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Durable High Efficiency Membrane and Electrode Assemblies for Heavy Duty Fuel Cell Vehicles
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Durable High Efficiency Membrane and Electrode Assemblies for Heavy Duty Fuel Cell Vehicles
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Advanced Electrode Structures for Proton Exchange Membrane Fuel Cells: Current Status and Path Forward
Abstract Proton exchange membrane fuel cells (PEMFCs) have demonstrated their viability as a promising candidate for clean energy applications. However, performance of conventional PEMFC electrodes, especially the cathode electrode, suffers from low catalyst utilization and sluggish mass transport due to the randomly distributed components and tortuous transport pathways. Development of alternative architectures in which the electrode structure is controlled across a range of length scales provides a promising path toward overcoming these limitations. Here, we provide a comprehensive review of recent research and development of advanced electrode structures, organized by decreasing length-scale from the millimeter-scale to the nanometer-scale. Specifically, advanced electrode structures are categorized into five unique architectures for specific functions: (1) macro-patterned electrodes for enhanced macro-scale mass transport, (2) micro-patterned electrodes for enhanced micro-scale mass transport, (3) electrospun electrodes with fiber-based morphology for enhanced in-plane proton transport and through-plane O 2 transport, (4) enhanced-porosity electrodes for improved oxygen transport through selective inclusion of void space, and (5) catalyst film electrodes for elimination of carbon corrosion and ionomer poisoning. The PEMFC performance results achieved from each alternative electrode structure are presented and tabulated for comparison with conventional electrode architectures. Moreover, analysis of mechanisms by which new electrode structures can improve performance is presented and discussed. Finally, an overview of current limitations and future research needs is presented to guide the development of electrode structures for next generation PEMFCs. Graphical Abstract Development of improved electrode architectures with the control of structure on length scales ranging from millimeters to nanometers could enable a new generation of fuel cells with increased performance and reduced cost. This paper presents an in-depth review and critical analysis of recent developments and future outlook on the design of advanced electrode structures.
Atomically dispersed metal–nitrogen–carbon catalysts for fuel cells: advances in catalyst design, electrode performance, and durability improvement
The urgent need to address the high-cost issue of proton-exchange membrane fuel cell (PEMFC) technologies, particularly for transportation applications, drives the development of simultaneously highly active and durable platinum group metal-free (PGM-free) catalysts and electrodes. The past decade has witnessed remarkable progress in exploring PGM-free cathode catalysts for the oxygen reduction reaction (ORR) to overcome sluggish kinetics and catalyst instability in acids. Among others, scientists have identified the newly emerging atomically dispersed transition metal (M: Fe, Co, or/and Mn) and nitrogen co-doped carbon (M–N–C) catalysts as the most promising alternative to PGM catalysts. Here, we provide a comprehensive review of significant breakthroughs, remaining challenges, and perspectives regarding the M–N–C catalysts in terms of catalyst activity, stability, and membrane electrode assembly (MEA) performance. A variety of novel synthetic strategies demonstrated effectiveness in improving intrinsic activity, increasing active site density, and attaining optimal porous structures of catalysts. Rationally designing and engineering the coordination environment of single metal MN x sites and their local structures are crucial for enhancing intrinsic activity. Increasing the site density relies on the innovative strategies of restricting the migration and agglomeration of single metal sites into metallic clusters. Relevant understandings provide the correlations among the nature of active sites, nanostructures, and catalytic activity of M–N–C catalysts at the atomic scale through a combination of experimentation and theory. Current knowledge of the transferring catalytic properties of M–N–C catalysts to MEA performance is limited. Rationally designing morphologic features of M–N–C catalysts play a vital role in boosting electrode performance through exposing more accessible active sites, realizing uniform ionomer distribution, and facilitating mass/proton transports. We outline future research directions concerning the comprehensive evaluation of M–N–C catalysts in MEAs. The most considerable challenge of current M–N–C catalysts is the unsatisfied stability and rapid performance degradation in MEAs. Therefore, we further discuss practical methods and strategies to mitigate catalyst and electrode degradation, which is fundamentally essential to make M–N–C catalysts viable in PEMFC technologies.
Probing Anion Exchange Membrane Fuel Cell Cathodes by Varying Electrocatalysts and Electrode Processing
To date, several high-performing anion exchange membrane fuel cells (AEMFCs) have been demonstrated, but most these studies have focused on Pt containing cathodes with high loadings. Here, we explore and compare the performance and perform electrochemical diagnostics on three leading AEMFC cathode electrocatalysts: Pt/C, Ag/C, and Fe–N–C with electrodes that have been processed with either powder or dispersion-based ionomers using perfluorinated anion exchange polymers. Pt/C had the highest performance but also showed a strong dependence on ionomer type, with powder ionomer exhibiting much higher performance. These results were consistent with the observations for Ag/C but did not hold for the Fe–N–C catalyst where almost no change was observed between powder and dispersion-based ionomers. This is the first-time the impact of powder and dispersion ionomer with different classes of cathode electrocatalysts on the fuel cell performance have been compared, and the results have strong implications for the ability to achieve high performance at low loadings and for better understanding catalyst-ionomer interactions within AEMFCs.
Simultaneously improved reversibility and hydrogen production of solid oxide cells through infiltrating air electrode
Among the various fuel cells, solid oxide cells (SOCs) are the unique type that can principally operate reversibly as either fuel cells to produce electricity or as an electrolyser to split water and produce green hydrogen (H 2 ). Nevertheless, the SOCs' reversibility presents enormous challenges that are manifested by the fast degradation through the cycling between fuel cell and electrolysis mode. While the La 0.8 Sr 0.2 MnO 3 /yttria-stabilized zirconia (LSM/YSZ) air electrode possesses significant advantages in terms of high electrical conductivity and high thermal stability under fuel cell mode, the SOCs with the LSM/YSZ air electrode experience rapid performance degradation with catastrophic electrode delamination shortly after switching from fuel cell to electrolysis mode. To prevent such catastrophic delamination and enable the electrolysis H 2 production, a chemical solution with the designed chemistry of SrFe 2 O 4-d was infiltrated into the LSM/YSZ air electrode. The infiltration immediately mitigates the catastrophic delamination, and the infiltrated cells exhibit significantly improved reversibility upon the electrochemical operation. Nanostructure examination reveals nanoscale cracks and second-phase nanograins formed in the air electrode from the baseline cell. By contrast, no delamination was observed at either the micron or the nanoscale for the infiltrated cell, which is attributed to the increased ion conductivity of the Fe-doped LSM mixed conductor induced by the significant interdiffusion between the LSM backbone and infiltrates. Here, this study presents a viable method for preventing electrode delamination while enhancing the durability of H 2 production and power generation for reversible fuel cell/electrolysis cell operation. It further opens new research directions of modifying the electrochemical activity of the electrode of inherently functional cells through the infiltration of the solutions with different chemistry.
A robust protonic ceramic fuel cell with a triple conducting oxygen electrode under accelerated stress tests
Accelerated stress test of protonic ceramic fuel cells for evaluating the durability of materials and interfaces.
Highly-Accessible Catalysts for Durable High-Power Performance (Final Technical Report)
Reduction of costly Pt usage in proton exchange membrane fuel cell (PEMFC) electrodes is one of the major challenges towards development and commercialization of fuel cell electric vehicles (FCEV). However, reducing the Pt loading results in increasing local mass transport fluxes, and eventual performance loss, especially at high power. In this project, a team of 4 universities, 2 companies, and a national lab came together to develop fuel cell catalysts and electrodes with high performance and durability. The were several key concepts addressed in this project. The first concept is to develop a carbon support that possess internal porosity which are believed to enhance kinetic activity of the catalysts, and yet the pore morphology allows for good reactant transport. The second concept is to improve the Pt-electrolyte interface in hope to reduce the local transport resistance. This was done by using new ionomers and ionic liquids. The last concept involves improving the catalyst stability by introducing Pt alloy catalyst with ordered intermetallic phase. The collaborative platform provided by DOE funding enabled development of a highly active and durable catalyst with performance that exceeds previous catalysts and meets the DOE targets for light duty vehicle application.
High-Efficiency Solar-To-Fuel Photoelectrochemistry in Disordered Photonic Glass Electrodes (Final Technical Report)
This project investigated how photonic glass (PG) photoelectrodes—disordered arrangements of dielectric scatterers—can serve as scalable, tunable platforms for light trapping in photoelectrochemical (PEC) solar-to-fuel systems. By leveraging disorder-driven optical phenomena such as multiple scattering resonances and light localization, PG structures offer an alternative to conventional photonic crystals and inverse opals that require high structural precision. The scientific goals were to twofold: (1) develop approaches to predictive models for high performance PG electrodes based on light absorption simulations, and (2) fabricate, characterize, and optimize PG-based photoelectrodes for solar-to-hydrogen and solar-to-fuel photoelectrochemical applications. To overcome the complexity of ensemble optical simulations for disordered materials, the researchers developed a machine-learning-accelerated emulation of all configurations in the design space. With this approach, PG photoelectrodes based on a TiO2 semiconductor were designed to enhance PEC currents of up to one hundred times higher than the equivalent ultra-thin film photoanodes and several times higher than the equivalent photonic crystal. The research also explored integrated systems for electrochemical hydrogen production based on replacing water oxidation with the specific glycerol oxidation electrocatalysis. Overall, the project outlined an approach to a simple-to-fabricate photoelectrode system to drive photoelectrochemical reactions relevant to solar photochemical energy conversion.
Fabrication of high-performance gas-diffusion-electrode based membrane-electrode assemblies
This paper demonstrates the fabrication and processing steps required to produce high performance fuel cell membrane electrode assemblies (MEAs) based on spray-coated gas-diffusion electrodes (GDEs). It is demonstrated that coating the catalyst layer with a thin layer of ionomer and then hot pressing the GDEs to the membrane is required to achieve comparable catalyst activity and air performance to catalyst-coated-membrane MEAs. We show that there is a critical amount of ionomer required to achieve maximized performance. Using electron microscopy, we show that the combination of the ionomer overlayer and hot-pressing bonds the catalyst layer to the membrane, increasing the interfacial contact area and quality of this interface. We also find that the ionomer overlayer smooths the surface of the GDE and provides increased contact area between the GDE and the membrane. Additionally, we demonstrate that much less ionomer is required for high-performance than has been previously reported. Through model fitting of electrochemical impedance spectroscopy, we show that this improvement in the catalyst layer - membrane interface reduces the effective catalyst layer resistance, which reduces Ohmic losses and increases catalyst utilization.
Photo-driven growth of a monolayer of platinum spherical-nanocrowns uniformly coated on a membrane toward fuel cell applications
Membrane electrode assemblies (MEAs) serve as the core units of polymer electrolyte membrane fuel cells (PEMFCs) and are regularly fabricated by painting a slurry of commercial Pt/C onto a membrane, leading to thick and disordered electrocatalyst layers (CLs). Herein, we report a photo-driven fabrication of MEAs with ultra-thin and ordered CLs by growing a monolayer of dendritic platinum spherical nanocrowns onto each side of a photocatalyst-modified membrane. This approach allows us to control the thickness and platinum loading of ordered CLs by simply varying the concentration of the platinum precursor under tungsten light irradiation. The resultant MEAs exhibit an excellent fuel cell power density of 1.01 ± 0.05 W cm –2 at a platinum loading of 53 ± 1.5 μg cm cathode –2 . Furthermore, this exceptional activity likely arises from the nanostructured platinum crowns, efficient mass transport, and uniform reaction rate in the ultrathin (59 ± 12 nm thick) and ordered CLs according to electrochemical and theoretical investigations.
A redox-reversible A/B-site co-doped BaFeO 3 electrode for direct hydrocarbon solid oxide fuel cells
Solid oxide fuel cells (SOFCs) can directly convert the chemical energy in fuel to electrical energy with fuel flexibility; however, the conventional nickel-based anodes face great challenges due to coking upon direct oxidation of hydrocarbon fuels and redox instability. Thus, developing new anode materials which can provide high coking resistance as well as redox stability is crucial. In this work, Ba 0.6 La 0.4 Fe 0.8 Mo 0.1 Ni 0.1 O 3-δ (BLFMN) has been synthesized in air using a sol–gel combustion method, resulting in a dual phase consisting of a cubic BLFMN main phase and scheelite BaMoO 4 (BMO 4 ) secondary phase. By heat-treating the BLFMN dual phase in H 2 at 800 °C for 5 h, a metallic nanoparticle-decorated BLFMN triple phase compound comprising cubic BLFMN, cubic BaMoO 3 (BMO 3 ) and in situ exsolved FeNi 3 alloy was obtained. BLFMN was subsequently investigated as an electrode material for La 0.8 Sr 0.2 Ga 0.83 Mg 0.17 O 3-δ (LSGM) electrolyte (300 μm) supported SOFCs. Symmetrical cells using BLFMN as electrodes with the cell configuration of BLFMN//LSGM//BLFMN showed excellent redox reversibility and a peak power density (PPD) of 1.32 W cm -2 at 850 °C when using H 2 as fuel. Single cell with the cell configuration of BLFMN//LSGM//LSCF (La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3-δ ) reached PPD of 1.61 and 0.41 W cm -2 at 850 °C when operating with H 2 and CH 4 fuel, respectively. Moreover, the single cell exhibit excellent stability (over 300 h) upon direct oxidation of hydrocarbon fuels of CH 4 and C 3 H 8 . This study indicates that BLFMN is a promising redox reversible and coking resistant anode for SOFCs.
Rare Earth Nickelate Electrodes Containing Heavily Doped Ceria for Reversible Solid Oxide Fuel Cells
The electrochemical performance of composite rare-earth nickelate-rare-earth doped ceria oxygen electrodes, with a high level of rare-earth doping in ceria are reported. Additionally, the chemical stability of these compositions is reported at both the sintering (1240 ?C) and operating temperature (800 ?C). Specifically, a lanthanum nickelate La2NiO4+d (LNO) ?? 50 mol% lanthanum doped ceria (LDC50) oxygen electrode and a neodymium nickelate Nd2NiO4+d (NNO) ?? 50 mol% neodymium doped ceria (NDC50) oxygen electrode are tested in solid oxide fuel cell (SOFC) and solid oxide electrolysis cell (SOEC) modes and compared to a composite (La0.75Sr0.25)0.95MnO3±d (LSM)-8 mol% yttria stabilized zirconia (YSZ) electrode. The LNO–LDC50 oxygen electrode reaches a current density which is approximately three times that of the LSM-YSZ electrode in SOFC mode at 0.7 V and approximately two times the LSM-YSZ electrode at 1.2 V in SOEC mode. Similarly the NNONDC50 oxygen electrode reaches a current density which is approximately two times and approximately one and a half times that of LSM-YSZ at 0.7 V and 1.2 V respectively. Oxygen surface exchange results for LNO and NNO are also reported which show different oxygen exchange kinetics during oxidation versus reduction steps.
Theory Guided Fine‐Tune of Strain Effects in Pt Ternary Alloy via Rare Earth Templating: Achieving High Performance PEMFCs Catalysts
The sluggish kinetics and insufficient durability of platinum-based catalysts remain crucial barriers limiting proton-exchange-membrane fuel cells (PEMFCs) deployment. Here, we report a theory-guided synthesis combined with rare-earth templating to realize a previously inaccessible Pt 5 Co-like phase with tailored atomic-scale strain. Guided by density functional theory (DFT) calculations, we identified that a Pt 5 Co-like sublayer can induce a unique mild compressive strain (−1.24%) to the Pt(111) shell and an optimal *OH binding energy shift (ΔE ≈ 0.11 eV). This shift positions the alloy catalyst near the apex of the oxygen reduction reaction activity volcano. This prediction guided the synthesis of ternary alloy Pt 5 (Ce)Co@Pt multilayer nanoparticles, featuring a Ce-stabilized core, a Pt 5 Co-like sublayer, and a Pt-rich shell. This catalyst demonstrates both exceptionally high activity and durability, achieving a mass activity of 2.6 A∙mg Pt −1 in rotating disk electrode testing. In fuel cell membrane electrode assembly tests, Pt 5 (Ce)Co@Pt achieves a current density of 1.9 A∙cm −2 at 0.7 V under heavy-duty vehicle conditions. Remarkably, it maintains 1.2 A∙cm −2 after 1 80 000 AST cycles, doubling the U.S. DOE 2025 target. This work demonstrates a rational design strategy that DFT-guided strain engineering integrates with rare-earth templating to advance Pt-based catalysts for fuel cell applications.
Comparison of different chemical treatments of brush and flat carbon electrodes to improve performance of microbial fuel cells
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