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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

High-Platinum-Content Catalysts on Atomically Dispersed and Nitrogen Coordinated Single Manganese Site Carbons for Heavy-Duty Fuel Cells

Fuel cells for heavy-duty vehicles (HDVs) have attracted considerable attention because of their unique scalability, better fuel economy, the less demand for hydrogen refilling infrastructure. However, the potential application requires more stringent fuel cell durability up to 25,000 h. Membrane electrode assemblies (MEAs) made from platinum group metal (PGM) catalyst with relatively high loading 0.3 mgPt cm –2 play a crucial role in ensuring high-power and long-term durability. Integrating fine PGM nanoparticles and robust carbon support with strengthened interactions is critical for improving MEA performance and durability. Herein, a unique atomically dispersed and nitrogen coordinated single Mn site-rich carbon (M–N–C) support was developed for high content (40 wt%) platinum catalysts for the oxygen reduction reaction (ORR) cathode with reduced thickness. Compared with two controls studied in this work (e.g., a porous graphitic carbon-supported Pt and a commercial TKK Pt/C catalysts), the Pt (40 wt%)/Mn–N–C catalyst exhibited much enhanced catalytic activity and stability for the ORR in both aqueous acidic electrolyte and polymer electrolyte-based MEA. Here, we carefully elucidated the—role of the Mn–N–C support in promoting Pt catalyst concerning its high surface area, partially graphitic structure, and nitrogen dopants, providing better Pt nanoparticle dispersion, and strengthened interactions between Pt and carbon. Consequently, the MEA from the Pt (40 wt%)/Mn–N–C catalyst generated a 1.61 A cm –2 at 0.7 V based on HDV conditions (0.2 mgPt cm –2 and 250 kPa air). More importantly, the MEA is highly durable and can retain 1.31 A cm –2 at 0.7 V after 30,000 voltage cycles (~19% loss), surpassing the commercial Pt/C catalyst (loss of ~56%). Therefore, the Mn–N–C carbon-supported Pt catalyst holds a great promise to meet the challenging DOE target (1.07 A cm –2 at 0.7 V after 150,000 cycles) for HDVs.

25 ENERGY STORAGE↗
DOE OSTI2022

Fine Gradient Electrode and Micro Porous Layer Structures for Improved Heavy Duty Fuel Cells (Final Report)

The commercial deployment of Heavy Duty Fuel Cells(HDFC) for applications such as large trucks (for example, Class 8 capable of carrying 50,000 lb. loads) depends vitally on achieving high efficiency and durability at reasonable costs. Furthermore, the HDFC must operate under practical conditions such as with fuel and air impurities, multiple stop-start cycles, and under the extremes of climate our planet offers – from hot and cold to dry and wet. These conditions place a premium on the stability and utilization of the materials comprising the membrane electrode assemblies (MEAs) powering the fuel cell. and the current catalysts, MicroPorous Layers, and Electrode structures and additives are insufficient for these needs. In Phase I Pajarito and Advent will develop durable electrocatalysts, MicroPorous Layer and electrode additives, and electrode structures for heavy duty fuel cells designed for zero-emission long-haul trucking. The electrocatalyst products are designed to solve the challenging durability and performance needs of fuel cells designed for long life and high efficiency through a combination of uniquely structured designed catalysts as well as new MicroPorous Layers (MPLs) and electrode structure additives. These improved materials will provide Pajarito both an expanded commercial opportunity in electrocatalysts, as well as new markets for MPL and electrode additives. The resulting public benefits include improved economics of fuel cells, a leading zero-emission technology for mobility, as well as reduced reliance on the critical minerals and metals used in the heavy-duty trucks industry. Possible follow-up Phase II and III projects would add full MEA products based on the Phase I efforts catalysts and additives, with full system validation by leading Fuel Cell Truck developers.

08 HYDROGEN↗
DOE OSTI2020

Impact of Carbon Support Structure on the Durability of PtCo Electrocatalysts

High performing, low-Pt content fuel cell membrane electrode assemblies (MEAs) are critical to the economic viability of proton exchange membrane fuel cells (PEMFCs) for the transportation industry. Considerable research has been conducted to reduce the Pt content in fuel cells, leading to the development of transition metal alloys, such as Platinum-Cobalt (PtCo). The degree of degradation of PtCo catalysts can be impacted by the catalyst metal itself and its interactions with the carbon support. Several low-loaded PtCo MEAs were fabricated, with various combinations of porous and solid carbon cathode catalyst supports. The MEAs were subjected to an accelerated stress test (AST), and the catalyst degradation characterized using electrochemical, X-ray scattering, and electron microscopy techniques. Porous supports retain more of their electrochemically-active surface area (ECSA) and demonstrate higher performance after the AST. Overall, this is believed to be due to the ability of the porous supports to trap the metal particles within the pores, slowing their dissolution/precipitation, and agglomeration.

25 ENERGY STORAGE↗
DOE OSTI2021

Impact of Carbon Support Structure on the Durability of PtCo Electrocatalysts

High performing, low-Pt content fuel cell membrane electrode assemblies (MEAs) are critical to the economic viability of proton exchange membrane fuel cells (PEMFCs) for the transportation industry. Considerable research has been conducted to reduce the Pt content in fuel cells, leading to the development of transition metal alloys, such as Platinum-Cobalt (PtCo). The degree of degradation of PtCo catalysts can be impacted by not only the composition and morphology of the catalyst particle itself, but also its interactions with the carbon support. In this study several low-PtCo MEAs were fabricated, with various combinations of porous and solid carbon cathode catalyst supports. The MEAs were subjected to an accelerated stress test (AST), and the catalyst degradation characterized using electrochemical, X-ray scattering, and electron microscopy techniques. Porous supports retain more of their electrochemically-active surface area (ECSA) and demonstrate higher performance after the AST. This is believed to be due to the ability of the porous supports to trap the metal particles within the pores, slowing their dissolution/precipitation, and agglomeration. However porous supports also exhibit greater increases in transport resistance probably associated with enhanced Co leaching under the AST conditions.

25 ENERGY STORAGE↗
DOE OSTI2025

Visualizing degradation mechanisms in a gas-fed CO 2 reduction cell via operando X-ray tomography

We utilize operando X-ray computed tomography, coupled with real-time electrochemical analysis, to reveal the underlying failure mechanisms of membrane electrode assemblies (MEAs) for electrochemical CO 2 reduction (eCO 2 R). Through operando imaging, we can obtain unprecedented insights into the dynamic behavior of the MEA under different operating conditions, revealing critical changes in interface interactions, phase distribution, and structural integrity over time. Our findings identify phenomena giving rise to the transition from CO 2 R to the hydrogen evolution reaction (HER), as evidenced by shifts in cathode potential and CO 2 R selectivity. The formation of inhomogeneous precipitates at the gas diffusion electrode disrupts the CO 2 supply and reduces the active sites for eCO 2 R, resulting in a shift toward H2 production during low current density operation. Additionally, under high current density conditions, rapid water crossover up to the microporous layer/gas diffusion layer promotes the transition from CO 2 R to HER, further shifting cell potential toward anodic direction. Oscillating voltage conditions reveal the dissolution and regrowth of precipitates, providing direct visualization of the competing selectivity of CO 2 R and HER. This work offers new insight into the degradation mechanisms of MEAs, with implications for the design of more durable CO 2 R systems.

Lee, Sol A [California Institute of Technology (Ca↗
DOE OSTI2022

Elucidating the impact of the ionomer equivalent weight on a platinum group metal-free PEMFC cathode via oxygen limiting current

Leveraging the interactions between ionomer and catalyst can increase the performance of proton exchange membrane fuel cells. The impacts of the equivalent weight (EW) of perfluorosulfonic acid–based ionomers on the platinum group metal-free electrode structure and fuel cell performance have not been fully explored. Four membrane electrode assemblies (MEAs) were prepared by using a commercial Fe–N–C catalyst, two perfluorosulfonic acid ionomers with different EWs, that is, Aquivion 720 (A720) and Nafion 1100 (N1100), and two ionomer-to-catalyst (I/C) ratios. The four MEAs were characterized to understand the impact of the ionomer EW and content on the capacitance, proton conductivity, and mass transport on the cathode. The mass transport resistance was measured for the first time using a new oxygen reduction reaction limiting current method enabling to couple the effects of oxygen diffusion with liquid water generation. Low EW ionomer combined with a moderate I/C results in improved performance due to its enhanced proton conductivity. However, when used at high I/C, it can cause severe water flooding at high current density due to the enhanced liquid water uptake, especially at high relative humidity, resulting in lower catalyst utilization and higher mass transport resistance.

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

Modeling ammonia-fueled co-flow dual-channel protonic-ceramic fuel cells

This paper reports the model development for a dual-channel protonic-ceramic fuel cell (PCFC) operating on ammonia fuel. The model considers the coupled interactions of several physical and chemical processes, including three-dimensional heat conduction within the bipolar plates and the membrane-electrode assembly (MEA), one-dimensional flow within the fuel and air channels, detailed heterogeneous catalytic reactions within the porous composite anode structure, Butler–Volmer representation of the charge-transfer chemistry, and Nernst–Planck transport of three charged defects (protons, oxygen vacancies, and small polarons) within the dense electrolyte membrane. The membrane-electrode assembly is composed of a Ni-BCZYYb (BaCe 0.7 Zr 0.1 Y 0.1 Yb 0.1 O 3-δ ) anode, a BCZYYb electrolyte membrane, and a BCFZY (BaCo 0.4 Fe 0.4 Zr 0.1 Y 0.1 O 3-δ ) cathode. Chemical and physical parameters for the MEA model are established using previously published button-cell data. One aspect of the study is to investigate the partial ammonia decomposition upstream of the fuel cell. Such fuel cracking increases the H 2 content of the fuel entering the PCFC, which may have benefits. However, endothermic ammonia pyrolysis within the composite anode structure assists with thermal control of the cell. The dual-channel model can be considered as the unit cell of a full fuel-cell stack.

25 ENERGY STORAGE↗
DOE OSTI2023

Deformation and failure of the CrCoNi medium-entropy alloy subjected to extreme shock loading

The extraordinary work hardening ability and fracture toughness of the face-centered cubic (fcc) high-entropy alloys render them ideal candidates for many structural applications. Here, the deformation and failure mechanisms of an equiatomic CrCoNi medium-entropyalloy (MEA) were investigated by powerful laser-driven shock experiments. Multiscale characterization demonstrates that profuse planar defects including stacking faults, nanotwins, and hexagonal nanolamella were generated during shock compression, forming a three-dimensional network. During shock release, the MEA fractured by strong tensile deformation and numerous voids was observed in the vicinity of the fracture plane. High defect populations, nanorecrystallization, and amorphization were found adjacent to these areas of localized deformation. Molecular dynamics simulations corroborate the experimental results and suggest that deformation-induced defects formed before void nucleation govern the geometry of void growth and delay their coalescence. Our results indicate that the CrCoNi-based alloys are impact resistant, damage tolerant, and potentially suitable in applications under extreme conditions.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Countercurrent flow characteristics of next generation solvent in novel 3D printed columns for carbon capture

Solvent based absorption for carbon dioxide capture in a packed column is being considered as an efficient technology for the decarbonization process of point source. Significant efforts are underway to improve the design of packings with the cutting edge 3D printing technology for efficient carbon capture. Accordingly, multiphase flow studies were conducted to assess the performance of novel 3D printed columns with various triply periodic minimal surface (TPMS) designs. The effects of solvent properties, liquid and gas loads on the performance of TPMS columns are extensively explored. Hydrodynamics of the potential water-lean solvents (EEMPA) as well as aqueous monoethanolamine (MEA) solvent for carbon capture are evaluated and compared. The interfacial area and liquid holdup increase with increasing liquid loads (q L ) for TPMS columns. Schwarz column consistently shows the highest liquid holdup value. The EEMPA exhibits higher values for the interfacial area (10–15 %) and liquid holdup (~4 %) in comparison to the MEA. TPMS columns exhibit the intermediate value of dry pressure drop between the random and the structure packed columns. Among selected TPMS columns, the gyroid packing shows the lowest pressure drop. The gas load has marginal impact on the interfacial area at lower value while a higher gas load leads to column’s flooding. Prior to the flooding, the interfacial area in TMPS packings rises with increased gas load at a fixed liquid load except Schwarz packing where interfacial area is incentive to the gas load. Additionally, the liquid holdup and wet pressure drop rise as gas load increases in TPMS columns. Overall, Fisher Koch packing is more susceptible to flood as compared to other TPMS packings. Flow regimes: loading and flooding are also delineated in the TPMS packings.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Surface Decoration of Platinum Catalysts by ZrO 2– x Nanoclusters for Durable Fuel Cell Applications

Improving the activity and durability of carbon-supported platinum catalysts for the oxygen-reduction reaction (ORR) in acidic electrolytes is crucial to reducing the high overpotentials and power loss over time in proton-exchange membrane fuel cells (PEMFCs). We found that platinum nanoparticle catalyst deposited on an engineered carbon support in the presence of zirconium enabled higher ORR activity and 25% better retention in electrochemically active surface area (ECSA), thereby improving durability. The use of zirconium precursor in the carbon synthesis process led to the formation of atomically dispersed Zr and ZrO 2 nanoparticles on the support. Upon Pt deposition and subsequent heat treatment, the ZrO 2 particles preferentially rearranged on and around the platinum nanoparticles in a chemically reduced form as zirconium suboxide (ZrO 2-x ) surface-decorated nanoclusters, which mitigated Pt nanoparticle coarsening. Finally, analysis of the here-to-fore unknown catalyst structure as well as its performance and durability in a PEM fuel cell membrane electrode assembly (MEA) is discussed.

25 ENERGY STORAGE↗
DOE OSTI2022

Active and Durable PGM-free Cathodic Electrocatalysts for Fuel Cell Application

Platinum Group Metal-free (PGM-free) Oxygen Reduction Reaction (ORR) electrocatalysts possess high intrinsic activity measured by a Rotating Disk Electrode (RDE) method. However, under fuel cell operating conditions, PGM-free ORR electrocatalysts have underperformed compared to platinum catalysts. PGM-free ORR electrocatalyst’s fuel cell performance can be improved by designing and optimizing the cathodic catalyst layer (CL) and Membrane Electrode Assembly (MEA) construction such that: 1) it efficiently provides oxygen access to ORR active sites (through catalyst morphology control); 2) it removes water from the CL (by tuning the hydrophobicity of the PGM-free catalysts and the catalyst layer structure); and 3) it increases proton conductivity (by homogeneous mixing of catalysts and ionomer). Studying the CL is complex due to the absence of well-established protocols of MEA activation, especially compared to platinum-containing catalysts. PGM-free fuel cell testing protocols would need to optimize potentiostatic vs galvanostatic measurements, scan rates, parameters of Electrochemical Impedance Spectroscopy (EIS) and Beginning of Experiment (BOE) criteria. To make the PGM-free catalyst’s fuel cell performance comparable to platinum, the synergistic effort of materials design, fine tuning of the catalyst layer and comprehensive electrochemical analysis is required.

08 HYDROGEN↗
DOE OSTI2021

Recent developments in Pt–Co catalysts for proton-exchange membrane fuel cells

Development of Pt-based oxygen reduction reaction catalysts with high efficiency and high durability is central to the application of proton-exchange membrane fuel cell systems. Pt–Co bimetallic catalysts have drawn extensive attention owing to their capability of delivering high performance and long lifetime for fuel cell applications including light-duty and heavy-duty vehicles. However, further improvements in durability and performance are needed to meet market requirements. To fully exploit the potential of Pt–Co catalysts, new insights into the relationship between catalyst properties and fuel cell performance and durability are needed, and more effective methods to tailor the features of Pt–Co catalysts need to be developed. This review provides a summary and perspective on recent efforts, including work on customizing the Pt shell and Pt:Co ratio, tailoring the crystal structure, and improving carbon support properties, with a particular emphasis on mechanisms leading to enhancement of mass activity, power density, and durability in membrane electrode assembly testing.

25 ENERGY STORAGE↗
DOE OSTI2020

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.

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

A modified electrolyte non-random two-liquid model with analytical expression for excess enthalpy: Application to the MEA-H 2 O-CO 2 system

We report accurate thermodynamic properties of electrolyte systems are critical for the design and operation of many chemical processes. A comprehensive description of the thermodynamic framework for multi-electrolyte mixed solvent systems is presented, where the parameter structure of the symmetric electrolyte-Non-Random Two Liquid (e-NRTL) model is reformulated and a thermodynamically consistent and analytically derived formulation for the excess enthalpy is developed from the e-NRTL model. The refined parameter structure of the e-NRTL model avoids numerical singularities of the analytical formulation for the excess enthalpy in the absence of ionic species and extends the derived excess enthalpy formulation to non-electrolyte systems. The thermodynamic framework is demonstrated for the MEA-H 2 O-CO 2 case study using experimental data on thermodynamic quantities for the binary MEA-H 2 O system and the ternary MEA-H 2 O-CO 2 system. The model is implemented in Pyomo and will be available for release in the Institute for the Design of Advanced Energy Systems (IDAES) computational platform.

Monoethanolamine↗
DOE OSTI2025

A comparative TEA of a two-step process using chemical solvents for producing an ultra-sweet natural gas

Here, a comprehensive Techno-Economic Analysis (TEA) was performed to evaluate the economic feasibility of a novel two-step process (TSP) developed in Aspen Plus V12.1 to desulfurize and decarbonize a raw natural gas containing (2 mol% H 2 S and 5 mol% CO 2 ) into an ultra-sweet natural gas containing (1.72 ppmv H 2 S and 4.19 ppmv CO 2 ). The raw natural gas flow rate used in the TSP was 117.74 kg/s at 60 °C and 50 bar. The TSP combines an H 2 S desulfurization step using potassium carbonate (K 2 CO 3 ) and a CO 2 capture step using 3 different chemical solvents, monoethanolamine (MEA), sodium glycinate (SGS), and potassium glycinate (PGS). Both steps employ fixed-bed absorbers packed with Mellapak 250Y structured packing. The hydraulics and mass transfer characteristics for the TSP were calculated, indicating normal operation with higher gas-side (k G ) than liquid-side (k L ) mass transfer coefficients. The TEA of TSP indicated that PGS had the most promising economic feasibility among the 3 solvents as it exhibited the lowest Levelized Cost of CO 2 capture (LCOC) of $\$$47.54/ton.CO 2 at a Capital Expenditure (CAPEX) of $\$$24.98 million, and an Operating Expenditure (OPEX) of $\$$12.20 million/year. Also, the TSP could produce one MMSCF of ultra-sweet natural gas at a total cost of $\$$339.55.

03 NATURAL GAS↗
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↗
DOE OSTI2025

Constructing Highly Durable Fuel Cell Catalysts Through Integrating Graphitic Shell‐Protected Composite Carbon Support with Gaseous Co Deposition‐Driven PtCo Intermetallics

Metal dissolution, nanoparticle agglomeration, and carbon support corrosion cause significant performance degradation of current PtCo catalysts under acidic and oxidative oxygen reduction reaction. Here, in this study, an integrated strategy is presented to design high-performance Pt 3 Co intermetallic catalysts by regulating gaseous Co deposition-driven diffusion into Pt nanoparticles supported on a composite carbon. The composite carbon is derived from ZIF-8/polyaniline, consisting of a high-surface-area (HSC) core and a protective graphitic shell (GS), which is employed to design 40 wt.% Pt/HSC@GS catalyst. The corresponding membrane electrode assemblies (MEAs) can maintain 1.09 A cm −2 at 0.7 V (20. 7% loss) after 10 000 cycles (1.0–1.5 V for carbon stability) and 1.15 A cm −2 (16.1% loss) after 150 000 cycles (0.60–0.95 V for catalyst stability). A ordered Pt 3 Co intermetallic is synthesized via a gaseous Co-deposition process, which yields a homogeneous Co-rich layer onto the Pt nanoparticles on the composite support, thereby facilitating Co diffusion into Pt crystal during subsequent ordering annealing to form the ordered intermetallic structure. This gaseous deposition leads to a thin carbon layer on PtCo nanoparticles, inhibiting particle growth during the annealing and mitigating Co dissolution under dynamic electrochemical conditions. The PtCo catalyst achieves impressive MEA performance and long-term durability (1.45 A cm −2 at 0.7 V after 120 000 cycles) under heavy-duty conditions.

30 DIRECT ENERGY CONVERSION↗