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At least 1,387 records · Page 77
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Lignin-Derived Methoxyterephthalates for Performance-Advantaged Polymers and Plasticizers

Lignin-derived aromatic carboxylic acids can be produced from oxidative catalytic processes and are promising building blocks for performance-advantaged bioproducts that leverage their inherent heteroatom functionalities. Here, we synthesize 2-methoxyterephthalate and 2,6-dimethoxyterephthalate derivatives by electrochemical carboxylation of guaiacyl- and syringyl-derived lignin monomers obtained from the oxidative deconstruction of lignin. These methoxylated terephthalates are evaluated as comonomers in poly(ethylene terephthalate) (PET) and as plasticizers that could replace petrochemically-derived isophthalate and phthalate, respectively. Specifically, we copolymerize 2-methoxy- and 2,6-dimethoxyterephthalate with dimethyl terephthalate to form several PET copolymers, both of which enable the properties of PET to be tuned, with an incorporation beyond 25% producing amorphous polyesters. At 10 mol % loading in the copolymers, we demonstrate that the bioderived comonomers exhibit comparable behavior to isophthalic acid, a commonly used comonomer in PET, by lowering the crystallinity and melting temperature. Moreover, methoxyterephthalate esters (2-ethylhexyl and butyl) are compared to phthalate and terephthalate ester counterparts used as poly(vinyl chloride) (PVC) plasticizers. The bioderived plasticizers are comparable to the petroleum-derived incumbents in reducing the glass transition temperature and increasing the thermal stability of PVC. Furthermore, the dimethoxyterephthalic esters are expected to have an extended lifetime in the polymer matrix due to their lower volatility and lower diffusion coefficients calculated by molecular dynamic simulations. These results demonstrate that the isophthalate and phthalate components in polyesters and plasticizers, respectively, could be substituted with biobased methoxyterephthalate derivatives.

09 BIOMASS FUELS↗
DOE OSTI2024

Manufacturing Cathodes via Dry-Processing for Lithium-Ion Batteries

Conventional lithium-ion battery (LIB) electrodes are prepared through a wet slurry process with n-methyl pyrrolidone solvent, especially for cathodes. The wet slurry process encounters several disadvantages such as binder migration, electrode cracking in thick electrodes, energy intense heat-dry NMP solvent removal, and costly NMP recovery. The cost and energy consumption of coating and drying of electrode are about 11.5 % and > 46 % in LIB manufacturing, respectively. Thereby, it is essential to develop a facile roll-to-roll solvent-free LIB electrode processing for reducing the cost and energy consumption. Recently, the Maxwell-type dry processing (DP) shines new lights on LIB manufacturing, which mainly bases on dry mixing (DM) of electrode component powder followed by calendering into electrode films and laminating onto current collectors, realizing the rapid manufacturing of LIB electrodes in a powder-to-film manner for industries. This report shares some recent progress on the DP from our group. We aim to further advance the manufacturing science of DP by correlating the processing conditions with electrode properties and performance. Particularly, we investigate the effect of DM, and compression on the polytetrafluoroethylene (PTFE) binder fiberization, porosity, mechanical properties, electrical conductivity and electrochemical behaviors of electrodes. The DM study suggests that PTFE fiberization heavily relies on the degree of DM. Insufficient DM results in poor PTFE fiberization while outrageous DM damages the formed PTFE fibers. Both negatively affect the mechanical behaviors of the electrodes and their rate capability. However, moderate DM is highly beneficial. In addition, our study of the porosity impact reveals that LiNi0.8Mn0.1Co0.1O2 (NMC) secondary particles can be broken into primary particles due to compression, especially at low porosity. Those fractured NMC secondary particles exhibit lower modulus. We propose that a moderate porosity of around 32% favors the electronic conductivity, charge transfer impedance and rate capability. The study of the cathodic electrolyte interphase layer of PTFE-based DPed electrode confirms that side reactions of PTFE binder due to the formation of LiF in LiClO4-based electrolyte.

Tao, Runming↗
DOE OSTI2020

Plasma enhanced atomic layer deposition of thin film Li 1+x Mn 2-x O 4 for realization of all solid-state 3D lithium-ion microbatteries

Here, the plasma enhanced atomic layer deposition (PEALD) process for MnO 2 was demonstrated, exhibiting self-limiting growth as well as stable composition and stable growth rate over a temperature window of 205–265 °C. The PEALD process for MnO 2 was combined with the thermal ALD process for LiOH to synthesize Li 1+x Mn 2-x O 4 thin film cathodes, where the stoichiometry was effectively controlled to allow for crystallization in the electrochemically active spinel phase. A 3D nanostructure consisting of an Li 1+x Mn 2-x O 4 cathode layer, ALD Li x Al y Si z O solid electrolyte, and SiGe nanowire anode was fabricated and characterized via TEM. The Li 1+x Mn 2-x O 4 thin films maintained 66% of the areal capacity upon a 100× increase in the rate (4–360 μ A cm -2 ) as well as 97% capacity retention over 100 cycles at ~5C. The ALD Li 1+x Mn 2-x O 4 thin films exhibited a volumetric capacity of 52 μ Ah cm -2 μ m -1 at a C-rate of ~0.5C and, coupled with the high operating voltage (4.0 V), offer some of best areal energy densities for ALD thin film cathodes, making it a viable material for integration with 3D lithium-ion microbatteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Status Report on the Electroreduction of Metal Oxides

SRNL is working with Argonne National Laboratory (ANL) to adapt and demonstrate the electroreduction technology. SRNL will also draw on the extensive work cited in the literature and the experience gained at Y-12. Since most of the development efforts have focused on irradiated UO 2 fuel pellets, several noteworthy gaps exist in the technology for processing purified U 3 O 8 powder. SRNL research efforts will address some of those gaps. This report focuses on two activities. Task 1 is to establish an electrochemical reduction test capability at SRNL. Task 2 is to evaluate potential alternate anode materials.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2024

Elucidating the Link Between Alkali Metal Ions and Reaction-Transport Mechanisms in Cathode Electrodes for Alkali-ion Batteries

Our long-term goal is to improve the reliability of electrode materials and their ability to transport and store various metal ions for electrochemical energy storage applications. The main objective of this work was to investigate the intrinsic relationship between the role of alkali metal ions and electrochemically driven mechanical stability and kinetic properties of battery materials. The overall question was “What is the role of alkali metal ions on the electrochemical and mechanical behavior of cathode electrodes? Our guiding hypothesis was that intercalation of larger alkali metal ions (Na and K) inevitably alters the coupled transport-reaction processes during battery operation in organic electrolytes, leading to more intensive chemo-mechanical instabilities in cathode electrodes, resulting in rapid capacity fade. To validate the hypothesis, we experimentally characterized the reaction-transport processes and governing forces driving the instability of electrode materials in different alkali metal-ion environments. The project had three main tasks. The first one was to investigate intercalation-induced strains and associated stress generation, and their impact on structural deformations in composite cathode electrodes. The second task focused on identifying potential-dependent dynamic changes in the electrode-electrolyte interface in alkali metal ion batteries. The last task was focused on determining how larger alkali metal ions with slower diffusivity affect the transport-mechanics coupling at faster scan rates, compared to smaller ions with faster diffusivity in electrodes. We shortly provided the outcome of each task in the accomplishment section. This project produced 10 peer-reviewed publications (9 research papers and one review manuscript) and supported two Ph.D. students, who graduated from Oklahoma State University.

25 ENERGY STORAGE↗
NASA NTRS2007

Multiple-Parameter, Low-False-Alarm Fire-Detection Systems

Fire-detection systems incorporating multiple sensors that measure multiple parameters are being developed for use in storage depots, cargo bays of ships and aircraft, and other locations not amenable to frequent, direct visual inspection. These systems are intended to improve upon conventional smoke detectors, now used in such locations, that reliably detect fires but also frequently generate false alarms: for example, conventional smoke detectors based on the blockage of light by smoke particles are also affected by dust particles and water droplets and, thus, are often susceptible to false alarms. In contrast, by utilizing multiple parameters associated with fires, i.e. not only obscuration by smoke particles but also concentrations of multiple chemical species that are commonly generated in combustion, false alarms can be significantly decreased while still detecting fires as reliably as older smoke-detector systems do. The present development includes fabrication of sensors that have, variously, micrometer- or nanometer-sized features so that such multiple sensors can be integrated into arrays that have sizes, weights, and power demands smaller than those of older macroscopic sensors. The sensors include resistors, electrochemical cells, and Schottky diodes that exhibit different sensitivities to the various airborne chemicals of interest. In a system of this type, the sensor readings are digitized and processed by advanced signal-processing hardware and software to extract such chemical indications of fires as abnormally high concentrations of CO and CO2, possibly in combination with H2 and/or hydrocarbons. The system also includes a microelectromechanical systems (MEMS)-based particle detector and classifier device to increase the reliability of measurements of chemical species and particulates. In parallel research, software for modeling the evolution of a fire within an aircraft cargo bay has been developed. The model implemented in the software can describe the concentrations of chemical species and of particulate matter as functions of time. A system of the present developmental type and a conventional fire detector were tested under both fire and false-alarm conditions in a Federal Aviation Administration cargo-compartment- testing facility. Both systems consistently detected fires. However, the conventional fire detector consistently generated false alarms, whereas the developmental system did not generate any false alarms.

Hunter, Gary W.↗
DOE OSTI2023

Investigation of the Hydrogen Embrittlement of API 5L Natural Gas Pipeline Steels

Hydrogen ions produced during corrosion or through hydrogen blending into natural gas pipelines can lead to the degradation of ductility of metals used in these transmission pipelines. The effect of hydrogen on the mechanical properties of pipeline steels was studied for three grades of API 5L steels: X56, X65, and X100. These steels are either commonly used in or considered for use in natural gas transmission pipelines which are being considered for use in hydrogen blending. These steels were subjected to constant strain rate tensile testing after charging with electrochemically generated hydrogen. This presentation reports on work to extend the life of the natural gas pipeline network via understanding the effect of hydrogen embrittlement induced by corrosion processes.

Teeter, Lucas↗
DOE OSTI2025

Reward based optimization of resonance-enhanced piezoresponse spectroscopy

Dynamic spectroscopies in scanning probe microscopy (SPM) are critical for probing material properties, such as force interactions, mechanical properties, polarization switching, electrochemical reactions, and ionic dynamics. However, the practical implementation of these measurements is constrained by the need to balance imaging time and data quality. Signal to noise requirements favor long acquisition times and high frequencies to improve signal fidelity. However, these are limited on the low end by contact resonant frequency and photodiode sensitivity and on the high end by the time needed to acquire high-resolution spectra or the propensity for sample degradation under high field excitation over long times. The interdependence of key parameters such as instrument settings, acquisition times, and sampling rates makes manual tuning labor-intensive and highly dependent on user expertise, often yielding operator-dependent results. These limitations are prominent in techniques like dual amplitude resonance tracking in piezoresponse force microscopy that utilize multiple concurrent feedback loops for topography and resonance frequency tracking. Here, a reward-driven workflow is proposed that automates the tuning process, adapting experimental conditions in real time to optimize data quality. Furthermore, this approach significantly reduces the complexity and time required for manual adjustments and can be extended to other SPM spectroscopic methods, enhancing overall efficiency and reproducibility.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Core–Multishell-Structured Digital-Gradient Cathode Materials with Enhanced Mechanical and Electrochemical Durability

Ni-rich cathode materials provide high energy density, but their structural and surface instability limits their cyclability and thermal stability. As one of the approaches to mitigate this problem, cathode materials comprising Ni-rich high-capacity core wrapped in Mn-rich multiple shells are produced successfully. In contrast to the conventional batch-type process for concentration-gradient materials, a digital-gradient cascade coprecipitation process described here achieves the improvements in productivity and quality consistency needed to move toward large-scale manufacturing. The core-multishell cathode materials produced in this manner not only have longer cycle life and improved rate performance compared to homogeneous Ni-rich cathode materials having the same overall composition, but also show remarkably enhanced thermal stability and low impedance growth characteristics. In a novel attempt to determine the correlation between the mechanical properties of the core-multishell cathode particles and their electrochemical cyclabilities, their breaking force and elasticity were successfully measured using a statistical approach, which indicates that a cathode particle with stable surface composition as well as high breaking force has improved capacity retention and durability. These results guide the realization of long life and high thermal stability in Ni-rich cathode materials through heterogeneous particle engineering.

25 ENERGY STORAGE↗
DOE OSTI2026

Establishment of a Vertically Integrated Domestic Manufacturing Process for Production of Substrates Needed for Manufacture of Gas Diffusion Layers

In this project, AvCarb, LLC evaluated the baseline performance metrics of commercial carbon veils and their corresponding Gas Diffusion Layers (GDLs) with the goal of establishing an optimized, vertically integrated production system for wet-laid nonwoven substrates used in gas diffusion media for electrochemical energy storage and conversion devices. Mechanical testing and microstructural characterization were conducted and used to develop a multiscale computational model capable of simulating and predicting the performance of GDLs in fuel cells. Although the project successfully generated foundational transport and modeling data, it was terminated prior to identifying the critical GDL design parameters necessary for full optimization. The program aimed to improve carbon veil fabrication through enhanced fiber dispersion, fiber-fiber adhesion control, and improved web formation, enabling the production of high-quality, uniform substrates. Simulations were intended to guide mixing and solution delivery system design and process conditions, followed by production-scale trials to evaluate fiber dispersion, web uniformity, and mechanical robustness. At full deployment, the proposed production line would have been capable of producing approximately 650,000 m² of carbon veil annually. This capability remains strategically important, as the United States currently lacks a domestic source of wet-laid nonwoven carbon substrates that satisfy the stringent quality requirements for fuel-cell GDLs and electrolyzers representing an ongoing supply-chain vulnerability. Beyond supply-chain benefits, the project established a robust benchmarking dataset for existing commercial carbon veils while advancing next-generation material concepts targeting improved performance and manufacturing consistency.

Olson, Cynthia Lemay↗
NASA NTRS1993

Advances in Studies of Electrode Kinetics and Mass Transport in AMTEC Cells

Previous work reported from JPL has included characterization of electrode kinetics and alkali atom transport from electrodes including Mo, W, WRh x (Mn), in sodium AMTEC cells and vapor exposure cells; and Mo in potassium vapor exposure cells. These studies were generally performed in cells with small area electrodes (about 1 to 5 cm 2 ), and device geometry had little effect on transport. Alkali metal diffusion coefficients through these electrodes have been characterized, and approximate surface diffusion coefficients were derived in cases of activated transport. A basic model of electrode kinetics and transport at the alkali metal vapor/pourous metal electrode/alkali beta"-alumina solid electrolyte (BASE) three phase boundary has been proposed which accounts for electrochemical reaction rates with a collision frequency near the three phase boundary and tunneling from the porous electrode partially covered with adsorbed alkali metal atoms. The small electrode effect in AMTEC cells has been discussed in several papers, but quantitative investigations have described only the overall effect and the important contribution of electrolyte resistance. The quantitative characterization of transport losses in cells with large area electrodes has been limited to simulations of large area electrode effects, or characterization of transport losses from large area electrodes with significant longitudinal temperature gradients. This paper describes new investigations of electrochemical kinetics and transport, with four 14.4 cm 2 WPt 3.5 electrodes, including the influence of electrode size on the mass transport loss in the AMTEC cell. These electrodes exhibit very slow sintering, as well as excellent sodium transport properties, making them attractive candidates for AMTEC power conversion use. However, the facile sodium transport in WPt 3.5 electrodes makes characterization of the transport process difficult.

electrode↗
NASA NTRS2009

Processing and Probability Analysis of Pulsed Terahertz NDE of Corrosion under Shuttle Tile Data

This paper examines data processing and probability analysis of pulsed terahertz NDE scans of corrosion defects under a Shuttle tile. Pulsed terahertz data collected from an aluminum plate with fabricated corrosion defects and covered with a Shuttle tile is presented. The corrosion defects imaged were fabricated by electrochemically etching areas of various diameter and depth in the plate. In this work, the aluminum plate echo signal is located in the terahertz time-of-flight data and a threshold is applied to produce a binary image of sample features. Feature location and area are examined and identified as corrosion through comparison with the known defect layout. The results are tabulated with hit, miss, or false call information for a probability of detection analysis that is used to identify an optimal processing threshold.

Anastasi, Robert F.↗
DOE OSTI2022

Radical Polymer-Based Organic Electrochemical Transistors

Organic electrochemical transistors (OECTs) are an emerging platform for bioelectronic applications. Significant effort has been placed in designing advanced polymers that simultaneously transport both charge and ions (i.e., macromolecules that are mixed conductors). Furthermore, the considerations for mixed organic conductors are often different from the established principles that are well-known in the solid-state organic electronics field; thus, the discovery of new OECT macromolecular systems is highly desired. Here, we demonstrate a new materials system by blending a radical polymer (i.e., a macromolecule with a nonconjugated backbone and with stable open-shell sites at its pendant group) with a frequently used conjugated polymer. Specifically, poly(4-glycidyloxy-2,2,6,6-tetramethylpiperidine-1-oxyl) (PTEO) was blended with poly(3-hexylthiophene) (P 3 HT) to create thin films with distinct closed-shell and open-shell domains. Importantly, the sharp and unique oxidation–reduction (redox) potential associated with the radical moieties of the PTEO chain provided a distinct actuation feature to the blended films that modulated the ionic transport of the OECT devices. In turn, this led to controlled regulation of the doping of the P 3 HT phase in the composite film. By decoupling the ionic and electronic transport into two distinct phases and by using an ion transport phase with well-controlled redox activity, never-before-seen performance for a P3HT-based OECT was observed. That is, at loadings as low as 5% PTEO (by weight) OECTs achieved figure-of-merit (i.e., μC*) values >150 F V –1 cm –1 s –1 , which place the performance on the same order as state-of-the-art conjugated polymers despite the relatively common conjugated macromolecular moiety implemented. As such, this effort presents a design platform by which to readily create a tailored OECT response through strategic macromolecular selection and polymer processing.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Robust hierarchical three dimensional nickel cobalt tungstate-MXene nanocomposite for high performance symmetric coin cell supercapacitors

Design of rational electrode materials with hierarchically structured pseudocapacitive materials has been identified as a successful strategy for revamping the electrochemical characteristics of supercapacitors. However, the simultaneous assurance of strong electrical conductivity and higher specific capacitance via a simple and cost-effective synthesis protocol is of concern today. In this work, Ni-CoWO 4 incorporated MXene nanocomposite has been successfully prepared by a facile hydrothermal process. The structure, morphology, stoichiometry, and chemical characterization of the prepared Ni-CoWO 4 , Ti 3 C 2 T x , and Ni-CoWO4@MXene nanocomposite were explored extensively. MXene demonstrated a layered 2D nanoscale structure whereas pure Ni-CoWO 4 was composed of spherical nanoparticles. The composite Ni-CoWO 4 @MXene revealed the morphology of spherical Ni-CoWO 4 nanoparticles decorated on MXene sheets. Furthermore, a series of electrochemical characterizations illustrated the contribution of the delightful morphology of Ni-CoWO 4 @MXene composite to excellent electrochemistry. The resultant Ni-CoWO 4 @MXene electrode exhibited high specific capacitance of 582 Fg -1 at 1 A g -1 and 93.5 % capacitance retention over the 10,000 cycles., which is higher than that of the individual counterparts Ni-CoWO 4 and MXene. The excellent electrochemical performance of Ni-CoWO 4 @MXene is attributed to the synergistic interaction between Ni-CoWO4 nanoparticles and nanolayered MXene that may create new active sites that enhanced the charge transfer, charge/discharge kinetics and the electrical conductivity. Significantly, the unique Ni-CoWO 4 @MXene supercapacitor prototype delivered a higher energy density of 85.7 Wh kg -1 and power density of 0.85 kW kg -1 establishing its superiority over other Cosingle bondW based supercapacitors. A theoretical study was also performed to correlate the improved charge storage capacity of the prepared Ni-CoWO 4 @MXene composite.

25 ENERGY STORAGE↗
DOE OSTI2020

Fluorination effect for stabilizing cationic and anionic redox activities in cation-disordered cathode materials

We see that cation-disordered Li-excess cathodes with oxygen redox reactions are promising candidates for high-energy-density Li ion batteries. Nevertheless, the oxygen redox process that is required for the high capacity often comes with the oxygen loss, which leads to severe capacity degradation and voltage decay. In this work, we have successfully synthesized a series of Li-excess cation-disordered cathodes (Li 1.2 Mn 0.4+x Ti 0.4-x O 2-x Fx) (0 ≤ x ≤ 0.2) with different fluorine (F) contents. The electrochemical performance results show that the Li 1.2 Mn 0.55 Ti 0.25 O 1.85 F 0.15 (LMTOF0.15) exhibits the highest reversible capacity (275 mAh g -1 , under 30 mA g -1 ), cyclability, and voltage retentions. The mapping of resonant inelastic X-ray scattering (mRIXS) and differential electrochemical mass spectroscopy (DEMS) results reveal that the fluorination enhances the reversible lattice oxygen redox reaction while suppressing irreversible gas release and surface reactions. The X-ray Absorption Spectroscopy (XAS) during the initial two cycles shows that F-substitution alleviates the reduction of the Mn valence state during the whole (dis)charge processes in the bulk and at the surface of the material, results in higher average discharge voltage. In addition, the introduction of F improves the structural stability and suppresses local lattice distortion of the material. Therefore, LMTOF 0.15 is able to cycle with smaller polarization, less interfacial side reaction and Mn dissolution, and therefore results in enhanced cyclability. This work provides a comprehensive understanding of the fluorination effect on the cationic and anionic redox activities in cation-disordered Li-excess cathodes.

25 ENERGY STORAGE↗
DOE OSTI2024

Ketjenblack-Supported and Unsupported ZrO 2 –ZrN Nanoparticle Systems for Enabling Efficient Electrochemical Nitrogen Reduction to Ammonia

Artificial N 2 fixation via the electrocatalytic nitrogen (N 2 ) reduction reaction (NRR) has been recently promoted as a rational route toward reducing energy consumption and CO 2 emission as compared with the traditional Haber–Bosch process. Nevertheless, optimizing NRR relies on developing highly efficient electrocatalysts. Herein, we report on the reliable and reproducible synthesis of two promising electrocatalysts in either the presence or absence of Ketjenblack (KB), namely, ZrO 2 –ZrN@KB and ZrO 2 –ZrN systems, synthesized through the nitriding of Zr. Both materials had never previously been considered for NRR, to the best of our knowledge. Nevertheless, both of these electrocatalysts incorporated a combination of tetragonal ZrO 2 , ZrON, and cubic ZrN and showed excellent activity and durability toward NH 3 formation. Moreover, the maximum NH3 production rate of 84.1 μg h –1 mg –1 at -0.7 V vs a reversible hydrogen electrode (RHE) was achieved with the ZrO 2 –ZrN electrocatalyst with an impressive Faradaic efficiency of 21.2% at -0.6 V vs RHE, indicating a high selectivity associated with the NRR. Additionally, the catalysts demonstrated excellent stability during the electrolysis process and recycling tests. Here we postulate that the combination of exposed active sites of ZrN and ZrO 2 likely contributes to the enhanced NRR performance attributed to ZrO 2 –ZrN.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2001

Characterization of the electromechanical properties of EAP materials

Electroactive polymers (EAP) are an emerging class of actuation materials. Their large electrically induced strains (longitudinal or bending), low density, mechanical flexibility, and ease of processing offer advantages over traditional electroactive materials. However, before the capability of these materials can be exploited, their electrical and mechanical behavior must be properly quantified. Two general types of EAP can be identified. The first type is ionic EAP, which requires relatively low voltages (<10V) to achieve large bending deflections. This class usually needs to be hydrated and electrochemical reactions may occur. The second type is Electronic-EAP and it involves electrostrictive and/or Maxwell stresses. This type of materials requires large electric fields (>100MV/m) to achieve longitudinal deformations at the range from 4 - 360%. Some of the difficulties in characterizing EAP include: nonlinear properties, large compliance (large mismatch with metal electrodes), nonhomogeneity resulting from processing, etc. To support the need for reliable data, the authors are developing characterization techniques to quantify the electroactive responses and material properties of EAP materials. The emphasis of the current study is on addressing electromechanical issues related to the ion-exchange type EAP also known as IPMC. The analysis, experiments and test results are discussed in this paper.

actuators↗
DOE OSTI2023

Ion Conducting Polymer Interfaces for Lithium Metal Anodes: Impact on the Electrodeposition Kinetics

Electrochemical cells that utilize metals (e.g., lithium, sodium, zinc) as anodes are under intense investigation as they are projected to replace the current lithium-ion batteries to serve as a more energy-dense option for commercial applications. In addition, metal electrodes provide opportunities for fundamental research of different phenomena, such as ion transport and electrochemical kinetics, in the complex environment of reactive metal-electrodeposition. In this work, computationally and experimentally the competing effects related to transport and kinetics during the metal electrodeposition process are examined. Using Brownian dynamics simulations, it is shown that slower deposition kinetics results in a more compact and uniform Li morphology. This finding is experimentally implemented by designing ion-containing polymeric coatings on the electrodes that simultaneously provide pathways for lithium-ion transport, while impeding the charge transfer (Li + + e - → Li) at heterogeneous surfaces. It is further shown that these ionic polymer interfaces can significantly extend the cell-lifetime of a lithium metal battery in both ether-based and carbonate-based electrolytes. Through theoretical and experimental investigations, it is found that a low kinetic to transport rate ratio is a major factor in influencing the Li plating morphology. The plating morphology can be further fine-tuned by increasing ionic conductivity.

36 MATERIALS SCIENCE↗