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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Design of Graded Cathode Catalyst Layers with Various Ionomers for Fuel Cell Application

Proton exchange membrane fuel cells (PEMFCs) powered by green hydrogen (H2) have become a promising alternative to conventional hydrocarbon-fueled power generators. Despite technological advancements, further improvements in efficiency, durability, and low-cost production are required for the widespread adoption of PEMFCs. Though numerous approaches to improve PEMFC electrodes have been reported, most strategies utilize a single material set (e.g., one combination of catalyst and ionomer) to improve performance. Alternatively, anisotropic (graded) electrode structures with locally tunable properties may yield superior electrode performance due to improved ionic and gas phase transport. In this work, graded cathode catalyst layers (CCLs) incorporating different ionomers (Nafion D2020, Aquivion D79-25BS, and HOPI) were designed and prepared. Performance screening shows that some of these graded electrode structures have comparable performance to optimized single-ionomer electrode structures (D2020) suggesting some synergistic benefit. Additionally, we show that electrodes with lower equivalent weight (EW) D79 ionomer near the membrane and D2020 ionomer near the gas diffusion media outperformed electrodes with the inverted configuration. Finally, EIS analysis shows some graded ionomer structures (e.g. D79/D2020) have better than expected H+ conductivity, generally leading to better electrode performance. However, further optimization of ionomer content and catalyst ink formulations is needed to improve overall PEMFC performance.

DIRECT ENERGY CONVERSION↗
NASA NTRS2005

Proton-Exchange-Membrane Fuel Cell Powerplants Developed and Tested for Exploration Missions

Proton-exchange-membrane fuel cell (PEMFC) technology has received major attention for terrestrial applications, such as the automotive and residential markets, for the past 20 years. This attention has significantly advanced the maturity of the technology, resulting in ever more compact, efficient, reliable, and inexpensive PEMFC designs. In comparison to the terrestrial operating environment, the space operating environment is much more demanding. Microgravity to high-gravity loads and the need to use pure oxygen (rather than air) as the fuel cell oxidizer place more stringent demands on PEMFC technology. NASA and its partners from industry are leveraging terrestrial PEMFC advancements by conducting parallel space technology development for future exploration missions. A team from the NASA Glenn Research Center, NASA Johnson Space Center, and NASA Kennedy Space Center recently completed the first phase of a PEMFC powerplant development effort for exploration missions. The industry partners for this phase of the development effort were ElectroChem, Inc., and Teledyne Energy Systems, Inc. Under contract to Glenn, both of these industry partners successfully designed, fabricated, and tested a breadboard PEMFC powerplant in the 1- to 5-kW power range. These powerplants were based on existing company-proprietary fuel cell stack designs, combined with off-the-shelf components, which formed the balance of the powerplant design. Subsequent to the contractor development efforts, both powerplants were independently tested at Johnson to verify operational and performance characteristics, and to determine suitability for further technology development in the second phase of the NASA-led effort. Following the independent NASA testing, Teledyne Energy Systems, Inc., was selected to develop an engineering model PEMFC powerplant. This effort was initiated by the 2nd Generation Reusable Launch Vehicle (RLV) Program Office in 2001; it transitioned to the Next Generation Launch Technologies (NGLT) Program Office in 2003. The effort is now being funded by the Exploration Program Office. We plan to summarize the results from the ongoing engineering model PEMFC powerplant development in a future Research & Technology article.

Hoberecht, Mark A.↗
DOE OSTI2020

Recent developments in catalyst-related PEM fuel cell durability

Cost and durability remain the two major barriers to the widespread commercialization of polymer electrolyte membrane fuel cell (PEMFC)-based power systems, especially for the most impactful but challenging fuel cell electric vehicle (FCEV) application. Commercial FCEVs are now on the road; however, their PEMFC systems do not meet the cost targets established by the U.S. Department of Energy, primarily due to the high platinum loading needed on the cathode to achieve the requisite performance and lifetime. Furthermore, while the activities of a number of commercial Pt-based alloy cathode catalysts exceed the beginning-of-life (BOL) targets, these activities, and the overall cathode performance, degrade via a variety of mechanisms described herein. Degradation is mitigated in current FCEVs by utilizing a cathode catalyst with a lower BOL activity (e.g., much lower transition metal alloy content and larger BOL nanoparticle size), necessitating higher catalyst loadings, and through the utilization of system controls that avoid conditions known to exacerbate degradation processes, such as limiting the fuel cell stack voltage range. The design and development of active and robust materials and eliminating the need for vehicle mitigation strategies would greatly simplify the operating system, allowing for greater transient operation, avoiding large hybridization, and curtailing of fuel cell power. Although system mitigation strategies have provided the near-term pathway for FCEV commercialization, material-specific solutions are required to further reduce costs and improve operability and efficiency. Future material developments should focus on stabilization of the electrode structure and minimization of the catalyst particle susceptibility to dissolution caused by oxide formation and reduction over PEMFC cathode-relevant operating potentials plus minimization of support corrosion. Ex situ accelerated stress tests have provided insight into the processes responsible for material and performance degradation and will continue to provide useful information on the relative stability of materials and benchmarks for robust and stable materials-based solutions not requiring system mitigation strategies to achieve adequate lifetime.

25 ENERGY STORAGE↗
DOE OSTI2020

Sensitivity Analysis and Effective Parametrization of PEM Fuel Cell Models

The cost of proton-exchange-membrane fuel cells (PEMFCs) remains a major hurdle in large-scale commercialization of this technology. To improve their performance and reduce cost, novel materials and electrode designs are continuously envisioned, e.g., non-PGM catalyst layers, ultra-thin Pt/Pt-Ni based catalyst layers, structured ionomer arrays or NSTF catalyst layers.1 Understanding the impact of these improvement strategies can be extremely time and cost intensive due to complex physical phenomena and large design space. We have previously developed a PEMFC modeling framework2 which has been a time and cost effective tool for understanding and optimizing the complex multi-physics phenomena within PEMFCs; however, several of the cell parameters used in the modeling have large spread in measured data.3 Furthermore, several transport parameters such as water adsorption kinetics have not been accurately measured and the approximations are spread over several orders of magnitude. These uncertainties cause problems in ascertaining accuracy of the modeling approach and they reduce the predictive power of the numerical models. The aim of this work is to identify the sensitivity of PEFC numerical model outputs to various input parameters. The previously in-house developed MEA modeling framework2 is used for PEMFC modeling. The sensitivity of the model outputs with respect to inputs parameters is obtained by analyzing the condition numbers for different output-input pairs at varying operating conditions. An example of the sensitivity analysis is shown in Figure 1. The condition numbers are obtained for the entire possible range of input parameters at varying operating conditions to identify the most crucial parameters of the PEMFC model. Based on our preliminary analysis, parameters related to kinetics (exchange current density and ECSA) and heat/water management in electrodes and ionomer (ionomer fraction, thermal conductivity) are most crucial. One of the major goals of this work is to identify the most crucial set of parameters towards which the model shows maximum sensitivity. This will guide future experimentalists to measure these properties with higher accuracy. Furthermore, the sensitivity analysis will also enable us to optimize the PEMFC performance by selectively targeting the most sensitive parameters and thereby making the largest impact. Acknowledgements The work is funded under the Fuel Cell Performance and Durability Consortium (FC-PAD), by the Fuel Cell Technologies Office (FCTO), Office of Energy Efficiency and Renewable Energy (EERE), of the U.S. Department of Energy under contract number DE-AC02-05CH11231. The authors would like to thank Nathan Craig at Robert Bosch LLC for his valuable input in designing the sensitivity analysis. The authors would also like to thank Giovanna Bucci and Matthias Hanauer at Robert Bosch for their valuable inputs and discussion. References P. K. Sinha, W. Gu, A. Kongkanand and E. Thompson, J. Electrochem. Soc., 158, B831 (2011). L. M. Pant, M. R. Gerhardt, N. Macauley, R. Mukundan, R. L. Borup and A. Z. Weber, Electrochim. Acta, 326, 134963 (2019). R. Vetter and J. O. Schumacher, ArXiv181110091 Phys. (2018). Figure 1

Pant, Lalit↗
NASA NTRS1993

A High Performance H2-Cl2 Fuel Cell for Space Power Applications

NASA has numerous airborne/spaceborne applications for which high power and energy density power sources are needed. The proton exchange membrane fuel cell (PEMFC) is an attractive candidate for such a power source. PEMFC's offer many advantages for airborne/spaceborne applications. They have high power and energy densities, convert fuel to electrical power with high efficiency at both part and full load, and can rapidly startup and shutdown. In addition, PEMFC's are lightweight and operate silently. A significant impediment to the attainment of very high power and energy densities by PEMFC's is their current exclusive reliance on oxygen as the oxidant. Conventional PEMFC's oxidize hydrogen at the anode and reduce oxygen at the cathode. The electrode kinetics of oxygen reduction are known to be highly irreversible, incurring large overpotential losses. In addition, the modest open circuit potential of 1.2V for the H2-O2 fuel cell is unattainable due to mixed potential effects at the oxygen electrode. Because of the high overpotential losses, cells using H2 and O2 are capable of achieving high current densities only at very low cell voltages, greatly curtailing their power output. Based on experimental work on chlorine reduction in a gas diffusion electrode, we believe significant increases in both the energy and power densities of PEMFC systems can be achieved by employing chlorine as an alternative oxidant.

Anderson, Everett B.↗
NASA NTRS2004

High Temperature Polymers for use in Fuel Cells

NASA Glenn Research Center (GRC) is currently working on polymers for fuel cell and lithium battery applications. The desire for more efficient, higher power density, and a lower environmental impact power sources has led to interest in proton exchanges membrane fuels cells (PEMFC) and lithium batteries. A PEMFC has many advantages as a power source. The fuel cell uses oxygen and hydrogen as reactants. The resulting products are electricity, heat, and water. The PEMFC consists of electrodes with a catalyst, and an electrolyte. The electrolyte is an ion-conducting polymer that transports protons from the anode to the cathode. Typically, a PEMFC is operated at a temperature of about 80 C. There is intense interest in developing a fuel cell membrane that can operate at higher temperatures in the range of 80 C- 120 C. Operating the he1 cell at higher temperatures increases the kinetics of the fuel cell reaction as well as decreasing the susceptibility of the catalyst to be poisoned by impurities. Currently, Nafion made by Dupont is the most widely used polymer membrane in PEMFC. Nafion does not function well above 80 C due to a significant decrease in the conductivity of the membrane from a loss of hydration. In addition to the loss of conductivity at high temperatures, the long term stability and relatively high cost of Nafion have stimulated many researches to find a substitute for Nafion. Lithium ion batteries are popular for use in portable electronic devices, such as laptop computers and mobile phones. The high power density of lithium batteries makes them ideal for the high power demand of today s advanced electronics. NASA is developing a solid polymer electrolyte that can be used for lithium batteries. Solid polymer electrolytes have many advantages over the current gel or liquid based systems that are used currently. Among these advantages are the potential for increased power density and design flexibility. Automobiles, computers, and cell phones require highly efficient power density for lowering emissions and meeting increasing consumer demands. Many of the solutions can be provided by proton exchange membrane fuel cells and lithium batteries. NASA Glenn Research Center has recognized this need, and is presently engaged in a solution. The goals for the summer include mastering synthesis techniques, understanding the reactions occurring during the synthesis, and characterizing the resulting polymer membranes using NMR, DSC, and TGA for the PEMFC and lithium batteries.

Peplowski, Katherine M.↗
DOE OSTI2020

Application of electrospinning for the fabrication of proton-exchange membrane fuel cell electrodes

We report electrospun materials have been gaining great interest in the energy sector. Their tunability and robustness make them highly attractive, particularly for proton-exchange membrane fuel cell (PEMFC) electrodes. Conventional PEMFC electrodes, prepared by either spraying, painting, or slot-die coating, have not yet met the needs of large-scale PEMFC use. Electrospinning of fibrous materials has already shown great promise as an alternative methodology for electrode fabrication. Electrospinning has been used in fuel cell electrodes through two primary means: (1) segmented carbon or inorganic fibers to serve as precious metal catalyst support, and (2) high aspect ratio polymer/particle fibers to serve directly as the electrode. The use of electrospun fibrous electrodes has led to improved PEMFC durability and increased power output at low catalyst loadings, both of which are of paramount importance to large-scale commercialization of PEMFC electric vehicles.

36 MATERIALS SCIENCE↗
DOE OSTI2022

PGM-Free Oxygen-Reduction Catalyst Development for Proton-Exchange Membrane Fuel Cells: Challenges, Solutions, and Promises

Proton-exchange membrane fuel cells (PEMFCs) are efficient and clean hydrogen energy technologies for transportation and stationary applications. Highly active and durable low-cost cathode catalysts for the oxygen-reduction reaction (ORR) under challenging acidic environments are desperately needed to address the cost and durability issues of PEMFCs. The most promising platinum group metal (PGM)-free catalysts for the ORR in acidic media are atomically dispersed and nitrogen-coordinated metal site catalysts denoted as M–N–C, M = Fe, Co, or Mn. Due to significant efforts in the past few decades, these catalysts have demonstrated much-improved ORR activity and promising initial fuel cell performance approaching traditional Pt/C catalysts. However, the insufficient long-term stability (up to 5000 h) under PEMFC operation represents a primary technical barrier to making current PGM-free catalysts less viable yet in PEMFCs. In this Account, we highlight recent advances in synthesizing efficient PGM-free catalysts for the ORR in PEMFCs, emphasizing effective strategies to improve mass and intrinsic activity and the possible degradation mechanisms. In particular, a chemical doping method based on the zeolitic imidazolate framework (ZIF)-8 represents the key to developing efficient M–N–C catalysts containing atomically dispersed and nitrogen-coordinated single metal active sites (i.e., MN 4 ). The newly acquired understanding of the formation mechanism of MN 4 active sites during the thermal activation and its correlation to catalytic properties guide the rational catalyst design rather than relying on current trial-and-error approaches. Considerable efforts have further been invested in increasing the active site density and enhancing intrinsic activity by regulating carbon-phase structures and the local coordination environment. Furthermore, these highly active catalysts usually suffer from significant activity loss during the ORR. Therefore, breaking the activity–stability trade-off is the key to simultaneously achieving activity and stability in one catalyst, which is discussed on the basis of our recent successes in regulating local carbon structures surrounding active single metal sites. Significant research efforts toward understanding the degradation mechanisms and improving the lifetime of PGM-free catalysts are still crucial for viable applications in the future. Novel electrode designing strategies are needed to translate the PGM-free catalysts’ ORR activity to solid-state electrolyte-based membrane electrode assemblies (MEAs) with robust three-phase (i.e., gas–liquid–solid) interfaces for efficient charge and mass transports for performance improvement. On the basis of our effort at the University at Buffalo supported by ElectroCat Consortium associated with U.S. DOE’s Hydrogen and Fuel Cell Technologies Office, we provide a perspective on PGM-free cathode catalysts concerning remaining bottlenecks and future opportunities, aiming to inspire the community in both mechanistic understanding and technological development.

08 HYDROGEN↗
DOE OSTI2022

Advanced Pt-Based Core–Shell Electrocatalysts for Fuel Cell Cathodes

Proton-exchange membrane fuel cells (PEMFCs) are highly efficient energy storage and conversion devices. Thus, the platinum group metal (PGM)-based catalysts which are the dominant choice for the PEMFCs have received extensive interest during the past couple of decades. However, the drawbacks in the existing PGM-based catalysts (i.e., high cost, slow kinetics, poor stability, etc.) still limit their applications in fuel cells. The Pt-based core–shell catalysts potentially alleviate these issues through the low Pt loading with the associated low cost and the high corrosion resistance and further improve the oxygen reduction reaction’s (ORR’s) activity and stability. This Account focuses on the synthetic strategies, catalytic mechanisms, factors influencing enhanced ORR performance, and applications in PEMFCs for the Pt-based core–shell catalysts. We first highlight the synthetic strategies for Pt-based core–shell catalysts including the galvanic displacement of an underpotentially deposited non-noble metal monolayer, thermal annealing, and dealloying methods, which can be scaled-up to meet the requirements of fuel cell operations. Subsequently, catalytic mechanisms such as the self-healing mechanism in the Pt monolayer on Pd core catalysts, the pinning effect of nitrogen (N) dopants in N-doped PtNi core–shell catalysts, and the ligand effect of the ordered intermetallic structure in L10-Pt/CoPt core–shell catalysts and their synergistic effects in N-doped L10-PtNi catalysts are described in detail. Additionally, the core–shell structure in the Pt-based catalysts have two main effects for enhanced ORR performance: (i) the interaction between Pt shells and core substrates can tune the electronic state of the surface Pt, thus boosting the ORR activity and stability, and (ii) the outer Pt shell with modest thickness can enhance the oxidation and dissolution resistance of the core, resulting in improved durability. We then review the recent attempts to optimize the ORR performance of the Pt-based core–shell catalysts by considering the shape, composition, surface orientation, and shell thickness. The factors influencing the ORR performance can be grouped into two categories: the effect of the core and the effect of the shell. In the former, PtM core–shell catalysts which use different non-PGM element cores (M) are summarized, and in the latter, Pt-based core–shell catalysts with different shell structures and compositions are described. The modifications of the core and/or shell structure can not only optimize the intermediate-binding energetics on the Pt surface through tuning the strain of the surface Pt, which increases the intrinsic activity and stability, but also offer a significantly decreased catalyst cost. Finally, we discuss the membrane electrode assembly performance of Pt-based core–shell catalysts in fuel cell cathodes and evaluate their potential in real PEMFCs for light-duty and heavy-duty vehicle applications. Even though some challenges to the activity and lifetime in the fuel cells remain, the Pt-based core–shell catalysts are expected to be promising for many practical PEMFC applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Multi-Scale Modeling of Hydrogen Transport in a Porous Fuel Cell Anode

Proton-exchange-membrane fuel cells (PEMFC) are a clean energy conversion alternative to traditional fossil-fuel combustion; however, transport resistances in the electrode pose a lower-limit to catalyst loading and commercialization of PEMFCs. PEMFCs consist of simultaneous hydrogen (H 2 ) oxidation and oxygen (O 2 ) reduction at the anode and cathode, respectively. Here, while oxygen transport resistances in PEMFCs have been widely studied both experimentally and analytically, hydrogen transport resistances are less understood. Herein, we present a physics-based model that encompasses multi-scale transport within the anode side of the PEMFC. The O 2 in the cathode here is omitted and replaced with H 2 to deconvolute O 2 transport resistance contributions, similar to that of a hydrogen pump. Replication of the hydrogen pump setup allows for comparison of the model against experimental analysis of H 2 gas-transport resistance in H 2 limiting-current experiments, which can also inform gas transport (including oxygen) in general. Herein, we present a multi-scale analytical model of the porous anode catalyst layers and individual catalyst agglomerates that enables determination of the effects of electrode morphology such as agglomerate size, catalyst loading, etc. on H 2 transport resistance through the porous electrode to complement and better understand H 2 limiting current experiments and deconvolute local H 2 transport resistances.

Zhang, Rosa↗
DOE OSTI2022

Unveiling the Degradation Nature of Pt/NbOx/C Catalysts for Oxygen Reduction Reaction via in situ X-ray Absorption Spectroscopy

Among various metal nanoparticles supported on metal oxide (MMO) catalysts, the Pt/NbOx/C system has promising oxygen reduction reaction (ORR) activity as cathode for proton exchange membrane fuel cells (PEMFCs). Herein, we study a series of Pt/NbOx/C catalysts with tunable structural and electronic properties via physical vapor deposition and unravel the nature of metal and metal oxide interaction (MMOI) by characterizing this system under reactive conditions. By conducting in situ X-ray absorption spectroscopy (XAS) experiments, we demonstrate the Pt preferably interacts with O but not Nb in the Pt/NbOx/C system and such Pt-O interaction benefits the ORR activity via electronic effect rather than strain effect. We also provide clear evidence for the formation of metallic Nb phase at the early stage of PEMFC operation and identify severe particle growth of Pt after long-term PEMFC operation. These findings deepen our understanding of the degradation mechanism of MMO catalysts during long-term PEMFC operation.

MMO catalyst↗
DOE OSTI2021

Recent Advances in Electrocatalysts for Proton Exchange Membrane Fuel Cells and Alkaline Membrane Fuel Cells

The rapid progress of proton exchange membrane fuel cells (PEMFCs) and alkaline exchange membrane fuel cells (AMFCs) has boosted the hydrogen economy concept via diverse energy applications in the past decades. For a holistic understanding of the development status of PEMFCs and AMFCs, recent advancements in electrocatalyst design and catalyst layer optimization, along with cell performance in terms of activity and durability in PEMFCs and AMFCs, are summarized in this report. The activity, stability, and fuel cell performance of different types of electrocatalysts for both oxygen reduction reaction and hydrogen oxidation reaction are discussed and compared. Research directions on the further development of active, stable, and low-cost electrocatalysts to meet the ultimate commercialization of PEMFCs and AMFCs are also discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Electrolyzer and Fuel Cell Recycling for a Circular Hydrogen Economy

Abstract Electrolyzers and fuel cells will be crucial for achieving global clean hydrogen and industrial decarbonization goals. However, the nascent clean hydrogen sector faces uncertainties around material supply chains and technology end‐of‐life management. This work aims to guide the transition to a circular hydrogen economy by using process modeling, techno‐economic analysis, and life cycle assessment to evaluate the material cost, energy use, greenhouse gas (GHG) emissions, toxicity, and water use of five potential recycling strategies for proton exchange membrane electrolyzers (PEMWE) and fuel cells (PEMFC). Hydrometallurgy, acid dissolution, and electrochemical dissolution are shown to offer 2–7 times improvement across all assessed metrics relative to the manufacturing of PEMWE and PEMFC from raw materials. Recycling can also lower the raw material demand, material cost, energy use, and GHG emissions associated with PEMWE and PEMFC deployment in the United States in 2050 by 23%, 19%, 21%, and 16%, respectively. This study provides key insights into the costs, benefits, and complexities of recycling strategies for PEMWE and PEMFC, aiding the development of a circular economy that is synergistic with clean hydrogen deployment.

08 HYDROGEN↗
DOE OSTI2024

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.

25 ENERGY STORAGE↗
DOE OSTI2026

Influence of Pt-Metal Alloy Catalysts with Various Ionomers on Oxygen Reduction Reaction in Fuel Cell Application

Pt-M/C (M = Co, Ni, Mn, etc.) alloy catalysts exhibit superior oxygen reduction reaction (ORR) activity compared to pure Pt/C, leading to a high energy efficiency in hydrogen fuel cells. However, many Pt-M/C alloy catalysts were synthesized and evaluated at the lab scale in model test-bed systems like rotating disc electrodes, which don't always correlate to performance within a fuel cell system; there is a clear need to evaluate catalysts in electrodes that can be prepared at industrially relevant scales to evaluate how factors like ink formulation can greatly affect device-level of fuel cell performance. Herein, three commercial Pt-M/C alloy catalysts (two Pt-Co/C and one Pt-Ni/C) were comprehensively characterized by various techniques. The results show that the average particle sizes of the three catalysts are close to 5 nm; the atomic ratio of Pt/M is around 4; and the M was successfully embedded into Pt lattice, resulting in the positive shift of Pt 4f in XPS spectra and XRD patterns. These catalytic materials were incorporated into 9 different cathode catalyst layers (CCLs) with three kinds of ionomers (Nafion D2020, high oxygen permeability ionomer (HOPI), and Aquivion D79-25BS), and their performance in proton exchange membrane fuel cells (PEMFCs) were investigated. The results demonstrate that the Pt-Co/C catalysts possess a higher mass activity (MA) than Pt-Ni/C; the cathodes with Nafion ionomer provide the highest MA while electrodes with Aquivion ionomer showed the lowest activity, attributed to poor H+ conductivity resulting from suboptimal ionomer incorporation. Finally, these alloys were shown to exceed DOE targets for MA and H2/Air performance reported in the recent publications at beginning of life and after 90k cycle catalyst AST protocol. This study provides valuable performance benchmarks for these materials guiding future Pt-M/C catalyst design and material integration for heavy duty PEMFC applications.

08 HYDROGEN↗
DOE OSTI2021

Mesoporous Textured Fe-N-C Electrocatalysts as Highly Efficient Cathodes for Proton Exchange Membrane Fuel Cells

A new platinum group metal (PGM)-free proton exchange membrane fuel cell (PEMFC) cathode catalyst materials, synthesized using the VariPore™ method by Pajarito Powder, LLC, are characterized for their structure and activity. The physico-chemical analysis of the iron-nitrogen-carbon (Fe-N-C) electrocatalysts show mesoporous carbon material effectively doped with iron and nitrogen. The materials have an average pore size of 7-8 nm and high specific surface area. The Fe-N-C catalysts exhibit good oxygen reduction reaction (ORR) activity in 0.5 M H2SO4 electrolyte with high half-wave potential and sustainable electrochemical stability over 10,000 repeated potential cycles with insignificant losses in their activities. As cathode catalysts in a PEMFC, the Fe-N-C materials deliver remarkably good fuel cell performance at low overpotential approaching that of the commercial Pt catalyst. The high ORR electrocatalytic activity of these Fe-N-C catalysts is credited to the synergy between nitrogen-moieties, specifically pyrrolic-N, pyridinic-N, and graphitic-N, and iron in addition to the high mesoporosity that facilitate an effective reaction path in boosting the electrocatalytic activity and stability.

DIRECT ENERGY CONVERSION↗
DOE OSTI2020

Mediated Fuel Cells: Soluble Redox Mediators and their Applications to Electrochemical Reduction of O2 and Oxidation of H2, Alcohols, Biomass, and Complex Fuels

Mediated fuel cells are electrochemical devices that produce power in a manner similar to that of conventional proton exchange membrane fuel cells (PEMFCs). They differ from PEMFCs in their use of redox mediators dissolved in liquid electrolyte to conduct oxidation of the fuel or reduction of the oxidant, typically O2, in bulk solution. The mediators transport electrons (and often protons) between the electrode and the catalysts or chemical reagents in solution. This strategy can help overcome many of the challenges associated with conventional fuel cells, including managing complex multi-phase reactions (as in O2 reduction) or the use of challenging or heterogeneous fuels, such as hydrocarbons, polyols and biomass. Mediators are also commonly used in enzymatic fuel cells, where direct electron transfer from the electrode to the enzymatic active site can be slow. This review provides a comprehensive survey of historical and recent mediated fuel cell efforts, including applications using chemical and enzymatic catalysts. Our research on in this field has been exploring a number of different topics and has been supported different funding sources: the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences (molecular mediators for catalytic oxygen reduction); the Great Lakes Bioenergy Research Center, DOE Office of Science DE-SC0018409 (research on biomass-based fuels; U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Program, DE-FG02-05ER15690 (copper-catalyzed oxidation reactions); and the NIH NIGMS, R01 GM100143 and R35 GM134929 (use of molecular mediators for organic chemical synthesis).

Anson, Colin W.↗
DOE OSTI2021

Characterization of a Sulfonated Poly(Ionic Liquid) Block Copolymer as an Ionomer for Proton Exchange Membrane Fuel Cells using Rotating Disk Electrode

Ionic liquid (IL) additives to both traditional and advanced oxygen reduction reaction (ORR) electrocatalysts have yielded remarkable improvements in catalyst performance and durability. However, incorporating ILs or IL-modified catalysts into the electrodes of a proton exchange membrane fuel cell (PEMFC) membrane electrode assembly (MEA) has proven to be challenging. Sulfonated poly(ionic liquid) block copolymers (S-PILBCP) present an opportunity to incorporate IL functionality directly into the ionomer, orthogonal to protonic conductivity. Here, we use a rotating disc electrode (RDE) to characterize the interface between a S-PILBCP and Pt catalyst in comparison to Nafion. Catalyst thin films prepared with S-PILBCP show an 80% improvement in the ORR activity over those containing Nafion. Thin films of S-PILBCP also show a significantly reduced degree of poisoning sulfonate adsorption on a Pt(111) surface in comparison to Nafion. Furthermore, these half-cell results provide useful insights that help to highlight the source of the impact of the S-PILBCP on PEMFC MEA performance.

25 ENERGY STORAGE↗