is hindered by the degradation of cathode catalyst and carbon support, making it crucial to understand these mechanisms. This study compares the cathode catalyst and carbon support degradations mechanisms using commercial gas diffusion electrode in operating PEMFCs. The impact of the accelerated stress tests (ASTs) is monitored by recording the polarisation, electrochemical surface area (ECSA) and mass activity. Furthermore, the electrochemical impedance spectroscopy (EIS) is monitored at seven operating points from 0.05 to 1 A cm−2. For both phenomena, the charge transfer resistance increases at high current densities, which is attributed to the losses in activity observed with the ECSA and the mass activity degradations. In the carbon–corroded PEMFC, the mass transport resistance first reduces by 45% (0–100 cycles), suggesting an increase in electrode porosity due to carbon corrosion. At a later stage (200–5000 cycles), the mass transport resistance increases by 225% as the electrode collapses. On the other hand, in the catalyst–degraded PEMFC, the mass transport resistance uniformly reduces while the charge transfer resistance increases by 30%. Altogether, EIS provides additional sensitivity to differentiate catalyst and carbon support degradation within PEMFCs.

Abstract In order to achieve a perfect bottom-up electroplated Cu filling with a minimal surface thickness, 2-mercaptopyridine (2-MP) was investigated as a new leveler for replacing Janus Green B (JGB) for bottom-up copper filling. Electrochemical impedence results indicate that 2-MP has a stronger suppression for Cu deposition than JGB. With the addition of 2-MP, the filling capability of the electroplating solution is improved significantly with the Cu thickness on surface decreasing from ∼16 μm to ∼10 μm. The interaction mechanisms of 2-MP, bis(3-sulfopropyl) disulfide (SPS), Cl − and tri-block copolymer of PEG and PPG with ethylene oxide terminal blocks (EPE) in the plating solution are studied by galvanostatic measurements (GMs). The acceleration effect of SPS and the inhibition effect of 2-MP on copper deposition occur in the presence of EPE, and the convection-dependent adsorption (CDA) behavior of additives usually occurs with the injection of four additives at optional concentrations. Further, it was found that when 1.0 ppm 2-MP, 1.0 ppm SPS and 200 ppm EPE were injected into the basic electrolyte, the potential difference ( Δ h) value of the electrolyte became positive, and the bottom-up electroplated copper filling was obtained in the electrolyte in absence of Cl − . The interaction mechanisms of three additives for bottom-up filling have been investigated by GMs.

AbstractProton exchange membrane fuel cells, consuming hydrogen and oxygen to generate clean electricity and water, suffer acute liquid water challenges. Accurate liquid water modelling is inherently challenging due to the multi-phase, multi-component, reactive dynamics within multi-scale, multi-layered porous media. In addition, currently inadequate imaging and modelling capabilities are limiting simulations to small areas (<1 mm2) or simplified architectures. Herein, an advancement in water modelling is achieved using X-ray micro-computed tomography, deep learned super-resolution, multi-label segmentation, and direct multi-phase simulation. The resulting image is the most resolved domain (16 mm2with 700 nm voxel resolution) and the largest direct multi-phase flow simulation of a fuel cell. This generalisable approach unveils multi-scale water clustering and transport mechanisms over large dry and flooded areas in the gas diffusion layer and flow fields, paving the way for next generation proton exchange membrane fuel cells with optimised structures and wettabilities.

Abstract Proton exchange membrane fuel cells (PEMFCs) are considered a significant player in the hydrogen economy. However, before mass production is possible, significant improvements in durability are necessary. Monitoring the changes in the electrode structure is challenging without a complex measurement apparatus. Precisely, the changes in electrode properties during carbon corrosion (increase in the porosity and electrode collapse) cannot be quantified using conventional electrochemical methods. Here, we report capturing the oxygen diffusivity in the PEMFC cathode catalyst layer using low-frequency electrochemical impedance spectroscopy (0.3-0.01 Hz). The low-frequency arc is fitted with resistance, inductance, and capacitance in parallel to represent the resistance to oxygen supply, inertia to oxygen diffusion, and oxygen storage capacity in the catalyst layer, respectively. Over 600 cycles of accelerated stress test (ASTs) of carbon corrosion, the capacitance increases by 25–45% (0–150 ASTs), indicating an increase in oxygen storage capacity and electrode porosity. Then, (150–600 ASTs) the resistance and inductance increase while the capacitance decreases by 80%, highlighting a decrease of the oxygen diffusivity and storage in the catalyst layer as the electrode collapses, which causes oxygen starvation. Altogether, this low-frequency approach correlates electrochemical impedance measurements with the changes in electrode structure during carbon corrosion.