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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
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

High-performance ionomerless cathode anion-exchange membrane fuel cells with ultra-low-loading Ag–Pd alloy electrocatalysts

Rapid translation of catalysts from fundamental studies to high-performance devices could facilitate the process of developing and commercializing anion-exchange membrane fuel cells (AEMFCs). Traditionally, translation from material screening in three-electrode rotating disk electrode (RDE) cells to AEMFCs is complicated by differences in microenvironments, e.g. solid ionomer/membrane vs liquid electrolyte. Herein, we introduce a platform for translation to devices that utilizes ionomerless ultra-low-loading Ag-Pd alloy electrocatalyst cathodes synthesized by co-physical vapor deposition (PVD). Our ionomerless cathodes allow for systematic H 2 -O 2 AEMFC experiments while demonstrating comparable activity trends to those in three-electrode cells. Furthermore, here we show that our Ag 10 Pd 90 -based AEMFC reaches a peak power density of ~1 W cm$_{geo}^{-2}$ and ~10 W mg$_{PGM Cathode}^{-1}$ satisfying the U.S. Department of Energy’s platinum-group-metal (PGM) loading and cost targets. Our approach shows promise in facilitating the rapid translation between three-electrode studies and AEMFCs, offering a simple and effective design for decreasing PGM loadings.

25 ENERGY STORAGE↗
DOE OSTI2022

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.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2017

Burning lithium in CS 2 for high-performing compact Li 2 S–graphene nanocapsules for Li–S–batteries

Here, tremendous efforts have been made to design the cathode of Li–S batteries to improve their energy density and cycling life. However, challenges remain in achieving fast electronic and ionic transport while accommodating the significant cathode volumetric change, especially for the cathode with a high practical mass loading. Here we report a cathode architecture, which is constructed by burning lithium foils in a CS 2 vapour. The obtained structure features crystalline Li 2 S nanoparticles wrapped by few-layer graphene (Li 2 S@graphene nanocapsules). Because of the improvement on the volumetric efficiency for accommodating sulfur active species and electrical properties, the cathode design enables promising electrochemical performance. More notably, at a loading of 10 mg Li 2 S cm –2 , the electrode exhibits a high reversible capacity of 1,160 mAh g –1 s, namely, an area capacity of 8.1 mAh cm –2 . Li 2 S@graphene cathode demonstrates a great potential for Li-ion batteries, where the Li 2 S@graphene-cathode//graphite-anode cell displays a high capacity of 730 mAh g –1 s as well as stable cycle performance.

25 ENERGY STORAGE↗
DOE OSTI2021

All solid thick oxide cathodes based on low temperature sintering for high energy solid batteries

Solid-state batteries (SSBs) could significantly improve the safety and energy density over conventional liquid cells. One key enabling technology is the use of solid electrolytes. NASICON-type Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) is a very attractive solid-state electrolyte for the cathode side due to its high oxidation potential and high ionic conductivity. The usage, however, is limited by its large interfacial resistance against most of the cathode materials as well as the thermodynamic instability during high temperature sintering needed to achieve high mass density. Here we construct thin, percolative, and mixed conductive interphases through in situ low-melting-point liquid sintering. These mixed conductive interphases drastically improve the kinetics, leading to high-loading solid LATP/LiCoO 2 cathodes achieving capacity loading of up to ~6 mA h cm –2 . The technique is also applicable to Ni-rich cathode materials, achieving up to ~10 mAh cm –2 , which can lead to more than 400 W h kg –1 cells in SSBs. Furthermore, our composite cathodes show a ten-times and three-times area capacity improvement over the state-of-the-art cathodes using oxide and sulfide SSEs, respectively.

25 ENERGY STORAGE↗
DOE OSTI2017

Polarization loss correction derived from hydrogen local-resistance measurement in low Pt-loaded polymer-electrolyte fuel cells

The reduction of platinum-loading on the cathode side of polymer-electrolyte fuel cells leads to a poorly understood increase in mass-transport resistance (MTR) at high current densities. This local resistance was measured using a facile hydrogen-pump technique with dilute active gases for membrane-electrode assemblies with catalyst layers of varying platinum-loading (0.03-0.40 mgPt/cm²). Furthermore, polarization curves in H 2 /air were measured and corrected for the overpotential caused by the increased MTR for low loadings on the air side due to the reduced concentration of reactant gas at the catalyst surface. The difference in performance after correction for all resistances including the MTR is minor, suggesting its origin to be diffusive in nature, and proving the meaningfulness of the facile hydrogen-pump technique for the characterization of the cathode catalyst layer under defined operation conditions.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2021

Investigating Multiscale Spatial Distribution of Sulfur in a CNT Scaffold and Its Impact on Li–S Cell Performance

Ever increasing demand on high energy density batteries positions sulfur as a very promising cathode material for next-generation energy storage due to its high theoretical capacity of 1675 mAh/g. Electronically sulfur is highly insulating, and therefore integration of a conducting framework such as a carbon nanotube (CNT) scaffold with sulfur is a key aspect of the cathode design. Despite numerous efforts dedicated to S-CNT cathode development, increasing sulfur loading to above 1 mg/cm 2 while maintaining the cycling stability of the Li–S cell remains challenging. This could be partly due to the lack of understanding of the spatial distribution of sulfur in the CNT matrix and its location with respect to the morphology of the CNT scaffold. We demonstrate herein that the sulfur has a hierarchical distribution in the CNT cathode at high sulfur loading (>5 mg/cm 2 ) spanning multiple length scales (from nanometer to submillimeter). Sulfur infiltration into the CNT rather than the sulfur loading plays a key role in determining the redox reaction kinetics, Li + ion diffusion, and the galvanostatic cycling capacity and stability of Li–S cells. This study provides new insights for the design and fabrication of high loading, binder-free sulfur–carbon-based cathode architectures for next-generation high energy Li–S batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Regulating catalyst and ionomer interactions to promote oxygen transport in fuel cells

The cost of proton exchange membrane fuel cells (PEMFCs) has been a major impediment to their widespread commercialization. Reducing platinum (Pt) usage in PEMFC represents an essential step in lowering the cost. However, decreasing Pt loading in the cathode catalyst layer (CCL) often leads to a significant increase in the local oxygen transport resistance (R Local ), which not only slows the oxygen reduction reaction but also causes a higher polarization overpotential. The poisoning of Pt by perfluorosulfonic acid ionomers also becomes more predominant at low Pt loadings. Therefore, regulating catalyst and ionomer interactions by optimizing their interface in the CCL is crucial to improving PEMFC performance. Here, in this review, the strategies of improving oxygen transport by controlling Pt-ionomer interactions and interfaces through catalyst design, ionomer structure, and incorporation of additives are summarized. Finally, perspectives on future optimization of catalyst and ionomer interactions are proposed.

25 ENERGY STORAGE↗
DOE OSTI2023

Electrochemical conversion of methane to ethylene, olefins, and paraffins using metal-supported solid oxide cells

Electrochemical oxidative coupling of methane (E-OCM) with Sr 2 Fe 1·5 Mo 0·5 O 6–δ (SFM) catalyst is demonstrated with metal-supported solid oxide cells (MS-SOC). SFM anode and Pr 6 O 11 cathode catalysts are loaded into a porous symmetric-architecture cell by infiltration and firing. The most effective chelating agent (citric acid/ethyl glycol) and optimal firing/reducing temperatures (850 °C/750 °C) for the SFM catalyst precursor solution are selected and confirmed by cell testing. Operating temperature, cell voltage, and oxygen concentration at the cathode greatly affect the methane conversion rate and product selectivity by controlling the oxygen ion flow. CH 4 conversion of 85.8% is obtained, with C 2 H 4 , C 2 H 6 , and H 2 concentrations of 10.5%, 12.3%, and 25.6% at 800 °C, respectively, in the product exhaust gas. Reasonable stability of the current density and methane conversion is demonstrated during 200 h operation. Furthermore, this research demonstrates technical progress in catalyst and device development for the E-OCM reaction to synthesize valuable chemicals.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2023

Enhancing the Electrode Gravimetric Capacity of Li 1.2 Mn 0.4 Ti 0.4 O 2 Cathode Using Interfacial Carbon Deposition and Carbon Nanotube-Mediated Electrical Percolation

Mn-based cation disordered rocksalt oxides (Mn-DRX) are emerging as promising cathode materials for next-generation Li-ion batteries due to their high specific capacities and cobalt and nickel free characteristic. However, to reach the theoretical capacity, solid-state method synthesized Mn-DRX materials require activation via post-synthetic ball milling, typically incorporating more than 20 wt.% conductive carbon that adversely reduces the electrode level gravimetric capacity. To solve this issue, we firstly deposit amorphous carbon on the surface of the Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO) particles to increase the electrical conductivity by a five order of magnitude. Although the cathode material gravimetric first charge capacity reaches 180 mAh/g, its highly irreversible behavior leads to a 70 mAh/g first discharge capacity. Subsequently, to ensure a good electrical percolation network, the LMTO material is ball milled with multi-wall carbon nanotube (CNT) to obtain a 78.7 wt.% LMTO active material loading in the cathode electrode (LMTO-CNT). As a result, a 210 mAh/g cathode electrode gravimetric first charge and 165 mAh/g first discharge capacity are obtained, compared to the respective capacity values of 222 mAh/g and 155 mAh/g for the LMTO ball milled with 20 wt.% SuperP C65 electrode (LMTO-SP). After 50 cycles, the LMTO-CNT delivers a 121 mAh/g electrode gravimetric discharge capacity, largely outperforming the 44 mAh/g value of the LMTO-SP. In conclusion, our study demonstrates that while ball milling is necessary to achieve the theoretical capacity of LMTO, a careful selection of the additive, such as CNT, effectively reduces the required carbon quantity to achieve a higher electrode gravimetric discharge capacity.

25 ENERGY STORAGE↗
DOE OSTI2017

Modeling Electrochemical Performance of the Hierarchical Morphology of Precious Group Metal-free Cathode for Polymer Electrolyte Fuel Cell

Here, this paper presents a two-dimensional (2D) computational model of a polymer electrolyte fuel cell (PEFC) with a platinum group metal-free (PGM-free) catalyst cathode that can significantly reduce PEFC costs by eliminating the need for expensive platinum catalysts. Due to their comparatively low volumetric activity, PGM-free cathodes are an order of magnitude thicker than their Pt-based counterpart. The resulting need for greater electrode thickness to achieve sufficient power density requires careful attention to the transport losses across the thicker cathodes. The presented model is used to correlate the composition and morphology of the cathode to PEFC performance. The model is a complete cell, continuum model that includes an advanced agglomerate model for a microstructurally consistent representation of the cathode. A unique feature of the approach is the integration of morphology and transport parameter statistics extracted from nano-scale resolution X-ray computed tomography (nano-CT) imaging of PGM-free cathodes. The model was validated with experimental results of PGM-free cathodes with varying Nafion loading. Lastly, our key findings are a need for increased cathode hydrophobicity and increased ionomer conductivity through either reduced tortuosity or increased bulk conductivity. We further use the model to evaluate targets for the volumetric activity and active site density for future catalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2019

Iron Single Atoms on Graphene as Nonprecious Metal Catalysts for High‐Temperature Polymer Electrolyte Membrane Fuel Cells

Abstract Iron single atom catalysts (Fe SACs) are the best‐known nonprecious metal (NPM) catalysts for the oxygen reduction reaction (ORR) of polymer electrolyte membrane fuel cells (PEMFCs), but their practical application has been constrained by the low Fe SACs loading (<2 wt%). Here, a one‐pot pyrolysis method is reported for the synthesis of iron single atoms on graphene (FeSA‐G) with a high Fe SAC loading of ≈7.7 ± 1.3 wt%. The as‐synthesized FeSA‐G shows an onset potential of 0.950 V and a half‐wave potential of 0.804 V in acid electrolyte for the ORR, similar to that of Pt/C catalysts but with a much higher stability and higher phosphate anion tolerance. High temperature SiO 2 nanoparticle‐doped phosphoric acid/polybenzimidazole (PA/PBI/SiO 2 ) composite membrane cells utilizing a FeSA‐G cathode with Fe SAC loading of 0.3 mg cm −2 delivers a peak power density of 325 mW cm −2 at 230 °C, better than 313 mW cm −2 obtained on the cell with a Pt/C cathode at a Pt loading of 1 mg cm −2 . The cell with FeSA‐G cathode exhibits superior stability at 230 °C, as compared to that with Pt/C cathode. Our results provide a new approach to developing practical NPM catalysts to replace Pt‐based catalysts for fuel cells.

25 ENERGY STORAGE↗
DOE OSTI2017

Microstructural Analysis and Transport Resistances of Low-Platinum-Loaded PEFC Electrodes

In this study, we present microstructural characterization for polymer electrolyte fuel cell (PEFC) cathodes with low platinum loadings (low-PGM). The characterization results are used to quantify the contribution of mass transport resistances to cell voltage losses observed in polarization curve data. Three-dimensional pore morphology and ionomer distribution are resolved using nano-scale X-ray computed tomography (nano-CT). Electrode structural properties are reported along with analysis of the impact of microstructure on the effective charge and reactant transport properties. These characterizations are incorporated with a two-dimensional multi-physics model that accounts for energy, charge, and mass transport along with the effect of liquid water flooding. Defining a total mass transport resistance for the whole polarization curve, contributions of transport mechanisms are identified. Analysis of the experimental polarization curves at different operating pressures and temperatures indicates that the mass transport resistance in the cathode is dominated by the transport processes in the electrode. It is shown that flooding in the electrode is a major contributor to transport losses especially at elevated operating pressures while the pressure-independent resistance at the catalyst surface due to transport through the ionomer film plays a significant role, especially at low temperatures and low catalyst loading. In addition, by performing a parametric study for varying catalyst loadings, the importance of electrode roughness (i.e, electrochemically-active surface area/geometric electrode area) in determining the mass transport losses is highlighted.

25 ENERGY STORAGE↗
DOE OSTI2020

Advanced electrolytes for fast-charging high-voltage lithium-ion batteries in wide-temperature range

LiNixMnyCo1-x-yO2 (NMC) cathode materials with Ni=0.8 have attracted great interest for application in high energy-density lithium (Li)-ion batteries (LIBs) because of their high specific capacities at high voltages. However, the practical application of Ni-rich NMC in LIBs under high charge voltages (e.g. 4.4 V and above) still faces big challenges due to the severe capacity fading, which is directly related to the instability of the cathode/electrolyte interface. In this work, we develop new localized high-concentration electrolytes (LHCEs) based on carbonate solvents, which are compatible with graphite (Gr) anode and have a high oxidation potential over 4.9 V vs. Li/Li+. The optimal LHCE enables the Gr||NMC811 cells with 2.8 mAh cm-2 cathode areal capacity loading to achieve an excellent cycling stability over 600 cycles with a capacity retention of 94.2 % under a charge cut-off voltage of 4.4 V at 25 ?C, good rate capabilities under fast charging or discharging up to 3C rate, and superior low-temperature discharge performance down to -30 ?C with a capacity retention of 85.6% at C/5 rate. The findings in this work shed light a very promising strategy to develop new electrolytes for practical high-energy LIBs with Ni-rich NMC cathodes.

Zhang, Xianhui↗
DOE OSTI2020

High-performance and cost-effective membrane electrode assemblies for advanced proton exchange membrane water electrolyzers: Long-term durability assessment

In this work, improved activity and durability performance of a two-cell (86 cm 2 ) proton exchange membrane water electrolyzer (PEMWE) stack is reported for the first time. Both membrane electrode assemblies (MEAs) contain one order of magnitude lower platinum group metal (PGM) loadings compared to the state-of-the-art PEMWEs and incorporate novel Pt recombination layers. The high-performance and cost-effective MEAs are fabricated by the unique reactive spray deposition technology (RSDT). This advanced methodology allows for one-step fabrication of MEAs and ensures precise control and distribution of the catalyst composition and loading. The RSDT-fabricated MEAs contain only 0.2 and 0.3 mg PGM cm –2 loading in the cathode and anode electrodes, respectively, and demonstrate excellent activity and durability for over 3000 h of operation at industrially-relevant operating conditions without showing significant loss in performance. This novel work shows that a significant cost reduction for PEMWEs is achieved while maintaining excellent durability, high catalysts activities, and low hydrogen cross-over.

Proton exchange membrane water electrolyzer↗
DOE OSTI2022

High-performance all-solid-state Li–S batteries enabled by an all-electrochem-active prelithiated Si anode

The development of all-solid-state Li–S batteries has been greatly impeded by dendrite growth and dendrite penetration, which are both related to the Li metal anode. As a compromised alternative, we report lithium silicide (Li x Si) as a dendrite-free and high-capacity anode with Li source. Here, the as-synthesized Li x Si is relatively soft, highly electronically conductive, and with a high Li diffusivity. These distinctive properties make Li x Si anode viable as an “all-electrochem-active” electrode (consisted of 100 wt.% Li x Si). Compared with the typical composite electrode, the all-electrochem-active electrode not merely maximizes the electrode-level energy density but also minimizes the electrolyte-related interfacial degradation. Li x Si symmetric cell demonstrates a reversible cycling at 4 mA cm –2 for over 320 h. Stress change and morphological evolution of the Li x Si electrode are investigated upon dealloying/alloying. When paired with a S cathode (active mass loading of 3 mg cm –2 ), Li x Si–S full cell shows a good cycling behavior over 500 cycles and rate performance (69% capacity retained at 1.2C) even at 25 °C.

25 ENERGY STORAGE↗
DOE OSTI2022

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↗