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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
NASA NTRS1990

Modeling and optimization of a regenerative fuel cell system using the ASPEN process simulator

The Hydrogen-Oxygen Regenerative Fuel Cell System was identified as a key component for energy storage in support of future lunar missions. Since the H2-O2 regenerative electrochemical conversion technology has not yet been tested in space applications, it is necessary to implement predictive techniques to develop initial feasible system designs. The ASPEN simulation software furnishes a constructive medium for analyzing and for optimizing such systems. A rudimentary regenerative fuel cell system design was examined using the ASPEN simulator and this modular approach allows for easy addition of supplementary ancillary components and easy integration with life support systems. The modules included in the preliminary analyses may serve as the fundamental structure for more complicated energy storage systems.

Maloney, Thomas M.↗
NASA NTRS1990

Modeling and optimization of a regenerative fuel cell system using the ASPEN process simulator

The Hydrogen-Oxygen Regenerative Fuel Cell System was identified as a key component for energy storage in support of future lunar missions. Since the H2-O2 regenerative electrochemical conversion technology has not yet been tested in space applications, it is necessary to implement predictive techniques to develop initial feasible system designs. The ASPEN simulation software furnishes a constructive medium for analyzing and optimizing such systems. A rudimentary regenerative fuel cell system design was examined using the ASPEN simulator and this modular approach allows for easy addition of supplementary ancillary components and easy integration with life support systems. The modules included in the preliminary analyses may serve as the fundamental structure for more complicated energy storage systems.

Maloney, Thomas M.↗
DOE OSTI2021

A multi-phase-field model of topological pattern formation during electrochemical dealloying of binary alloys

Porous metal structures produced by electrochemical dealloying have been extensively studied for use in various applications that require high surface areas. A new comprehensive multi-phase-field (MPF) model is proposed to study topological porous patterns formed by spontaneously etching a bulk binary alloy that involves electrochemical reactions, bulk and surface diffusion, ion transport, applied electrode potential, and charge conservation. The governing equations for the alloy-porous cluster-electrolyte system account for a generalized Butler-Volmer electrochemical reaction and are in accordance with the classical nucleation theory. Based on a quantitative examination of the effects of electrode potential and precursor composition, the simulation results reproduce typical phenomena including passive surface dealloying, active porosity evolution, critical potential, and characteristic length scale in two-dimension (2-D) and three-dimension (3-D). To consider more complicated dealloying systems, the evolutions of a bimodal porous metal structure, nanocomposite, and nested porous network with a structured hierarchy are investigated. Finally, the proposed model can be a useful tool for understanding and predicting the morphology evolution of diverse porous structures during electrochemical dealloying.

Hierarchical porous structure↗
DOE OSTI2024

NUMERICAL MODELING OF A SOLID OXIDE FUEL CELL FOR USE IN REAL-TIME SIMULATION AND CYBER-PHYSICAL SYSTEMS

Cyber-physical systems provide a mechanism with which to investigate the physical phenomena and behavior of traditionally cost-prohibitive or otherwise fragile equipment. For the National Energy Technology Laboratory (NETL), this approach resulted in the Hybrid Performance (Hyper) facility which features a gas turbine-SOFC hybrid cycle utilizing real turbomachinery and a simulated SOFC stack. This allows for the investigation of combined cycle performance and control strategies, in an exhaustive manner, both without fear of destroying delicate state-of-the-art fuel cells, and with the full accuracy of real-world turbomachinery. Issues arose between the transient response of the SOFC model being limited to a sample time of 80 milliseconds, due to the calculation time of the SOFC model taking on average 40 milliseconds to calculate for a given timestep with spikes in calculation time reaching the 80 millisecond threshold. In order to be able to match the speed of transients from the turbomachinery and likewise better discern transient behavior, it was determined that the SOFC model must be optimized to operate at a sample time of 5 milliseconds. Therefore, it is necessary to optimize the SOFC model in order to decrease the calculation time from around 40 milliseconds, down to at the most 5 milliseconds. To do this, both the electrochemical algorithm and the thermal algorithm used to simulate the physical behavior of the SOFC are investigated to determine where improvements can be made. To this end the rootfinding numerical recipes of the electrochemical algorithm are investigated as the complex electrochemistry requires a highly iterative nested dual convergence loop to resolve the voltage-current relationship, and likewise the temporal discretization of the thermal algorithm is modified for the sake of higher accuracy and stability. Ultimately the new electrochemical algorithm featuring higher order rootfinding schemes proves to be efficient enough to reach the sub 5 millisecond target, signifying an order of magnitude reduction in calculation time, and when coupled with the new temporal discretization similar calculation time characteristics show that a fully implicit, higher order temporal discretization can also successfully be used if desired. Ultimately this result means that the cyber-physical simulation system can operate at higher sample rates, and resolve transient events at significantly higher resolution and fidelity.

Arias, Jesus↗
DOE OSTI2020

Impact Modeling and Testing of Pouch and Prismatic Cells

Understanding battery response under impact is critical to improve the safety of electrified vehicles. Nevertheless, predicting the impact behaviors of batteries is not straightforward since a battery cell usually contains hundreds of thin layers with dramatically different material properties and multiple physical processes occur simultaneously during cell deformation. Here we utilized both empirical tests and numerical models to capture the failure process of pouch and prismatic cells in various impact scenarios. In each test, a cell was hit once by an indenter dropped from a certain height. During which the cell penetration, loading force, voltage and temperature were monitored to characterize the cell’s response. Meanwhile, numerical models were developed to capture the coupled mechanical, electrical, electrochemical and thermal responses of batteries. In these models, the cell bulk was treated as a homogeneous part to achieve computational efficiency required by large-scale simulations, and it was represented by the geologic cap model that allows both shear and compaction deformation. Simulation results showed agreement with experimental data in essential features of cell behaviors during impact. Details of the test setup, model development and cell failure behaviors are presented in this paper. Additionally, capabilities, limitations and future improvement of the battery safety modeling are discussed.

25 ENERGY STORAGE↗
DOE OSTI2024

Designing SOC electrodes for better lifetime performance

Presentation for talk at the 2024 Pacific Rim Meeting of the Electrochemical Society October 6-11, 2024. The talk covers a review of NETL's solid oxide cell (SOC) performance degradation modeling framework and present case studies on how simulations are used to design better SOC electrodes.

Abernathy, Harry↗
DOE OSTI2024

Communication—First-Principles Simulations of LiPF 6 Decomposition in Ethylene Carbonate-Based Electrolytes

We revisit a theoretical result by Okamoto (2013 Journal of The Electrochemical Society , 160 , A404) who calculated the energy barrier for the decomposition of lithium hexafluorophosphate (LiPF 6 ) into LiF + PF 5 when solvated in Ethylene carbonate (EC)-based electrolyte. Using different numerical techniques to discretize the Density Functional Theory (DFT) equations, and different continuum solvation models with the same dielectric constant, our results largely confirm the original calculation. However, simulations with a higher dielectric permittivity value, closer to that of EC, show a lower energy barrier. More importantly, First-Principles simulations with an explicit solvent show a substantially lower energy barrier.

25 ENERGY STORAGE↗
DOE OSTI2024

Theories of homogeneous and electrochemical electron transfer in complex media and interfaces (Final Technical Report)

This project makes the next step in establishing practical theories of charge transfer in complex media. The development of formal models is supported by extensive atomistic simulations, quantum calculations of force-field parameters, and direct measurements of charge-transfer spectra. All theory development is supported by experiment, extensive numerical simulations, and through external collaborations.

14 SOLAR ENERGY↗
NASA NTRSDate not supplied

SIBatt-3D: In-Space/On-Surface 3D Printing of Sodium Ion Batteries from ISRU Materials

Constructed more than 20 years ago, the International Space Station’s primary power system originally used nickel-hydrogen batteries with a lifetime of 6.5 years, until NASA began the process of replacing them in 2016 with lithium-ion batteries with a lifetime of 10 years. The demanding and costly process was accomplished after four flights of the Japanese H-II Transfer Vehicle cargo spacecraft (with a cost of about $10,000 per pound of payload), and 13 different astronauts conducting 14 spacewalks. Besides utilization in the ISS, rechargeable batteries are present in many space applications: they are installed in exploration robots, life support systems and in portable communication devices, to mention some. In this context, this project is focused on the in-space manufacturing of shape-conformable batteries using in-situ resources, and aims to address the NASA’s gaps related to the development of next generation of energy storage devices (TX03), as well as in-space manufacturing and in-situ resource utilization (TX07). The proposed work also tackles the HEOMD’s objectives targeting the in-space additive manufacturing (AM) from Lunar/Martian materials (regolith as AM feedstock) to reinvigorate America’s Human Space Exploration Program (SPD-1). This project is in direct alignment with the STMD’s objectives to demonstrate in-space autonomous manufacturing and assembly of complete systems by 2030, and to enable humans to live and explore in space and on planetary surfaces by 2040 thanks to in-space habitation, infrastructure development and in-situ resource utilization (ST1 and ST5). Manufacturing of shape conformable batteries directly in-space and using in-situ resources would also contribute to reducing the payload weight and volume (TX12) for future missions, thus reducing risk for long term Mars missions where rapid resupply is logistically infeasible. Nowadays, commercial batteries consist of stacked two-dimensional (2D) sheets, which are only manufactured in restricted geometries (cylindrical and coin cell). Evolving from conventional 2D, complex 3D battery architectures have been proven to increase the electrochemical active surface area and ion diffusion path, leading to improved areal energy density and power performance. This tendency was illustrated in our recent in-depth modeling studies by simulating a classical Ragone plot exhibiting the energy-power relationship. Our team demonstrated through modeling that a complex gyroidal 3D printed battery architecture exhibits significantly improved power performances (>150% at the current density of 6C; full discharge in 10 minutes) in comparison to a traditional 3D printed planar geometry. Motivated by these results and as the fabrication of intricate 3D battery design is only possible experimentally thanks to the geometric freedom offered by additive manufacturing (AM), our team has already initiated leveraging thermoplastic material extrusion at the laboratory scale. While 3D printing of batteries is relatively recent (2013), it has witnessed a growing interest during the last recent years, as next-generation shape-conformable 3D batteries can be co-designed with the system. Consequently, dead-volume and mass brought from Earth are minimized, in addition to improved battery performance, in alignment with the aforementioned NASA’s objectives. Further, while this project is specifically dedicated to batteries, it lends itself towards the maturation of in-space manufacturing via 3D printing using in-situ resources, stated in HEOMD and STMD goals.

In-Space Manufacturing↗
DOE OSTI2020

Two-Dimensional Conductive Ni-HAB as a Catalyst for the Electrochemical Oxygen Reduction Reaction

Catalytic systems whose properties can be systematically tuned via changes in synthesis conditions are highly desirable for the next-generation catalyst design and optimization. Herein, we present a two-dimensional (2D) conductive metal–organic framework consisting of M-N 4 units (M = Ni, Cu) and a hexaaminobenzene (HAB) linker as a catalyst for the oxygen reduction reaction. By varying synthetic conditions, we prepared two Ni-HAB catalysts with different crystallinities, resulting in catalytic systems with different electric conductivities, electrochemical activity, and stability. We show that crystallinity has a positive impact on conductivity and demonstrate that this improved crystallinity/conductivity improves the catalytic performance of our model system. Additionally, density functional theory simulations were performed to probe the origin of M-HAB’s catalytic activity, and they suggest that M-HAB’s organic linker acts as the active site with the role of the metal being to modulate the linker sites’ binding strength.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Sulfurized Polyacrylonitrile for High-Performance Lithium–Sulfur Batteries: In-Depth Computational Approach Revealing Multiple Sulfur’s Reduction Pathways and Hidden Li + Storage Mechanisms for Extra Discharge Capacity

Like no other sulfur host material, polyacrylonitrile-derived sulfurized carbon (SPAN) promises improved electrochemical performance for lithium–sulfur batteries, based on its compatibility with carbonate solvents and ability to prevent self-discharge and shuttle effect. However, a complete understanding of the SPAN’s lithiation mechanism is still missing because its structural features vary widely with synthesis conditions, and its electrochemical performance deviates from elemental sulfur. This study continues our research on the elucidation of the SPAN’s structural characteristics and lithiation mechanisms via computational approaches. Here, our models reproduce most experimental data regarding carbon’s graphitization level and conjugated ordering, sulfur–carbon covalent bonding, sulfur loading, and elemental composition. Our simulations emulate the discharge voltage observed in experiments for the first discharge, which reveals that sulfur follows multiple reduction pathways based on its interaction with the carbon backbone. Sulfur reduction takes place above 1.0 V vs Li/Li + mostly in the SPAN-like material, with no long-chain lithium polysulfide formation. Below 1.0 V vs Li/Li + , the backbone’s electrochemical activity occurs via multiple C–Li and N–Li interactions, mostly with edge carbon atoms and pyridinic nitrogen. Moreover, we identify Li + binding sites throughout the graphitized backbone that might lead to prohibited energy costs for Li + deintercalation, which may explain the irreversible capacity loss between the first and second discharges. This work improves understanding of lithiation mechanisms in sulfurized carbon, which is useful for rationally designing SPAN synthesis pathways tailored to increase sulfur loading and enhanced electrochemical performance.

25 ENERGY STORAGE↗
DOE OSTI2021

Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation

Alloying-type anodes are significantly governed by their chemo-mechanical performance during the electrochemical cycling. The reaction-induced huge volumetric change of these anodes may cause material degradation and failure under mechanical constraints. Here, we investigate the stress-dependent lithiation behavior of amorphous Si (a-Si) anodes using molecular dynamics simulations. It is indicated that a-Si anodes can sustain higher hydrostatic stress than biaxial/uniaxial ones without the occurrence of mechanical failure. Thermodynamic and electrochemical calculations demonstrate that although the lithiation procedure also affects the thermodynamic stability of a-Si anodes, it is mainly dominated by the external mean stresses. Compressive stress is confirmed to destabilize a-Si anodes and further trigger their capacity fading. Compared with our atomistic simulations, previous continuum models underestimate the open-cell potentials of a-Si anodes, due to their ignored large volumetric deformation at higher stresses and Li concentrations. Finally, this computational study provides the intensive atomic-level understanding of the stress-dependent lithiation behavior of a-Si anodes.

25 ENERGY STORAGE↗
NASA NTRS2018

Exploring Li-Air Batteries for High Specific Energy and High Power Applications: A Simulation Study

Commercialization of lithium-air batteries face many challenges, such as electrolyte decomposition, short cycle life, low energy efficiency, low power density, etc. However, commercialization of Li-air batteries for mass sensitive applications such as electric vehicles, portable power source, and drones is more challenging due to additional constraints of safety, electrolyte evaporation, high specific energy requirements, and reliable discharge times. In this presentation, we will present our finite element simulation results comparing Li-O2 and Li-air batteries using power density, energy density, specific power, and discharge times as metrics to evaluate different electrolytes and electrode geometry to reduce total mass and maximize discharge current. We use a finite element model and a discharge product model developed in which is based on porous electrode and concentrated electrolyte theories and the discharge product is modeled using quantum tunneling; for reaction kinetics and oxygen diffusion, an improved model was used. The electrolyte properties such as ion conductivity and ion diffusion were obtained from Molecular Dynamics (MD) simulations while the other parameters for the finite element model were calibrated to match experiments at high discharge current densities (>1.5 mA/cm2). The mass densities of different electrolytes were computed using MD simulations as well. For this presentation, we examine the practical electrochemical mass of a system at different current ratings, the sensitivity of mass to the use of ambient air as compared to pure oxygen as well as the electrolyte, which affects maximum current density and the total mass associated with the electrolyte (which includes the mass of additional components), and, the optimization of battery geometry for total discharge time, average discharge voltage, maximum discharge current, and minimum electrochemical mass.

Mehta, M.↗
DOE OSTI2024

Modeling Diurnal and Annual Ethylene Generation from Solar-Driven Electrochemical CO 2 Reduction Devices

Integrated solar fuels devices for CO 2 reduction (CO 2 R) are a promising technology class towards achieving net-negative carbon emissions. Designing integrated CO 2 R solar fuels devices requires careful co-design of electrochemical and photovoltaic components as well as consideration of the diurnal and seasonal effects of solar irradiance, temperature, and other meteorological factors expected for ‘on-sun’ deployment. Here, using a photovoltaic-electrochemical (PV-EC) platform, we developed a temperature and potential-dependent diurnal and annual model using experimental CO 2 R performance of Cu-based electrocatalysts, local meteorological data from the National Solar Radiation Database (NSRD), and modeled performance of commercial c-Si PVs. We simulated diurnal product outputs with and without the effects of ambient temperature to determine gaseous product temperature sensitivity. From these outputs, we observed seasonal variation in gaseous product generation, with up to two-fold increases in ethylene productivity between the Winter and Summer, analyzed the consequences of dynamic cloud coverage, and identified periods where device cooling/heating mechanisms could be implemented to maximize ethylene generation. Finally, we modeled the annual ethylene generation for a scaled 1 MW solar farm at three different locations (Beijing, CN; Sydney, AUS; Barstow, CA) to determine the consequences of local meteorological climates on PV-EC CO 2 R product output, recording a maximum ethylene output of 18.5 tonne/yr at Barstow. Overall, this model presents a critical tool for streamlining the translation of experimental solar-driven electrochemical research to real-world implementation.

Yap, Kyra M. K.↗
DOE OSTI2021

Advanced PGM-free Cathode Engineering for High Power Density and Durability

Polymer electrolyte fuel cells (PEFCs) are among the most promising technologies for future electric vehicles by using clean H2 with much-improved energy conversion efficiency, longer range, and rapid refueling. However, due to a large amount of platinum group metal (PGM) catalyst used in their electrodes, their prohibitively high cost hinders broad commercialization of PEFCs for transportation. Therefore, there is a critical need to develop low-cost, high-performance PGM-free cathode catalysts that have the potential to dramatically transform the economics of PEFC commercialization by reducing catalyst costs by one to two orders of magnitude. However, before PGM-free cathodes become viable, several technical challenges associated with PGM-free cathodes must be addressed, including insufficient activity and stability of the catalysts, as well as severe water flooding and large transport losses in the electrodes. Overcoming those barriers and ultimately meeting the challenging automotive PEFC performance targets was the focus of this comprehensive research and development effort on new PGM-free cathodes. To this end, we assembled a team including leading researchers from universities and industry with different but complementary expertise and capabilities. The project combined three novel and promising approaches: Advanced metal-organic framework (MOF)-derived M-N-C catalysts with a high activity and impressive durability, Novel PGM-free specific cathode architectures and fabrication strategies capable of addressing the substantial flooding and transport resistances in thicker cathodes by introducing engineered hydrophobicity through additives and support layers, and Advanced electrode ionomers with high proton conductivity for low ohmic losses across the electrode and more uniform catalyst utilization. The implementation of these new materials and electrode designs was supported by a suite of advanced experimental and simulation tools that allows us to identify performance and durability bottlenecks, devise solutions, and establish rational material design and synthesis targets. These methods include advanced electrochemical characterization, high-resolution imaging, and multi-scale modeling. In addition, the project team leveraged a broad cross-section of the ElectroCat consortium’s national laboratory facilities and expertise in advancing these materials and design strategies. Finally, the industry partners on the project facilitated the evaluation of scaled-up synthesis and manufacturing in the United States. Over its four-year period, the project made significant year-over-year advances in PGM-free cathode performance and viability. A combination of high activity and highly durable catalysts were developed through novel catalyst synthesis strategies, which met several performance and durability targets. More specifically, a catalyst prepared from MOFs and Fe2O3 nanoparticles with ammonium chloride and chemical vapor deposition treatments yielded a significant advancement in PGM-free cathode durability. Several novel strategies for fabricating cathodes were demonstrated, including those designed to reduce flooding and thickness of the cells for significantly increased volumetric power density. An optimized cathode with high conductivity ionomer and tuned ink processing for hydrophobicity yielded high fuel cell performance with new levels power density and maximum current. The scientific studies and modeling assessment also provided an outlook for future efforts, including a focus on catalysts with an increased density of the highly stable active sites developed in this project.

08 HYDROGEN↗