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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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At least 109 records · Page 6

Atomically dispersed Pt and Fe sites and Pt–Fe nanoparticles for durable proton exchange membrane fuel cells

Proton exchange membrane fuel cells convert hydrogen and oxygen into electricity without emissions. The high cost and low durability of Pt-based electrocatalysts for the oxygen reduction reaction hinder their wide application, and the development of non-precious metal electrocatalysts is limited by their low performance. Here we design a hybrid electrocatalyst that consists of atomically dispersed Pt and Fe single atoms and Pt–Fe alloy nanoparticles. Its Pt mass activity is 3.7 times higher than that of commercial Pt/C in a fuel cell. More importantly, the fuel cell with a low Pt loading in the cathode (0.015 mg Pt cm –2 ) shows an excellent durability, with a 97% activity retention after 100,000 cycles and no noticeable current drop at 0.6 V for over 200 hours. These results highlight the importance of the synergistic effects among active sites in hybrid electrocatalysts and provide an alternative way to design more active and durable low-Pt electrocatalysts for electrochemical devices.

25 ENERGY STORAGE↗

Efficient diffusion of superdense lithium via atomic channels for dendrite-free lithium–metal batteries

The non-uniform aggregation of fast-diffused Li on an anode surface would aggravate its tip-effect-induced nucleation/growth, leading to the notorious dendrite growth in Li metal batteries (LMBs). Tuning the Li diffusion on the anode surface has been regarded previously as a mainstream method to induce its uniform deposition, while the diffusion of Li in the anode bulk is usually ignored. In this study, conceptually different from the classic surface modification, we propose a molecular tunnelling strategy to construct atomic channels in graphite bulk, which enables the fast diffusion of superdense Li. Density functional theory calculations and ab initio molecular dynamics simulations prove that the bulk diffusion through atomic channels could become a new and dominating path. Its reversible and efficient diffusion has been further visualized by in situ transmission electron microscopy. As a result, when coupled with high-loading LiFePO 4 cathodes (20 mg cm –2 ), a high areal capacity and 100% capacity retention are achieved over 370 cycles. Through this work a new strategy is developed based on the bulk-diffusion of superdense Li for dendrite-free LMBs, which can be pervasive in other high-performance energy storage systems.

25 ENERGY STORAGE↗

Low Impedance Cathode/Electrolyte Interfaces for High Energy Density Solid-State Batteries

All-solid-state batteries (ASSBs) using a ceramic fast Li-ion conductor as a solid-state electrolyte (SSE) have been proposed as a promising strategy to significantly increase the energy density of lithium batteries. Due to their high ion conductivity and excellent stability, Li-stuffed garnets exhibit the most promising physical and chemical properties for SSEs. However, the typical microstructure, thick (>100 μm) bulk electrolyte and simple planar electrode/electrolyte interfaces, combined with poor electrode wetting of the garnet result in excessively high area specific resistances (ASRs) that severely limit achievable current density and cell energy density. In this project, the team is building on their demonstrated expertise with garnet electrolytes and ASSBs to accomplish the following: (1) engineer interfaces to overcome high NMC/LLZ interfacial impedance and interfacial degradation; (2) develop processing and fabrication techniques to achieve high loading NMC/LLZ composite cathodes with low resistance and high cyclability; and (3) integrate the NMC/LLZ cathodes into all-solid-state Li-metal/LLZ cells to achieve high-energy-density batteries.

25 ENERGY STORAGE↗

The development of a non-cryogenic nitrogen/oxygen supply system

Development of the hydrazine/water electrolysis process in a manned spacecraft to provide metabolic oxygen and both oxygen and nitrogen for cabin leakage makeup was studied. Electrode development efforts were directed to stability, achieved with catalyst additives and improved processing techniques, and a higher hydrazine conversion efficiency, achieved by reducing catalyst loading on the cathodes. Extensive testing of the one-man breadboard N2/02 system provided complete characterization of cabin atmosphere control aspects. A detailed design of a prototype modular N2/02 unit was conducted. The contact heat exchanger which is an integral component of this design was fabricated and sucessfully design-verification tested.

Greenough, B. M.↗

Applied-field magnetoplasmadynamic engine developments

There are potential space exploration missions which may significantly benefit from the use of electric propulsion at power levels of hundreds of kilowatts. The applied magnetic field MPD thruster is potentially capable of efficient, high specific impulse operation in this power range. This paper describes current experimental and analytical efforts to further the development of such a thruster and presents the latest results. In particular, efforts to measure, simultaneously, the thrust developed by the archead and by the electromagnet, and to evaluate the effect of a diffuser on vacuum tank back pressure, are presented and discussed. It was found that with ammonia vapor as propellant, the vacuum tank pressure was reduced from 8 to 4.9 Pa at a power level of 80 kW. This pressure decrease is expected to become greater as the power and applied field are increased. Also, the development of a cathode/plasma interaction model for determining the heat loads to the cathode as functions of the various free stream plasma parameters is presented. This model is combined with a cathode thermal model in order to provide a complete and integrated picture of MPD thruster cathode operation. Several computational examples are used to illustrate the combined model.

Goodfellow, K. D.↗

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↗

Impedance Spectroscopy Characterization of PEM Fuel Cells with Fe-N-C-Based Cathodes

We report impedance spectroscopy analysis of PEM fuel cells built with platinum group metal-free (PGM-free) Fe-N-C cathodes with the catalyst loading and ionomer to catalyst ratio being variable parameters. The dependence of key cathode transport and kinetic parameters on the cell current density J are obtained in the range from 0.025 to 0.4 A cm -2 . The electrode performance is evaluated using the characteristic current densities for proton and oxygen transport in the cathode catalyst layer. Overall, certain electrode configurations demonstrate proton and oxygen transport properties comparable to those of Pt/C systems, making them promising substitutes for platinum at cathodic side of PEM fuel cells.

36 MATERIALS SCIENCE↗

Modeling Nanoscale Ohmics in Carbon Supports of Fuel Cell Cathodes

Here, reducing platinum (Pt) loading in polymer electrolyte fuel cells (PEFCs) while meeting performace requirements is critical to their widespread deployment. However, significant polarization losses manifest at higher current densities in cathodes with lower Pt content. The morphology of the carbon supports in PEFC cathodes affects the location of Pt deposition into the micropits or onto the surface of the carbon support, translating into different kinetic and transport resistances. In this work, we derive an agglomerate scale model that differentiates the sink terms for Pt on the surface and in the pits of carbon supports. We develop an approach to assess the impact of nanoscale ohmic resistance to Pt in the micropits arising from weakly ionic solution in the carbon support on PEFC performance. Effectiveness factors relating the actual reaction rate to the maximum reaction rate (had all the Pt been exposed) are derived and embedded into a one-dimensional catalyst layer model. Parameters in the catalyst layer model are tuned based on experimental local oxygen transport resistances. Subsequently, we estimate bounds for the micropore resistances based on geometric and physical arguments. Lastly, polarization curves are simulated to assess the effect of the micropore resistance in fully-humidified and oxygen-rich environments.

25 ENERGY STORAGE↗

Anion Exchange Membrane Water Electrolysis Using a Catalyst-Coated Membrane Cathode

A catalyst-coated membrane (CCM) approach to electrode fabrication for high pH water electrolysis offers enhanced interfacial contact between the catalyst layer and the membrane surface in comparison to the catalyst-coated substrate (CCS) electrode configuration. The CCM facilitates enhanced ionic and water transport between the cathode and the anion exchange membrane (AEM). This advantage is particularly significant with AEM water electrolysis (compared to proton exchange membrane water electrolysis) because the cathode typically operates under dry conditions and relies solely on diffusive water transport across the AEM from the liquid-fed anode. This study presents a direct performance comparison between CCS and CCM cathode configurations using identical hydrogen evolution reaction (HER) catalysts and other components. The use of a pseudo-reference electrode integrated into the membrane electrode assembly enabled detailed analysis of the CCM cathode polarization behavior. Surface characterization provided insight into the degradation mechanisms associated with the CCM configuration. Optimization of the cathode ionomer cross-link density improved both the cathode polarization performance and the electrolysis device durability. Further optimization of the HER catalyst loading in the CCM cathode resulted in additional gains in the electrolysis efficiency. Collectively, these findings offer valuable guidance for the design and fabrication of high-performance, durable AEM electrolysis CCMs.

Water electrolysis↗

The Role of Catholyte Modulation in Suppressing the Initial Capacity Fade of Zinc Electrolytic Manganese Dioxide Coin Cells

Despite its potential for zinc–manganese oxide batteries, electrolytic manganese dioxide (EMD) can experience capacity fade due to a deficiency in the Mn 2+ supply at the cathode electrolyte interphase (CEI) from side reactions, even in the presence of an electrolyte additive. In this work, electrolyte loading modulation at the cathode electrolyte interface (CEI) was correlated with Zn∥EMD cell capacity retention and cycling performance, as a proposed measure to curb the initial capacity fade observed in EMD. Initial galvanostatic charge/discharge cycling, with varied electrolyte loading, revealed severe capacity fade (from ~188 to 10 mAh g –1 for the highest loading of 200 μL) within the first 15 cycles. Such a decrease in cell capacity is correlated with the formation of a Mn 4+ deposit on the current collector and consequently, the Mn 2+ depletion at CEI, as was supported by elemental and Raman analyses. Interestingly, confinement of the electrolyte to the CEI at a lower (≤15 μL) electrolyte loading mitigated Mn 4+ side-deposition, maintaining the cell capacity at >80% over the first 15 cycles. Interfacial Mn supply/depletion could be monitored via voltammetric analysis based on changes of the Zn 2+ insertionreduction peak. Additional galvanostatic experiments corroborated the voltammetric interpretation and the proposed degradation pathway in the studied cell conditions. The outcomes of this work provide practical insight into coin-cell design and configuration strategies for developing Zn∥EMD batteries.

25 ENERGY STORAGE↗

Ultrahigh Mass Loading Batteries with Holey Graphene-Enabled Dry-Pressed Cathode Architectures

Holey graphene is a structural derivative of graphene with arrays of nanometer-sized, through-thickness holes across the lateral surface of the atomically thin nanosheet. It has been widely acknowledged that the presence of holes improves ion transport through the graphene planes, making holey graphene an ideal electrode material for electrochemical energy storage. We recently discovered another unique attribute of holey graphene in that it can be directly compressed from powder into electrode in a single step without the use of solvent or binder. In addition to neat holey graphene electrodes, composite electrodes with holey graphene as an ultralightweight scaffold host filled with various active materials can also be readily prepared in a similar solvent-free and binder-free fashion. The active materials can be metal-containing catalysts for lithium-oxygen batteries, lithium-ion battery electrode materials, or high energy density components such as sulfur. Compared to the conventional slurry-based process, the dry-press method is comparably much more suitable toward the facile and scalable preparation of ultrahigh mass loading electrodes with ultrahigh areal capacities.

holey graphene, cathode scaffold, lithium metal, h↗

3D printing of architected sulfur cathodes with dual-site atomic catalysts for accelerated polysulfide kinetics and Li-ion transport in high areal-loading lithium–sulfur batteries

The practical deployment of lithium–sulfur batteries (LSBs) is hindered by fundamental limitations in conventional slurry-cast cathodes, including poor sulfur utilization, sluggish ion transport, and low areal capacity, particularly in thick electrodes required for high energy density. To address these challenges, we present direct ink writing (DIW) as an additive manufacturing strategy to fabricate advanced current-collector-free, 3D-printed sulfur cathodes (3DP S@CoNi-DSACs/NC) with hierarchically porous architectures that enhance lithium-ion diffusion, promote electrolyte penetration, and reduce interfacial resistance. The synergistic effects of Co/Ni dual-atom sites accelerate redox kinetics and mitigate polysulfide shuttling. As a result, the optimized 3DP cathode with a sulfur loading of 5.4 mg cm −2 demonstrated excellent rate capability, delivering a high reversible capacity of 1041.4 mAh g −1 at 1C with 85.5% capacity retention after 1000 cycles, significantly outperforming its cast counterpart. Remarkably, even at a higher sulfur loading of 8.1 mg cm −2 , the 3DP cathode maintains outstanding performance, achieving a discharge capacity of 1538.4 mAh g −1 and an areal capacity of 12.5 mAh cm −2 at 0.1C. This study not only demonstrates the functional integration of catalytically active materials into 3D printable sulfur cathode architectures but also offers a scalable and transformative platform for building high-performance LSBs beyond conventional electrode manufacturing methods.

3D electrode↗

Fatigue failure of hydrogen embrittled high strength steels

Results of an experimental investigation are presented concerning the fracture behavior of cathodically charged, quenched and tempered martensitic steels under cyclic load conditions. Introduction of H2 by cathodic charging reduced fatigue life by as much as 60%. It is proposed that subsurface transverse fatigue cracks nucleate simultaneously at multiple sites, such as at microcracks, voids, or inclusions. Fatigue crack growth then occurs on planes perpendicular to the major applied stress axis in the presence of the critical combination of applied external stress and hydrogen.

Kim, Y. G.↗

Unlocking Failure Mechanisms and Improvement of Practical Li-S Pouch Cells Through in Operando Pressure Study

For Lithium-sulfur (Li-S) battery commercialization, the study at a pouch cell level is essential, as some problems ignored or deemed minimal at the smaller level could have a greater effect on the performance of the larger pouch cell. Herein, the failure mechanisms of Li-S pouch cells are deeply investigated via in operando pressure analysis. It is found that highly porous structures of cathodes/separators and slow electrolyte diffusion through cathodes/separators can both lead to poor initial wetting. Additionally, Li-metal anode dominates the thickness variation of the whole pouch cell, which is verified by in situ measured pressure variation. Consequently, a real-time approach that combined normalized pressure with dP/dV analysis is proposed and validated to diagnose the morphology evolution of Li-metal anode. Moreover, applied pressure and porosity/tortuosity ratio of the cathode are both identified as independent factors that influence anode performance. In addition to stabilizing anodes, high pressure is proven to improve the cathode connectivity and avoid cathode cracking over cycling, which improves the possibility of developing cathodes with high sulfur mass loading. This work provides insights into Li-S pouch cell design (e.g., cathode and separator) and highlights pathways to improve cell capacity and cycling performance with applied and monitored pressure

25 ENERGY STORAGE↗

Selenium Nanocomposite Cathode with Long Cycle Life for Rechargeable Lithium‐Selenium Batteries

Abstract Selenium (Se) is a potential cathode material for high energy density rechargeable lithium batteries. In this study, a binder‐free Se‐carbon nanotube (CNT) composite electrode has been prepared by a facile chemical method. At initial state, Se is present in the form of branched nanowires with a diameter of <150 nm and a length of 1–2 μm, interwoven with CNTs. After discharge and re‐charge, the Se nanowires are converted to nanoparticles embedded in the CNT network. This synthesis method provides a path for fabricating the Se cathodes with controllable mass loading and thickness. By studying the composite electrodes with different Se loading and thickness, we found that the electrode thickness has a critical impact on the distribution of Se during repeated cycling. Promising cycling performance was achieved in thin electrodes with high Se loading. The composite electrode with 23 μm thickness and 60 % Se loading shows a high initial capacity of 537 mAh g −1 and stable cycling performance with a capacity of 401 mAh g −1 after 500 cycles at 1 C rate. This study reports a synthesis strategy to obtain Se/CNT composite cathode with long cycle life for rechargeable Li−Se batteries.

Cui, Yi↗

Unlocking Failure Mechanisms and Improvement of Practical Li–S Pouch Cells through In Operando Pressure Study

For Lithium-sulfur (Li-S) battery commercialization, the study at a pouch cell level is essential, as some problems ignored or deemed minimal at the smaller level could have a greater effect on the performance of the larger pouch cell. Herein, the failure mechanisms of Li-S pouch cells are deeply investigated via in operando pressure analysis. It is found that highly porous structures of cathodes/separators and slow electrolyte diffusion through cathodes/separators can both lead to poor initial wetting. Additionally, Li-metal anode dominates the thickness variation of the whole pouch cell, which is verified by in situ measured pressure variation. Consequently, a real-time approach that combined normalized pressure with dP/dV analysis is proposed and validated to diagnose the morphology evolution of Li-metal anode. Moreover, applied pressure and porosity/tortuosity ratio of the cathode are both identified as independent factors that influence anode performance. In addition to stabilizing anodes, high pressure is proven to improve the cathode connectivity and avoid cathode cracking over cycling, which improves the possibility of developing cathodes with high sulfur mass loading. Here, this work provides insights into Li-S pouch cell design (e.g., cathode and separator) and highlights pathways to improve cell capacity and cycling performance with applied and monitored pressure.

25 ENERGY STORAGE↗

Artificial cathode electrolyte interphase for improving high voltage cycling stability of thick electrode with Co-free 5 V spinel oxides

Spinel-type cathode LiNi 0.5 Mn 1.5 O 4 (LNMO) has intrigued the transportation industry due to its high operating voltage and total elimination of the expensive cobalt element. However, LNMO cathode with high mass loading (> 3 mAh/cm 2 in areal capacity) has suffered from excessive capacity degradation upon long cycling. Here, a robust Al 2 O 3 surface layer is introduced to the thick LNMO electrode via atomic layer deposition (ALD). The capacity retention in full cells with the graphite anode is improved from 46.3% to 75.3% after 300 cycles with cutoff voltage up to 4.85 V, while enabling average Coulombic efficiency of 99.9% during the cycling. The post-mortem analyses reveal that the Al 2 O 3 surface layer would convert to Al-O-F /Al-F species upon cycling, offering stable interphase to protect the cathode material. Furthermore, these results demonstrate the significance of surface modification enabling high voltage cathode for next-generation LIBs.

25 ENERGY STORAGE↗