Durability of Low Platinum Fuel Cells Operating at High Power Density

Abstract

Understanding and improving the durability of cost-competitive fuel cell stacks is imperative to successful deployment of the technology. Stacks will need to operate well beyond today’s state-of-the-art rated power density with very low platinum loading in order to achieve the cost targets set forth by DOE ($15/kW) and ultimately be competitive with incumbent technologies. An accelerated cost-reduction path presented by Nuvera focused on substantially increasing power density to address non-PGM material costs as well as platinum. The study developed a practical understanding of the degradation mechanisms impacting durability of fuel cells with low platinum loading (≤0.2mg/cm2) operating at high power density (≥1.0W/cm2) and worked out approaches for improving the durability of low-loaded, high-power stack designs. Of specific interest is the impact of combining low platinum loading with high power density operation, as this offers the best chance of achieving long-term cost targets. A design-of-experiments approach was utilized to reveal and quantify the sensitivity of durability-critical material properties to high current density at two levels of platinum loading (the more conventional 0.45 mgPt.cm–1 and the much lower 0.2 mgPt.cm–2) across several cell architectures. We studied the relevance of selected component accelerated stress tests (AST) to fuel cell operation in power producingmore » mode. New stress tests (NST) were designed to investigate the sensitivity to the addition of electrical current on the ASTs, along with combined humidity and load cycles and, eventually, relate to the combined city/highway drive cycle. Changes in the cathode electrochemical surface area (ECSA) and average oxygen partial pressure on the catalyst layer with aging under AST and NST protocols were compared based on the number of completed cycles. Studies showed elevated sensitivity of Pt growth to the potential limits and the initial particle size distribution. The ECSA loss was correlated with the upper potential limit in the cycle tests, although the performance degradation was found to be a strong function of initial Pt loading. A large fraction of the voltage degradation was found due to increased mass transfer overpotentials, especially in the lower Pt loading cells. Increased mass transfer overpotentials were responsible for a large fraction of the voltage degradation at high current densities. Analysis of the impedance and polarization data indicated O2 diffusion in the aged electrode ionomer to be the main source of the increased mass transfer overpotentials. Results from the experimental parametric studies were used to inform and calibrate newly developed durability model, simulating lifetime performance of the fuel cell under variety of load-cycle protocols, electrode loadings and throughout wide range of operating conditions, including elevated-to-3.0A/cm2 current densities. Complete durability model included several sub-models: platinum dissolution-and-growth as well as reaction-diffusion model of cathode electrode, applied sequentially to study the lifetime predictions of ECSA and polarization performance in the ASTs and NSTs. These models establish relations between changes in overpotentials, ECSA and oxygen mass transport in fuel cell cathodes. The model was calibrated using single cells with land-channel and open flowfield architectures. The model was validated against Nuvera Orion® (open flowfield) short stack data in the load cycle durability tests. The reaction-diffusion model was used to correlate the effective mass transfer coefficients for O2 diffusion in cathode ionomer and separately in gas pores with the operating conditions (pressure, temperature, gas velocity in flow field and current density), Pt loading, and ageing related growth in Pt particles and thinning of the electrode. Achievements of both modeling and experimental objectives were demonstrated in a full format, subscale stacks operating in a simulated but fully realistic ambient environment, using system-compatible operating protocols.« less