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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 523 records · Page 29
All sourcesNASA NTRSDOE OSTI
DOE OSTI2019

Three-Dimensionally Aligned Sulfur Electrodes by Directional Freeze Tape Casting

Rational design of sulfur electrodes is exceptionally important in enabling a high-performance lithium/sulfur cell. Constructing a continuous pore structure of the sulfur electrode that enables facile lithium ion transport into the electrode and mitigates the reconstruction of sulfur is a key factor for enhancing the electrochemical performance. Here, we report a three-dimensionally (3D) aligned sulfur electrode cast onto conventional aluminum foil by directional freeze tape casting. The 3D aligned sulfur-graphene oxide (S-GO) electrode consisting of few micron thick S-GO layers with 10-20 μm interlayer spacings demonstrates significant improvement in the performance of the Li/S cell. Moreover, the freeze tape cast graphene oxide electrode exhibits homogeneous reconfiguration behavior in the polysulfide catholyte cell tests and demonstrated extended cycling capability with only 4% decay of the specific capacity over 200 cycles. Finally, this work emphasizes the critical importance of proper structural design for sulfur-carbonaceous composite electrodes.

25 ENERGY STORAGE↗
DOE OSTI2024

Viability of Additively Manufactured Electrodes for Lithium-Ion Batteries

As the global economy becomes increasingly electrified, the demand for batteries and energy storage is expected to rise significantly, particularly in the transportation and electricity sectors. Lithium-ion batteries (LIBs) are currently the most advanced and widely used technology in this field. Traditionally, LIBs are manufactured using simple 2D planar geometries to maximize production efficiency and minimize costs. However, this approach limits energy density due to the restricted design flexibility of the electrodes. Additive manufacturing (AM) offers a promising solution to enhance the energy density and efficiency of LIBs by enabling the design of architectures that reduce diffusive losses and allow for a greater amount of active material to be incorporated within the same device footprint, thereby minimizing the use of inactive materials. Different AM techniques come with their own set of limitations, including printing speed, material compatibility, and scale, which must be considered when designing electrodes. Scalable and cost-effective methods are particularly important for electric vehicle batteries, while achieving higher energy densities in microbatteries is crucial for the miniaturization of wearable electronics and medical devices. Here, in this study, we simulate various 3D porous electrode designs for LIBs using graphite and nickel manganese cobalt oxide (NMC) electrodes. These designs are selected to represent structures that could be produced using different AM techniques, such as direct ink writing, fused deposition modeling, and stereolithography. Our results indicate that at higher charging rates and increased areal mass loading, 3D structures can outperform traditional 2D electrodes, although the benefits may diminish with more complex designs that are harder to manufacture. The observed gains in energy density are attributed to improved electrode utilization and reduced diffusive energy losses. This comprehensive analysis of structure–performance relationships will provide valuable insights to guide future research on 3D designs, material selection, and AM techniques for additively manufactured battery electrodes.

25 ENERGY STORAGE↗
DOE OSTI2023

Carbon Electrode with Sputtered Au Coating for Efficient and Stable Perovskite Solar Cells

Halide perovskite solar cells (PSCs) represent a low-cost and high-efficiency solar technology. However, most of the highly efficient PSCs need a noble electrode, such as Au, through thermal evaporation. Here it is reported that a sputtered Au electrode on a PSC could damage the organic hole transport layer (HTL) and the perovskite layer. Here, we report a simple, yet effective sputtered gold nanoparticle decorated carbon electrode to fabricate efficient and stable planar PSCs. The sputtered Au layer on the doctor-bladed coated carbon electrode can be directly applied to the perovskite semicells by mechanical stacking. By optimizing the gold thickness, a power conversion efficiency (PCE) of 16.87% was obtained for the composite electrode-based PSC, while the reference device recorded a PCE of 12.38%. The composite electrode-based device demonstrated 96% performance retention after being stored under humid conditions (50-60%) without encapsulation for ~100 h. This demonstrates a promising pathway toward the commercialization of large-scale manufacturable sputtered electrodes for the PSC solar module.

14 SOLAR ENERGY↗
DOE OSTI2019

Quantifying Reaction and Rate Heterogeneity in Battery Electrodes in 3D through Operando X-ray Diffraction Computed Tomography

In composite battery electrode architectures, local limitations in ionic and electronic transport can result in nonuniform energy storage reactions. Understanding such reaction heterogeneity is important to optimizing battery performance, including rate capability and mitigating degradation and failure. Here, we use spatially resolved X-ray diffraction computed tomography to map the reaction in a composite electrode based on the LiFePO 4 active material as it undergoes charge and discharge. Accelerated reactions at the electrode faces in contact with either the separator or the current collector demonstrate that both ionic and electronic transport limit the reaction progress. The data quantify how nonuniformity of the electrode reaction leads to variability in the charge/discharge rate, both as a function of time and position within the electrode architecture. Importantly, this local variation in the reaction rate means that the maximum rate that individual cathode particles experience can be substantially higher than the average, control charge/discharge rate, by a factor of at least 2-5 times. As a result, this rate heterogeneity may accelerate rate-dependent degradation pathways in regions of the composite electrode experiencing faster-than-average reaction and has important implications for understanding and optimizing rate-dependent battery performance. Benchmarking multiscale continuum model parameters against the observed reaction heterogeneity permits extension of these models to other electrode geometries.

25 ENERGY STORAGE↗
DOE OSTI2019

Electron Transfer Kinetics at Graphene Quantum Dot Assembly Electrodes

Electrochemical performance of nanostructured carbon electrodes was evaluated using cyclic voltammetry and a simple simulation model. The electrodes were prepared from soluble precursors by anodic electrodeposition of two sizes of graphene quantum dot assemblies (hexabenzocoronene (HBC) and carbon quantum dot (CQD)) onto a conductive support. Experimental and simulated voltammograms enabled the extraction of the following electrode parameters: conductivity of the electrodes (a combination of ionic and electronic contributions), density of available electrode states at different potentials, and tunneling rate constant (Marcus Gerischer model) for interfacial charge transfer to ferrocene/ferrocenium (Fc/Fc + ) couple. The parameters indicate that HBC and CQD have significant density of electronic states at potentials more positive than -0.5 V versus Ag/Ag + Enabled by these large densities, the electron transfer rates at the Fc/Fc + thermodynamic potential are several orders of magnitude slower than those commonly observed on other carbon electrodes. This study is expected to accelerate the discovery of improved synthetic carbon electrodes by providing fast screening methodology of their electrochemical behavior.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Superfast high-energy storage hybrid device composed of MXene and Chevrel-phase electrodes operated in saturated LiCl electrolyte solution

Development of high power devices with improved energy density is a highly desired target for advanced energy storage applications. Herein we propose a new strategy of triply-hybridized supercapacitive energy storage device composed of hybrid battery–supercapacitor negative electrode [Mo 6 S 8 (Chevrel-phase)/Ti 3 C 2 (MXene)] coupled with positive nanoporous carbon electrode, integrated with novel yet unexplored saturated (14 M) aqueous solution of LiCl. The electrochemical stability window of this electrolyte solution (2.70 V) significantly exceeds the cell voltage (2.05 V) relevant for the asymmetrical (hybrid anode vs. carbon cathode) cells. The aqueous 14 M LiCl solution has far superior characteristics to that of the previously studies 21 m LiTFSI aqueous solution. The paper is also focused on a deep electroanalytical analysis of a peculiar redox/capacitive heterogeneity of hybrid electrodes. It establishes a variety of additivity rules for both differential and integral equilibrium and kinetic characteristics of the charging processes in hybrid electrodes, solving the puzzle of potential distribution of specific electrochemical energy stored the hybrid electrodes. A careful 3-level hybridization design of asymmetric supercapacitive storage devices enabled the integration of battery and supercapacitor materials to get free-standing binderless electrodes suitable for high power/high energy density systems. Studying thoroughly the properties of highly concentrated solutions such as aqueous 14 M LiCl, which are very suitable for different types of supercapacitive devices, combined with profound analyses of the properties of hybrid electrodes, will pave the way for a rational design of very effective devices for energy storage and conversion.

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

Gradient porosity electrodes for fast charging lithium-ion batteries

The tendency of Li plating at the surface of thick graphite electrodes greatly limits their application in electrical vehicle (EV) batteries for fast charging applications. To address this concern, we proposed an innovative gradient porosity architecture to facilitate mass transport and suppress Li plating in the thick anodes for fast charging applications. This concept was approved through a thick 3-layered graphite electrode with the highest porosity in the top layer and the lowest porosity in the bottom layer, in contact with the current collector. Here, the gradient porosity structure in the 3-layered graphite electrodes was confirmed by electron microscopy and mercury porosimetry measurements. Used as the anodes of lithium-ion batteries, 3-layered graphite electrodes demonstrated unprecedentedly rate capability and durability superior to 1-layered electrodes. The post-mortem analysis on the cycled cells shows that 3-layered electrodes can significantly suppress Li plating at a high rate up to 4C, which might be responsible for the improved performance of the derived cells. The excellent electrochemical behaviors of 3-layered graphite electrodes are associated with the favored mass transport originating from the unique gradient porosity structure. This is consistent with theoretical studies showing that gradient porosity lowers the Li-ion concentration gradient in the electrolyte in the region close to the separator and slows down the process of reaching the Li plating threshold.

25 ENERGY STORAGE↗
DOE OSTI2013

Theoretical and experimental study of the bending influence on the capacitance of interdigitated micro-electrodes patterned on flexible substrates

Interdigitated electrodes are common structures in the fields of microelectronics and MEMS. Recent developments in flexible electronics compel an understanding of such structures under bending constraints. In this work, the behavior of interdigitated micro-electrodes when subjected to circular bending has been theoretically and experimentally studied through changes in capacitance. An analytical model has been developed to calculate the expected variation in capacitance of such structures while undergoing outward and inward bending along the direction perpendicular to the electrodes. The model combines conformal mapping techniques to account for the electric field redistribution and fundamental aspects of solid mechanics in order to define the geometrical deformation of the electrodes while bending. To experimentally verify our theoretical predictions, several interdigitated electrode structures with different geometries were fabricated on polymeric substrates by means of photolithography. The samples, placed in a customized bending setup, were bent to controlled radii of curvature while measuring their capacitance. A maximum variation in capacitance of less than 3% was observed at a minimum radius of curvature of 2.5 mm for all the devices tested with very thin electrodes whereas changes of up to 7% were found on stiffer, plated electrodes. Larger or smaller variations would be possible, in theory, by adjusting the geometry of the device. This work establishes a useful predictive tool for the design and evaluation of truly flexible/bendable electronics consisting of interdigitated structures, allowing one to tune the bending influence on the capacitance value through geometrical design.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Activated graphene nanoplatelets as a counter electrode for dye-sensitized solar cells

Activated graphene nanoplatelets (aGNPs) prepared by a hydrothermal method using KOH as activating agent were used as counter electrode for high efficiency dye-sensitized solar cells (DSSCs). After the KOH activation, the scanning electron microscopy image shows that aGNPs demonstrate a more curled, rough, and porous morphology which could contain both micro- and mesopores. The KOH activation changed the stacked layers of GNPs to a more crumpled and curved morphology. The microstructure of large pores significantly increased the electrode surface area and roughness, leading to the high electrocatalytic activity for triiodide reduction at the counter electrode. The DSSCs fabricated using aGNP as counter electrodes were tested under standard AM 1.5 illumination with an intensity of 91.5 mW/cm{sup 2}. The device achieved an overall power conversion efficiency of 7.7%, which is comparable to the conventional platinum counter electrode (8%). Therefore, the low cost and high performance aGNP based counter electrode is a promising alternative to conventional Pt counter electrode in DSSCs.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Designing a hybrid electrode toward high energy density with a staged Li + and PF 6 - deintercalation/intercalation mechanism

Existing lithium-ion battery technology is struggling to meet our increasing requirements for high energy density, long lifetime, and low-cost energy storage. Here, a hybrid electrode design is developed by a straightforward reengineering of commercial electrode materials, which has revolutionized the “rocking chair” mechanism by unlocking the role of anions in the electrolyte. Our proof-of-concept hybrid LiFePO 4 (LFP)/graphite electrode works with a staged deintercalation/intercalation mechanism of Li + cations and PF 6 - anions in a broadened voltage range, which was thoroughly studied by ex situ X-ray diffraction, ex situ Raman spectroscopy, and operando neutron powder diffraction. Introducing graphite into the hybrid electrode accelerates its conductivity, facilitating the rapid extraction/insertion of Li + from/into the LFP phase in 2.5 to 4.0 V. This charge/discharge process, in turn, triggers the in situ formation of the cathode/electrolyte interphase (CEI) layer, reinforcing the structural integrity of the whole electrode at high voltage. Consequently, this hybrid LFP/graphite-20% electrode displays a high capacity and long-term cycling stability over 3,500 cycles at 10 C, superior to LFP and graphite cathodes. Importantly, the broadened voltage range and high capacity of the hybrid electrode enhance its energy density, which is leveraged further in a full-cell configuration.

25 ENERGY STORAGE↗
DOE OSTI2018

Characterization of Surface Free Energy of Composite Electrodes for Lithium-Ion Batteries

One critical step in lithium-ion battery manufacturing process is the electrolyte wetting step, which usually takes up to several days at elevated temperatures, posing a distinctive bottleneck in the manufacturing process especially for large-size cells. The electrode wettability depends on both the surface tension of electrolyte and the surface free energy of electrodes. This work reports a systematic study on the characterization of surface free energy of battery electrodes and the correlation between surface free energy and electrode processing. It shows that, when switching manufacturing from conventional solvent based processing to aqueous processing, the polar component of surface free energy increases 74.1% for NMC532 electrodes and 48.2% for A12 graphite electrodes. The results provide valuable guidance for electrode processing to optimize the electrolyte wetting process, helping lower processing costs and enable higher product quality and throughput.

25 ENERGY STORAGE↗
DOE OSTI2018

Fabrication of Enhanced Pinch Weld Electrodes

Savannah River Site uses brazed copper / tungsten electrodes for a specialized weld referred to as a pinch weld. As part of an internally funded PDRD program, an alternative method to produce the pinch weld electrodes was sought to improve quality and to reduce the manufacturing steps. Back casting of pinch weld electrodes was selected as such a process. During preliminary testing, deformation of the electrodes was observed. A failure analysis was conducted, and the strength of the electrodes was found to be significantly less than required to enable welding of the tubes. This assessment includes compression testing metallographic analysis. The pinch weld electrodes fabricated by back casting do not meet the requirements with respect to strength. In addition, a minimum strength requirement for conventionally prepared electrodes is recommended.

42 ENGINEERING↗
DOE OSTI2025

Acoustophoretic Additive Manufacturing for Scalable 3D Battery Electrodes

This project focused on investigating two acoustic-based processing methods: a nozzle-based printhead and a chamber that map to two different battery electrode architectures: (1) a line-pattern electrode and (2) a grid-pattern electrode. These two parallel manufacturing and electrode geometry explorations were proposed for the project to understand the process space of acoustic-based manufacturing methods to fabricate patterned battery electrodes. This two-path exploration also allowed us to de-risk the overall project and not rely on a single process for creating patterned electrodes. This project consisted of six high-level tasks aimed at transitioning the concept of acoustic focusing for battery electrodes from a technology readiness level (TRL) of 1 to 3 by project conclusion. Overall, we believe we have developed a practical and high-impact processing method that is chemistry agnostic and suitable for large-area fabrication of both 3D LIBs and other functional material systems where structuring on the scale of tens of microns has the potential to break conventional bulk material trade-offs in performance. In the case of batteries for electric vehicles, structuring 3D LIBs with our acoustic process breaks traditional energy and power trade-offs observed with conventional flat battery packs.

25 ENERGY STORAGE↗
DOE OSTI2021

Stamping Nanoparticles onto the Electrode for Rapid Electrochemical Analysis in Microfluidics

Electrochemical analysis is an efficient way to study various materials. However, nanoparticles are challenging due to the difficulty in fabricating a uniform electrode containing nanoparticles. We developed novel approaches to incorporate nanoparticles as a working electrode (WE) in a three-electrode microfluidic electrochemical cell. Specifically, conductive epoxy was used as a medium for direct application of nanoparticles onto the electrode surface. Three approaches in this work were illustrated, including sequence stamping, mix stamping, and droplet stamping. Shadow masking was used to form the conductive structure in the WE surface on a thin silicon nitride (SiN) membrane. Two types of nanomaterials, namely cerium oxide (CeO2) and graphite, were chosen as representative nanoparticles. The as-fabricated electrodes with attached particles were characterized using atomic force microscopy (AFM) and time-of-flight secondary ion mass spectrometry (ToF-SIMS). Electrochemical analysis was performed to verify the feasibility of these nanoparticles as electrodes. Nanomaterials can be quickly assessed for their electrochemical properties using these new electrode fabrication methods in a microfluidic cell, offering a passport for rapid nanomaterial electrochemical analysis in the future.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRSDate not supplied

Layered Electrode Architectures Enabled by Holey Graphene Hosts

Battery electrodes are typically prepared using a slurry-based method, where high boiling point organic solvents are typically used with a polymer binder to disperse active electrode materials and conductive carbon additives followed by casting into current collector sheets. In this process, the use of organic solvents are environmentally hazardous, energy intensive, and time-consuming, while polymeric binders add weight and can undergo parasitic reactions during battery cycling. Here we discuss the use of a unique conductive carbon nanomaterial, namely holey graphene, as a multifunctional host that can be processed via a facile, solvent-free, binder-free, cold pressing method to prepare electrodes with unique architectures. This approach can accommodate a broad range of battery chemistries, such as lithium oxygen/carbon dioxide (Li-O2/CO2), lithium sulfur/selenium (Li-S/Se), and various lithium ion chemistries. The successful use of dry, cold compression allows the convenient modification of electrode mass loading with unique architectures containing active materials randomly mixed or layered with single or multiple layers of one or more active materials. In the conventional slurry-based electrode fabrication method, it is difficult, if not impossible, to achieve such layered architectures. In particular, the layered electrode architectures from the dry, cold press approach are easy to fabricate without significantly sacrificing device performance, and are amenable to continuous roll-to-roll dry processing. In addition, these architectures offer unprecedented perspectives on the battery material loading vs. utilization efficiency, as well as enabling unique characterization opportunities to advance mechanistic understanding of various battery chemistries. Potential applications of this unique electrode fabrication approach for solid-state batteries will also be discussed.

holey graphene, batteries, electrode architecture,↗
DOE OSTI2024

The influence of electrode crack dimensions on the durability of polymer electrolyte membrane fuel cells

Electrode cracks in polymer electrolyte membrane fuel cells (PEMFCs) are correlated with early onset failures. Here, in this work we investigate the influence of cracked gas diffusion electrodes (GDEs) on the durability of the membrane electrode assembly (MEA) using a combined chemical-mechanical accelerated stress test (AST). Electrode crack dimensions were systematically tuned using ink formulations and material selection strategies. A parameter to describe the crack width areal density (Φ CW ) was used to quantify the degree of discontinuity in the electrode surfaces. Open circuit voltage (OCV) transient analyses were used to benchmark and characterize the failure mechanisms in the MEAs as a function of the Φ CW . While smaller electrode-level cracks, on the order of microns, yielded a 28 % decrease in operating lifetime, larger cracks that propagated from a discontinuous, microporous layer (MPL) coating, decreased the operating lifetime by 56 %. This work emphasizes the need for material processing strategies that consider defect tolerances to limit membrane failures in PEMFCs.

08 HYDROGEN↗
DOE OSTI2015

Regulated Breathing Effect of Silicon Negative Electrode for Dramatically Enhanced Performance of Li-Ion Battery

Si is an attractive negative electrode material for lithium ion batteries due to its high specifi c capacity (≈3600 mAh g –1 ). However, the huge volume swelling and shrinking during cycling, which mimics a breathing effect at the material/electrode/cell level, leads to several coupled issues including fracture of Si particles, unstable solid electrolyte interphase, and low Coulombic effi ciency. In this work, the regulation of the breathing effect is reported by using Si–C yolk–shell nanocomposite which has been well-developed by other researchers. The focus is on understanding how the nanoscaled materials design impacts the mechanical and electrochemical response at electrode level. For the fi rst time, it is possible to observe one order of magnitude of reduction on breathing effect at the electrode level during cycling: the electrode thickness variation reduced down to 10%, comparing with 100% in the electrode with Si nanoparticles as active materials. The Si–C yolk–shell nanocomposite electrode exhibits excellent capacity retention and high cycle effi ciency. In situ transmission electron microscopy and fi nite element simulations consistently reveals that the dramatically enhanced performance is associated with the regulated breathing of the Si in the new composite, therefore the suppression of the overall electrode expansion.

Environmental Molecular Sciences Laboratory↗
DOE OSTI2025

Recent Advances in Scalable, High‐Mass Loaded Electrodes for Grid‐Scale Energy Storage

Abstract The increasing electrification of daily life as well as the intermittent characteristic of renewable energy sources require viable solutions for grid‐scale energy storage. Critical considerations for grid storage applications are electrode mass loading and electrode thickness as these features govern battery pack energy density, an important factor in determining manufacturing costs. For this reason, there is increased interest in finding new ways of creating electrodes with high mass loading. In this review, various high‐mass loading fabrication approaches are considered for positive electrode materials used in batteries. The benchmark used for high mass loading is above 20 mg cm −2 , which is higher than the practical limit of conventional tape‐cast electrodes. Several different electrode approaches are described including templating, laser patterning, direct ink writing, and electrodeposition. A variety of materials are covered with the most prominent being LiFe(PO 4 ) (LFP), LiCoO 2 (LCO), and MnO 2 . In research to date, scalable electrochemical performance has been achieved with mass loadings over 100 mg cm −2 . Areal capacities as high as 14.7 mAh cm −2 at 1.82 mA cm −2 have been achieved in non‐aqueous electrolytes and 9.8 mAh cm −2 at 10 mA cm −2 in aqueous electrolytes. These results establish that the mass loading of electrodes can be scaled up without compromising their electrochemical properties.

White, Makena [Department of Materials Science and↗