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  1. A PEM fuel cell with a hydrophobically treated cathode catalyst layer (CL) demonstrates ∼220% peak power increase with humidified air at 70 °C. To understand the reasons of the increase, a mathematical model was developed focusing on the oxygen-water two-phase transport phenomena in the CL. It suggests the treatment affects the CL in two ways. First, the interface of the ionomer layer exposed to the gas pores becomes more hydrophobic, facilitating less liquid water coverage and faster water drainage from the CL and resulting in better performance at high current densities. Second, it also affects the hydration level in the ionomer phase resulting in higher oxygen concentration in the ionomer phase on and in the catalyst agglomerates, leading to higher performance over the whole polarization curve. The properties having significant influence on the model fitting the experimental data are the capillary pressure property of the CL, the hydrophobic ionomer ratio in the catalyst agglomerate, and the oxygen solubility/diffusivity in the Nafion® phases. With this experimentally verified model, additional case studies combining the hydrophobic gas diffusion material with the hydrophobic CL demonstrate that the membrane’s self-humidification (zero-net-water flux) and peak power enhancement (∼15%) can be reached simultaneously, providing direction for the future materials development.

     
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  2. Redox flow batteries (RFBs) are ideal for large-scale, long-duration energy storage applications. However, the limited solubility of most ions and compounds in aqueous and non-aqueous solvents (1M–1.5 M) restricts their use in the days-energy storage scenario, which necessitates a large volume of solution in the numerous tanks and the vast floorspace for these tanks, making the RFB systems costly. To resolve the low energy storage density issue, this work presents a novel way in which the reactants and products are stored in both solid and soluble forms and only the liquid with soluble ions is circulated through the batteries. Storing the active ions in solid form can greatly increase the storage energy density of the system. With a solid to liquid storage ratio of 2:1, for example, the energy density of the electrolyte of vanadium sulfate (VOSO4), an active compound used in the all-vanadium RFB, can be increased from 40 Ah l−1to 163 Ah l−1(>4X), allowing an existing 6-h RFB system to become a 24-h system with minimal modifications. To show how the concept works, an H2-V flow battery with a solid/liquid storage system is used, and its successful demonstration validates the solid-liquid storage concept.

     
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  3. Abstract

    A PEM fuel cell with the Nafion ionomer phase of the cathode catalyst layer (CL) that was exposed to hot dry gas during the hot‐pressing process showed improved performance over the whole current density range and ~ 220% peak power increase with humidified air at 80°C. This enhanced performance is attributed to the modified structure of the perfluorosulfonic acid (PFSA) ionomer layer in the CL during the MEA's hot‐pressing process. The dry gas exposure above the glass transition temperature (Tg) results in the aggregation of the ionic groups to retain the residue water molecules. This process separates the ionomer into ionic‐group‐rich domains and ionic‐group‐sparse domains. The ionic‐group‐sparse domains create hydrophobic interface and reactant transport channels with lower water content and thus higher oxygen solubility in the ionomer. Accordingly, the water‐unsaturated ionomer and its surface hydrophobicity enhance the kinetic‐controlled and concentration‐polarized regions of the fuel cell polarization curve, respectively. The surface hydrophobicity of the ionomer layer is analyzed by the contact angle measurement and XPS. The durability of the hydrophobic effect belowTgis demonstrated by boiling the treated material. Re‐treating the hydrophobic sample with humidified gas exposure aboveTgeventually exhibits hydrophilic features, further proving the manipulability of the ionic group distribution.

     
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  4. During high current density operation, water production in the polymer electrolyte membrane fuel cell (PEMFC) cathode catalyst layer can negatively affect performance by lowering mass transport of oxygen into the cathode. In this paper, a novel heat treatment process for controlling the ionic polymer/gas interface property of the fuel cell catalyst layer is investigated and then incorporated into the membrane electrode assembly (MEA) fabrication process. XPS characterization of the catalyst layer’s ionomer-gas interface at its outer surface and its sublayers’ surfaces obtained by scraping off successive layers of the catalyst layers confirms that a hydrophobic ionomer interface can be achieved across the catalyst layer using a specific heat treatment condition. Based on the results of the catalyst layer study, the MEA fabrication process is modified to identify heat treatment configuration and conditions that will create an optimal hydrophobic ionomer-gas interface inside the cathode catalyst layer. Finally, fuel cell tests conducted on the conventional and new MEAs under different operating temperatures show the performance of the fuel cells with the treated MEAs was > 130% higher than that with the conventional MEA at 25 °C and 70 °C with humidified air and > 45% higher at 70 °C with dry air. The durability of the hydrophobic treatment on the cathode catalyst layer ionomer is also confirmed by the accelerated stress test. 
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