Search NASA⌕ Search

SEARCH · Search NASA

Results for “Localized concentrated electrolyte”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

170 records · Page 10

Morphology and Transport of Multivalent Cation-Exchanged Ionomer Membranes Using Perfluorosulfonic Acid–Ce Z+ as a Model System

Perfluorosulfonic acids (PFSAs) are commonly used as solid polymer electrolyte membranes (PEMs) in electrochemical energy devices, where they are vulnerable to attack by radical species during operation. A popular strategy to combat this problem is to introduce radical scavengers like cerium (Ce) ions that neutralize these species before they attack the PFSA. Such cation doping creates a multi-ion system, in which understanding the mechanisms of cation solvation and transport becomes important for the effective design and utilization of PFSA–cation systems. Ce ions also provide a representative model system for multication-exchanged ionomers in electrochemical systems. In this study, hydration and conductivity measurements, along with X-ray fluorescence and scattering, are employed to elucidate how Ce ion exchange alters PFSA’s ionic solvation, as well as nano- and mesoscale morphologies, which ultimately control its ion transport properties. A molecular transport model is used to deconvolute the impact of Ce ions on the local solvation structure of water in the membrane from mesoscale changes of the transport pathways. The combined experimental and theoretical analysis reveals a nonlinear decrease in conductivity driven by cation solvation at the molecular level and morphological changes at longer length scales. Migration–diffusion coupling, its nonlinear dependence on ion exchange and hydration, and its overall implications for ionomer performance are also discussed. Finally, these findings have the potential to be translated into other mixed cation–ionomer systems for a wide range of energy and environmental devices.

36 MATERIALS SCIENCE↗

Ion Size Effects on the Thermodynamic, Kinetic, and Mechanical Properties during Ion Exchange in Solid-State Electrolytes

Ion exchange offers a pathway to impose residual compressive stresses to mitigate the electro-chemo-mechanical cracking of solid-state electrolytes such as lithium lanthanum zirconium oxide. This study uses a coupled multiscale framework (integrating density functional theory (DFT), molecular dynamics (MD), and continuum modeling) to examine how exchange ion size influences stress, diffusion, fracture toughness, and electronic properties. Larger isovalent ions (Na + , Ag + , K + ) were exchanged with Li + , with DFT confirming their preference for octahedral 96h sites and a linear relationship between ion size and chemical free expansion coefficient. MD simulations reveal stress and concentration effects on exchange ion diffusivity at elevated temperatures, with Na + and Ag + maintaining favorable mobility while K + showing concentration-dependent clustering. Continuum modeling predicts the range of fracture strength improvements and the required ion exchange concentration profile. It was shown that a 5% surface exchange concentration can induce ∼0.6 GPa of surface compressive stress using Na + and ∼1.0 GPa of surface compressive stress using Ag + . On the other hand, larger ion exchange species may penalize Li + diffusivity by increasing the activation volume and activation energy. Interestingly, Na + has a negligible penalty on Li-ion diffusivity. The room temperature Li + ion diffusivity is reduced by ∼40% with Ag + ion exchange. Electronic band structure analysis shows no size-dependent change in the bandgap, though Ag + introduces localized defect states near the valence band maximum. This study highlights ion size as a key factor in optimizing LLZO properties, offering a framework to improve the solid-state battery performance.

Jagad, Harsh D. [Brown Univ., Providence, RI (Unit↗

Bipolar Membranes for Ion Management in (Photo)Electrochemical Energy Conversion

Conspectus (Photo)electrochemical energy conversion is important in the development of a carbon-neutral energy economy because it can provide a pathway for mitigating the intermittency of renewable energy sources such as wind and solar. In order to operate efficiently, these technologies, which include photoelectrochemical cells, water and CO 2 electrolyzers, fuel cells, and redox flow batteries, require fast charge transfer kinetics at the electrode/electrolyte interface as well as robust ion management in the electrolyte. In conventional electrolyzers and fuel cells, the electrolyte is strongly acidic or basic and ionic current is carried by H + or OH – ions. In contrast, photoelectrodes and electrocatalysts for water splitting are often studied in buffered solutions. The question of ion balance in these systems led us to analyze the polarization losses due to ion concentration gradients in cells that employed various buffer–membrane combinations. Continuously driving the buffer ions across an ionomer membrane not only lowers the buffer capacity of an aqueous electrolyte but also introduces pH gradients that result in significant energy losses. To address the problem, we and other groups have studied the use of reverse-biased bipolar membranes (BPMs) in (photo)electrolytic cells. BPMs consist of an anion exchange layer (AEL) laminated with a cation exchange layer (CEL) and are usually equipped with a catalytic layer in between to accelerate the water dissociation reaction. At the AEL/CEL interface, water dissociates into protons and hydroxide ions, which replenish those consumed at the cathode and anode. Compared to conventional water electrolyzers with proton/anion exchange membranes (PEM/AEM), BPM electrolyzers provide the unique advantage of continuously operating the cathode and anode under different pH conditions, which is desirable when the two electrode reactions have different pH requirements. BPMs also enable the use of buffered electrolytes at pH values that are optimized for electrode stability and product selectivity in applications such as CO 2 electrolysis. Product crossover losses and CO 2 pumping can be dramatically reduced in BPM-based CO 2 electrolyzers, relative to conventional alkaline membranes, by electrostatic repulsion (of anionic products) and electroosmotic drag (for neutral products). BPM-based gas fed CO 2 electrolyzers can achieve high current density, but they suffer from low Faradaic efficiency (FE) due to the acidic local environment of the CEL. This problem can be mitigated by adding an aqueous buffering layer or by creating a weak acid cation exchange film on the CEL face of the membrane. The use of BPMs in fuel cells and redox flow batteries offers some interesting advantages. Configurations with both reverse and forward bias have been studied, but forward bias has been favored due to material compatibility, reaction kinetics, and thermodynamic considerations. The net reaction at the AEL/CEL interface is the acid–base neutralization reaction, which has a high inherent reaction rate constant, but in the BPM is limited to a nanometric space-charge layer and requires efficient catalysis to achieve high current density. Understanding the mechanism of the acid–base neutralization and the opposite process, the water dissociation reaction, will be essential for improving the performance of forward-biased BPMs. In conclusion, this Account reviews our current understanding of the working mechanisms of BPMs and discusses how we can use them to effectively manage ions for various (photo)electrochemical applications.

Yan, Zhifei↗

Nanostructures for Electrical Energy Storage (NEES) (2020 Final Technical Report)

Nanostructures for Electrical Energy Storage (NEES, www.efrc.umd.edu) was an Energy Frontier Research Center supported by the DOE Office of Science, Basic Energy Sciences, from 8/1/2009 to 7/31/2020. Led by the University of Maryland, NEES enjoyed extensive collaborations with its funded partners, including two DOE Laboratories and six universities. The NEES vision has been to reveal a set of scientific insights and design principles that can underpin a next-generation electrical energy storage approach, building on advances in nanoscale science and technology to achieve simultaneous high power and high energy over extended charge/discharge cycling. The vision is motivated by the recognition that scaling into the nano regime opens the door to new physical phenomena and that the tools enlisted in nanoscale research provide major new opportunities for the synthesis not only of materials at molecular scale but for structures at nano scale and above. NEES has translated this vision into its research program based on two observations. First, while the behavior of ions and electrons in electrolytes and in electrode materials is crucial to electrical energy storage (or more appropriately electrochemical energy storage), it is the transport of ion and electron charge between different structural components of a storage device that ultimately determine its performance. With it well recognized that the choice of electrode materials typically constrain ion transport kinetics as well as maximum ion concentration, the search for better electrode materials has been a primary driver of battery research. At the same time the synthesis of electrodes is typically based on aggregation of particles with varying size, shape, and orientation in the electrode. Together with the presence of additional materials to impart electrical conductivity and cohesion to the composite electrode, change in electrode materials is necessarily accompanied by structural changes at the nano/micro scale that are difficult to categorize and manage. From the beginning, NEES’ vision has been to create and study simpler, highly controlled spatial arrangements of known materials as battery components (electrodes, current collectors, and electrolyte) and to understand how design and structure above the molecular scale determines the energy storage performance available from known materials. Second, advances in nanoscience dramatically expanded the portfolio of synthesis methods, structural motifs, and new phenomena available for research. Some of these gave rapid access to new building blocks at the deep nanoscale (e.g., carbon nanotubes grown by self-assembly, nanoscale arrays formed by electrochemical self-alignment, monolayer films controlled by self-limiting reaction). Such advances served as the enabler for the NEES vision to be pursued experimentally through study of 3D structures created and controlled at the nano, micro, and meso scales. Here, we use meso as in the BES MESO Report, implying not only intermediate or varying length scales, but very much the way behavior is influenced by other factors including aggregation of nanocomponents at different densities and spatial configurations, statistical variations in the aggregates, hierarchical architectures in which they can be assembled, or local 3D configurations that result from the architectures. Over its life cycle, NEES has pursued two overarching goals: (1) to understand the scientific fundamentals of electrochemical storage from the nanoscale to the mesoscale; and (2) to create and learn from innovative, controlled, heterogeneous nanostructures, where such nanostructures can enable the first goal and serve as models for future paradigms in energy storage. Specific goals have included: Synthesize heterogeneous nanostructures comprised of multiple materials arranged in controlled fashion and characterize their behavior; Demonstrate and elucidate design principles for achieving simultaneous high power and high energy; Develop materials processes which enable precision control of thin layers and 3D structures; Investigate the impact of artificial interphases on electrode stability during ion insertion/deinsertion; Create dense arrays of nanostructures to understand how the architecture of these assemblies, along with nanostructure design, influences energy storage behavior at the mesoscale; Identify and understand the consequences of nanoconfinement and local inhomogeneities in 3D mesoscale arrays; Develop and apply computational models to stimulate, guide and interpret experiments.

25 ENERGY STORAGE↗

Microstructure‐Dependent Sodium Storage Mechanisms in Hard Carbon Anodes

Sustainable energy storage is essential to support the transition to renewables and meet the increasing demand for energy. Sodium‐ion batteries (NIBs) are attractive for grid‐scale energy storage due to the abundance and low cost of sodium, sustainability of other battery components, and electrochemical performance. Hard carbon (HC) is a leading anode material for NIBs, but its complex microstructure complicates the understanding of sodium storage mechanisms. Using X‐ray total scattering and density functional theory calculations, this study clarifies how HC's microstructural variations influence sodium storage across the slope (high potential) and plateau (low potential) regions of the potential capacity curve. In the slope region, sodium initially adsorbs at high‐binding energy defect sites and subsequently intercalates between graphene layers, adsorbing at low‐binding energy defect sites, correlating with different slopes observed during initial sodiation. Initial irreversibility arises from sodium trapping at surface defects and solid electrolyte interface formation. In the plateau region, sodium simultaneously intercalates and fills pores, influenced by pore size, interlayer spacing, and defect concentration. HCs with larger pore sizes form larger sodium clusters. In conclusion, the proposed mechanism underscores the role of microstructure engineering in enhancing HC performance and advancing NIBs for grid‐scale energy storage.

36 MATERIALS SCIENCE↗

Evaluation of Amorphous Oxide Coatings for High-Voltage Li-Ion Battery Applications Using a First-Principles Framework

Cathode surface coatings are widely used industrially as a means to suppress degradation and improve electrochemical performance of lithium-ion batteries. However, developing an optimal coating is challenging, as different coating materials may enhance one aspect of performance while hindering another. Furthermore, to elucidate the fundamental thermodynamic and transport properties of amorphous cathode coating materials, here, we present a framework for calculating and analyzing the Li + and O 2- transport and the stability against delithiation in such materials. Our framework includes systematic workflows of ab-initio molecular dynamics calculations to obtain amorphous structures and diffusion trajectories coupled with an analysis of critical changes of the active-ion local environment during diffusion. Based on these data, we provide an estimate of room-temperature diffusivities, including statistical error bars, and the evaluation of the coating suitability in terms of its ability to facilitate Li + transport while blocking O 2- transport. Finally, we add the thermodynamic stability analysis of the coating chemistry within the operating voltage of common Li-ion cathodes. We apply this framework to two commonly used amorphous coating materials, Al 2 O 3 and ZnO. We find that (1) in general, a higher Li + content increases both Li + and O 2- diffusivities in both Al 2 O 3 and ZnO. Also, Li + and O 2- diffuse much faster in ZnO than in Al 2 O 3 . (2) However, neither Al 2 O 3 nor ZnO is expected to retain a significant concentration of Li + at high charge. (3) ZnO performs much more poorly in terms of O 2- blocking, and hence, Al 2 O 3 is preferred for high-voltage cathode applications. These results will help to quantitatively evaluate amorphous materials, such as metal oxides and fluorides, for different performance metrics and facilitate the development of optimal cathode coatings.

25 ENERGY STORAGE↗

Spatially Patterned Architectures to Modulate CO 2 Reduction Cascade Catalysis Kinetics

Electrochemical CO 2 reduction using renewable sources of electrical energy holds promise for converting CO 2 into fuels and chemicals. The complex interactions among chemical/electrochemical reactions and mass transport make it difficult to analyze the effect of an individual process on electrode performance based only on experimental methods. Here, we developed a generalized steady-state simulation to describe an electrode surface in which sequential cascade catalysts are patterned in a periodic trench design. If appropriately constructed, this trench geometry is hypothesized to be able to yield a higher net current density for a CO 2 reduction (CO 2 R) cascade reaction. We have used realistic experimental reaction kinetics to investigate the role of trench geometry in mass transport, local microenvironments, and selectivity for a model CO 2 R cascade reaction. The model considers local concentration gradients of bicarbonate species at quasi-equilibrium and catalytic surface reactions based on concentration-dependent Butler–Volmer kinetics. Our results suggest that varying the spatial distribution of active sites plays a significant role in facilitating effective mass transport between active sites, modulating selectivity for the cascade reaction, and enhancing the yield of desirable cascade products. Moreover, we observe that this trench geometry significantly alters the cascade reaction rate by affecting the local pH, which can cause inadvertent depletion of available aqueous CO 2 to limit the CO 2 R cascade kinetics and modest suppression of the hydrogen evolution reaction (HER). The results highlight the trade-offs between mass transport, pH, and reaction kinetics that become apparent only when considering the coupled physics of all processes at the electrode surface. Here, this model can thus serve as a primary tool to build more selective and efficient patterned architectures for the CO 2 R cascade catalysis.

CO2 reduction↗

Technology Strategy Assessment: Findings from Storage Innovations 2030 Bidirectional Hydrogen Storage

Hydrogen is the most common element in the universe, comprising nearly 75% of all normal matter, and it has been used by scientists for centuries, but it was not fully recognized as an element until 1766, when it was isolated by Henry Cavendish. Early work focused on the generation of hydrogen through the oxidation of metals in water, which released hydrogen gas. Hydrogen’s lighter-than-air and flammable properties were immediately used in engines, zeppelins, and as feedstock for a wide variety of chemical reactions. Several approaches were developed for the production of hydrogen with the most common being associated with the production and conversion of hydrocarbon-based fuels. Coal gasification, steam methane reforming, and other reformation processes provide the majority of current hydrogen production due to the relatively low cost of hydrogen produced through these processes. More than 95% of hydrogen production is used for industrial processes rather than energy storage. To facilitate affordable decarbonization of these industrial processes and to advance the use of hydrogen as a fuel in transportation, DOE launched the Hydrogen Shot as part of the Energy Earthshots Initiative. The goal of the Hydrogen Shot is to reduce the cost of clean hydrogen by 80% to $1/kg of clean hydrogen production within one decade (known as the “1 1 1” goal). This is distinct from the Long-Duration Storage Shot, which is the primary focus of this report; however, it is intrinsically linked to bidirectional hydrogen storage. Several important chemical synthesis processes are dependent upon hydrogen, and the production and use of hydrogen is generally driven by its connection to one of these markets. For example, ammonia is one of the most highly produced chemicals in the world and it depends chiefly on hydrogen. Ammonia is primarily used for agricultural fertilizer and is considered to be largely responsible for a doubling of agricultural production per unit of land over the last century. Another one of hydrogen’s primary uses is as a catalyst in petroleum refining during the desulfurization process. Beyond chemical production, hydrogen is used as a reductant in the production of steel and has been demonstrated as a substitute for metallurgical coal in the production of raw iron. It is even used in the hydrogenation reaction for food products to create more shelf-stable semi-solid fats. However, while hydrogen is produced on the order of 100 million metric tons/year globally to feed these industries, more than 95% of hydrogen is produced from hydrocarbons that emit CO2 during the process. Conversely, electrolysis is a process by which electricity is used to separate hydrogen and oxygen in water molecules, usually across a membrane. Hydrogen production via electrolysis lowers the carbon intensity of produced hydrogen when coupled with low-carbon electricity. Currently, global electrolysis capacity is on the order of 1 GW, which equates to about 500 metric tons/day of hydrogen production. To support large-scale industrial decarbonization, capacity will likely need to increase by two to three orders of magnitude. Electrolysis technology is broadly separated into groups that are defined by the electrolyte used, with further subdivision based on the operating characteristics. The majority of commercial electrolyzer systems are based around three main technology groups: liquid alkaline, proton exchange membrane, and solid oxide. Liquid Alkaline (LA) electrolysis is the oldest, most mature, least expensive, and most common commercial technology, with 400 plants in operation by 1902. Its hydrogen output is low relative to the size of the system due to a low current density. LA electrolysis utilizes a liquid potassium hydroxide solution as the electrolyte. Proton exchange membrane (PEM) electrolysis (also known as polymer electrolyte membrane electrolysis), described in 1960, relies on an acid-impregnated polymer membrane as the electrolyte and typically offers three to six times higher hydrogen production per unit cell area than LA electrolysis. Solid oxide electrolysis, or high-temperature electrolysis, utilizes a ceramic cell as the electrolyte and operates on steam rather than liquid water, enabling electrical efficiencies of more than 90%, which is up from 60% with PEM. Two pre-commercial electrolyzer technologies to note are alkaline exchange membrane (AEM) and proton-conducting solid oxide electrolysis cell (SOEC). AEM potentially has the advantages of both LA and PEM technologies in that it is able to use low-cost materials like LA but with the ability to operate at higher output pressures with a smaller footprint like PEM. Proton-conducting SOEC is similar to commercial SOEC, which uses an oxide-conducting ceramic; however, it uses a proton-conducting ceramic that has the potential to operate at lower temperatures and has lower capital costs. Each of these technologies is experiencing a rapid improvement in performance and a reduction in installed cost, and each appears to be well suited to specific applications. Besides differences in the type of electrolyzer used, the main difference in the architecture of bidirectional hydrogen systems is how the hydrogen is stored. Currently, the most cost-effective way to store large amounts of hydrogen gas is underground, such as in large salt caverns that have been hollowed out. These salt caverns are geographically concentrated in small portions of the United States and are not generally near large metropolitan areas; however, other subsurface architectures are being investigated to expand this reach. A more widely deployable option is aboveground pressurized tanks. These systems are about 10 times as expensive because of the materials and safety margins required to hold hydrogen at high pressures. A third option is using materials-based storage, such as liquid organic hydrogen carriers. By reversibly attaching the produced hydrogen to other molecules, it can be stored at near atmospheric pressure and room temperature. This has the potential to reduce the material cost of storage but may result in a reduction in the efficiency of the process because there are both hydrogen uptake and release processes. While materials-based storage has not been used extensively for large-scale hydrogen storage in the past, there is currently significant activity regarding developing materials and processes for use in large-scale hydrogen storage applications. Electrolysis-produced hydrogen offers an unusual opportunity for energy storage applications. Unlike more conventional energy storage approaches, such as batteries, which operate entirely within electrical markets, hydrogen is a valuable product beyond the electric market and can be directed to the most lucrative use. Hydrogen also can be directly converted back to electricity using either a fuel cell or turbine, or it can be sold to other markets, such as chemical synthesis, steel production, or even export. In this way, excess electricity can be upgraded to the most valuable product. Finally, its use can be actively managed between multiple off-takers; for example, local hydrogen storage can provide a specific amount of stored electricity and any excess can be exported to ammonia production. This flexibility is amplified by the fact that hydrogen storage has fully decoupled power and energy components, which allows for affordable scaling options. Together, this allows a substantial amount of creativity to enable the economic utilization of variable power resources while supporting decarbonization of the industry.

08 HYDROGEN↗