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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 1,063 records · Page 59
All sourcesNASA NTRSDOE OSTI
DOE OSTI2016

Performance of an i -SANEX System Based on a Water-Soluble BTP under Continuous Irradiation in a γ-Radiolysis Test Loop

Here, the i -SANEX solvent formulation consisting of nominally 0.2 M TODGA/5% 1-octanol/dodecane was γ-irradiated under realistic conditions in the Idaho National Laboratory radiolysis test loop, in contact with both extraction and stripping aqueous phases. The extraction aqueous phase was 4.5 M HNO 3 , and the stripping aqueous phase was 0.018 M SO 3 –Ph–BTP/0.35 M HNO 3 . When irradiated in contact with only the 4.5 M HNO 3 phase, the TODGA solvent maintained excellent extraction performance for americium, cerium, europium, and neodymium to a maximum absorbed dose of nearly 0.9 MGy. The results for preliminary static, batch irradiations were consistent with test loop findings. When the aqueous phase was changed to that containing the aqueous soluble BTP, the irradiated aqueous phase showed a dramatic color change, but this does not appear to have had adverse effect on solvent extraction performance. The distribution ratios for both the lanthanides and actinides were invariant with absorbed dose, and the separation factors were essentially unchanged to a maximum absorbed dose of 174 kGy. The results of inductively coupled plasma mass spectrometry analysis of the aqueous and organic phases showed that ruthenium and strontium were not extracted in the presence of the irradiated BTP-aqueous phase. Molybdenum was extracted under both conditions. Further, the buildup of corrosion products of stainless steel in the presence of the BTP was not dramatically greater than in the nitric acid-only system. Phase separation times were not adversely affected by irradiation for either system. The results presented here indicate that the performance of the TODGA/SO 3 –Ph–BTP, i -SANEX process under test loop radiolysis is much better than expected based on a literature report using single-phase batch irradiation experiments, and better than might be predicted based on diglycolamide radiolysis studies alone.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2019

Assessment of Impacts of Dissolved Organic Matter and Dissolved Iron on the Performance of Amidoxime-Based Adsorbents for Seawater Uranium Extraction

Research on extraction of uranium from seawater has been active in recent years because this technology can provide an additional supply of uranium for nuclear fuel from a much larger uranium reservoir (the oceans) and the processes are more environment friendly. One critical challenge of the development of this technology is to make uranium adsorbents perform well not just in the oversimplified laboratory system (e.g. artificial seawater) but also in the complex real seawater matrix, which is comprised of many competing ions and natural organic substances. Here, we conducted a systematic study using a continuous-flow seawater flume system to assess the potential impacts of dissolved organic matter (DOM) and dissolved iron on the uranium uptake performance (including adsorbent reusability) of amidoxime-based adsorbents. In the 28-day exposure, the adsorbent exposed in dissolved Fe-spiked seawater (low DOM/high Fe) and humic acid-spiked seawater (high DOM/high Fe) showed lower uranium adsorption loadings (73% and 56% of adsorption loading, respectively) than the same adsorbent exposed in seawater without spiking (low DOM/low Fe). Interestingly, the uranium adsorption loading of the reused adsorbent (after uranium stripping by a mild bicarbonate elution) in the dissolved Fe-spiked seawater dropped substantially to only 24% of the loading in the unspiked clean seawater counterpart; while not much change was observed in the performance of adsorbent exposed to the humic acid-spiked seawater. From comparison of FTIR signatures of adsorbent before and after the seawater exposure, we found that the amidoxime ligands in the adsorbent exposed to dissolved Fe-spiked seawater had severer degradation than the adsorbents exposed to humic acid-spiked seawater and unspiked clean seawater. Notably, unlike the adsorbent exposed to dissolved Fe-spiked seawater, the adsorbent exposed to humic acid-spiked seawater didn’t adsorb elevated level of Fe compared to the adsorbent in the unspiked clean seawater. This suggests that the species of Fe in the humic acid-spiked seawater (primarily humic acid bound Fe) didn’t interact with amidoxime-based adsorbent; while the Fe species in the Fe-spiked seawater strongly interacted with adsorbent and caused significant degradation of amidoxime ligands. On the other hand, highly variable uranium adsorption loadings were observed in adsorbent in contact with humic acid-spiked seawater, but not in the adsorbents exposed to dissolved Fe-spiked seawater and seawater without spike. Our observations thus indicate that seawater receiving high inputs of DOM and dissolved Fe, such as coastal waters, is not ideal for efficient extraction of uranium.

Uranium, Seawater, amidoxime-based adsorbents, dis↗
DOE OSTI2025

Advanced Analysis of X-ray Fluorescence Measurements of the Interfacial Density of Eu Ions at Liquid–Liquid Interfaces for Solvent Back-Extraction

X-ray fluorescence near total reflection (XFNTR) is the primary technique used to measure the element-specific interfacial density of ions at liquid−liquid interfaces. Fluorescence from ions in the bulk liquids can complicate the determination of the interfacial density; consequently, measurements have been previously limited to samples without ions in the upper phase and with concentrations on the order of 10 μM or less in the lower phase. We modify the analysis of XFNTR data to account for ions in both bulk phases, then demonstrate its use in the context of rare-earth separations processes. In a model of ion stripping (i.e., back-extraction), dodecane solutions of di(2-ethylhexyl)- phosphoric acid (HDEHP) loaded with Eu(III) at the 1 mM level are placed in contact with either pure water or aqueous solutions of nitric or citric acid at pH 3. XFNTR measurements of equilibrated, quiescent samples reveal that citric acid solutions produce a disproportionately large depletion of ions from the interface compared to that from the bulk organic solution, whereas stripping by pure water or nitric acid solutions is negligible. As a result, this advance in the methodology of XFNTR may have broad applicability to the investigation of metal ions in chemical and biological processes at liquid−liquid interfaces.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2018

From Microparticles to Nanowires and Back: Radical Transformations in Plated Li Metal Morphology Revealed via in Situ Scanning Electron Microscopy

We report that Li metal is the preferred anode material for all-solid-state Li batteries. However, a stable plating and stripping of Li metal at the anode–solid electrolyte interface remains a significant challenge particularly at practically feasible current densities. This problem usually relates to high and/or inhomogeneous Li-electrode–electrolyte interfacial impedance and formation and growth of high-aspect-ratio dendritic Li deposits at the electrode–electrolyte interface, which eventually shunt the battery. To better understand details of Li metal plating, we use operando electron microscopy and Auger spectroscopy to probe nucleation, growth, and stripping of Li metal during cycling of a model solid-state Li battery as a function of current density and oxygen pressure. We find a linear correlation between the nucleation density of Li clusters and the charging rate in an ultrahigh vacuum, which agrees with a classical nucleation and growth model. Moreover, the trace amount of oxidizing gas (≈10 –6 Pa of O 2 ) promotes the Li growth in a form of nanowires due to a fine balance between the ion current density and a growth rate of a thin lithium-oxide shell on the surface of the metallic Li. Interestingly, increasing the partial pressure of O 2 to 10 –5 Pa resumes Li plating in a form of 3D particles. In conclusion, our results demonstrate the importance of trace amounts of preexisting or ambient oxidizing species on lithiation processes in solid-state batteries.

25 ENERGY STORAGE↗
DOE OSTI2022

Li Morphology Evolution during Initial Cycles in a Gel Composite Polymer Electrolyte

Understanding and controlling lithium morphology evolution and lithium dendrite formation and growth during cycling is one of the key challenges for high-energy lithium metal batteries. This challenge applies to liquid electrolyte batteries as well as solid-state and semi-solid-state batteries. Our current knowledge about the evolution of the Li morphology is mostly obtained from liquid electrolyte-based studies in a Li–Li symmetrical cell configuration. The knowledge obtained in such conditions may not readily transfer into solid-state or semi-solid-state batteries. In this work, Li morphology evolution during initial cycling in a full cell configuration with the LiNi 0.6 Co 0.2 Mn 0.2 O 2 (NMC 622) cathode and a semi-solid-state gel composite electrolyte is monitored via post-mortem photographs and scanning electron microscopy at multiple length scales. The gel composite electrolyte contains a cross-linked poly(ethylene oxide)-based polymer electrolyte, ceramic fillers, and a liquid plasticizer. The results show that severe surface pitting occurs as early as the second stripping cycle. Pit formation and continuous dissolution during the stripping process are the main cause of the Li surface roughening and dendrite growth mechanism in the model gel composite electrolyte. Comparing Li dendrite growth mechanisms in liquid, polymer, and ceramic solid electrolytes, the dendrite growth mechanism observed in this model electrolyte resembles that of the liquid electrolyte the most. This study suggests that strategies to control Li morphology and prevent dendrite growth in a gel composite electrolyte should be similar to strategies applicable to liquid electrolytes.

25 ENERGY STORAGE↗
DOE OSTI2020

Solubility-Dependent Protective Effects of Binary Alloys for Lithium Anode

Recently, alloys have been widely utilized as protection layers for homogenized Li growth. However, the protective mechanisms for different alloys are not clearly understood. In this work, guided by the binary phase diagrams, Mg, Au, Zn, Al, Fe, and Cu protective layers have been selected for study of their protective abilities and mechanisms. The selected metals can be classified into three categories according to the nature of their associated alloy protective layers: (1) metals with high solubility in Li while not forming any intermediate line compounds, e.g., Mg, which is good for fast Li stripping; (2) metals with limited solid solubility but forming stable line compounds with Li upon the lithiation, e.g., Au, Zn, and Al, where the formed stable line compounds Li x Au, Li x Zn, and Li x Al will hamper Li kinetics; (3) metals with negligible mutual solubility and no line compound formation with Li, e.g., Fe and Cu, which block the Li stripping path and therefore result in the highest polarization voltage.

25 ENERGY STORAGE↗
DOE OSTI2017

Core–Shell Nanostructured Cobalt–Platinum Electrocatalysts with Enhanced Durability

Pt-bimetallic alloys involving 3d transition metals (Co, Ni, etc.) are promising electrocatalysts for the oxygen reduction reaction (ORR). Despite the enhanced catalytic activity versus Pt, the electrocatalytic performance of Pt-bimetallic catalysts is however limited by the lack of long-term durability, primarily due to the leaching of the non-noble element under harsh electrochemical conditions. In this work, our study shows that the core–shell nanostructure comprising a Pt shell and a cobalt core (denoted as Co@Pt) could overcome this limitation, demonstrating ~10 times improvement in catalytic activity versus commercial Pt catalysts and no more than 13% of loss after 30000 potential cycles. The evolutions of nanoscale and surface structures over the course of extensive potential cycling were followed by combining electron microscopic elemental mapping and electrochemical studies of CO stripping. Atomistic simulations and density functional theory calculations suggest that the core–shell nanostructure could protect the non-noble cobalt from leaching under the “electrochemical annealing” conditions while maintaining the beneficial mechanisms of bimetallic systems for catalytic activity enhancement.

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

Electrochemical Healing of Dendrites in Garnet-Based Solid Electrolytes

Garnet oxides are a promising material family for solid-state batteries (SSBs). Dendrite formation in solid electrolytes critically limits the applicability of SSBs because of limiting Coulombic efficiency and power capability. In this study, the authors report operando electrochemical healing of dendrites in a garnet-based solid electrolyte (SE). Dendrites were deliberately formed at high operational current density (2 mA cm –2 ) beyond the critical current density (0.55 mA cm –2 ) of the used garnet SE. Electrochemical impedance spectroscopy and scanning electron microscopy were used to confirm dendrite growth in the SE. Dendrites were subsequently healed electrochemically via plating and stripping at 20 and 1 μA cm –2 current densities. Removal of dendrites was shown by an increase in bulk and interfacial resistance and a progressive increase in polarization during galvanostatic plating and stripping. High local current density at the dendrite tips was identified as the mechanism for preferentially removing dendrites electrochemically. The dendrite detection and healing methods discussed here are crucial for extending the life of SSBs.

25 ENERGY STORAGE↗
DOE OSTI2025

The Crucial Role of Vacancy Concentration in Enabling Superatomic Diffusion in Lithium Intermetallics

Anode-free solid-state Li batteries promise significant increases in energy densities compared to current commercial batteries that rely on liquid electrolytes. Major challenges persist in controlling morphological evolution during the plating and stripping of lithium metal at the anode current collector. Elemental additives that alloy with lithium have been found to modify the plating and stripping behavior of lithium. Many alloying elements form intermetallics with lithium and the mobility of Li through these intermetallics is believed to have an important effect on morphological evolution. This study shows that Li transport coefficients through intermetallics span a wide range in values, with the B32 LiAl intermetallic predicted to have a Li tracer diffusion coefficient as high as 10 –6 cm 2 /s at room temperature, which is 8 orders of magnitude larger than that of isostructural B32 LiZn. This work demonstrates the crucial role of vacancy concentration in controlling the mobility of Li atoms through intermetallics. While the migration barriers for Li-vacancy exchanges in both LiAl and LiZn are remarkably low, the superatomic conductivity in LiAl is shown to arise from the unique electronic structure of the B32 LiAl compound, which favors high concentrations of vacancies.

25 ENERGY STORAGE↗
DOE OSTI2019

Underwater Organic Solar Cells via Selective Removal of Electron Acceptors near the Top Electrode

Electron acceptor degradation of organic solar cells is considered a main contributor to performance instability and a barrier for the commercialization of organic solar cells. In this work, we selectively remove the electron acceptors on the surface of donor:acceptor blend films using a tape stripping technique. The near-edge X-ray absorption fine structure (NEXAFS) spectrum reveals that only 6% of the acceptor component is left on the blend film surface after the tape stripping, creating a polymer-rich surface. The optimized morphology avoids direct contact of electron acceptors with the oxygen and water molecules from the film surface. Moreover, the polymer-rich surface dramatically enhances the adhesion between the photoactive layer and the top metal electrode, which prevents delamination of the electrode. Our results finally show that the selective removal of electron acceptors near the top electrode facilitates the realization of highly durable organic solar cells that can even function under water without encapsulation.

14 SOLAR ENERGY↗
DOE OSTI2021

Determination of Arsenic Content in Water Using a Silver Coordination Polymer

In this report, we describe a practical method for the colorimetric determination of dissolved inorganic arsenic content in water samples, using a silver coordination polymer as the sensing material. We demonstrate that a crystalline polymer framework can be used to stabilize silver(I) ions, greatly reducing both photosensitivity and water solubility, while still affording sufficient reactivity to detect arsenic in water samples at low parts-per-billion (ppb) levels. Test strips fabricated with the silver-based polymer are shown to be effective for field tests of groundwater under real-world operating conditions and display performance that is competitive with commercially available mercury-based test strips. Spectroscopic methods are also used to probe the reaction products formed, in order to better understand the sensing mechanism. Thus, our work provides the foundation for an improved field test that could be deployed to help manage groundwater usage in regions where arsenic contamination is problematic but sophisticated lab testing is not readily available.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Improving Lithium Metal Composite Anodes with Seeding and Pillaring Effects of Silicon Nanoparticles

Metallic lithium (Li) anodes are crucial for the development of high specific energy batteries yet plagued by their poor cycling efficiency. Electrode architecture engineering is vital for maintaining a stable anode volume and suppress Li corrosion during cycling. In this paper, a reduced graphene oxide “host” framework for Li metal anodes is further optimized by embedding silicon (Si) nanoparticles between the graphene layers. They serve as Li nucleation seeds to promote Li deposition within the framework even without pre-stored Li. Meanwhile, the LixSi alloy particles serve as supporting “pillars” between the graphene layers, enabling a minimized thickness shrinkage after full stripping of metallic Li. Combined with a Li compatible electrolyte, 99.4% Coulombic efficiency over ~600 cycles is achieved, and stable cycling of a Li||NMC532 full cell for ~380 cycles with negligible capacity decay is realized.

Wang, Hansen↗
DOE OSTI2025

Ambient Rare Earth Metal Electrodeposition in Nitrogen-Coordinated Silylamide Electrolyte

The transition to a sustainable, low-carbon economy demands energy-efficient and environmentally benign methods for rare earth metal (REM) production. Furthermore, while high-temperature molten salt electrolysis remains energy-intensive, corrosive, and environmentally unfriendly, emerging room-temperature processes based on conventional ionic liquids are also hindered by high viscosity and chemical instability. In this study, a nitrogen-coordinated, water-, oxygen-, and fluorine-free silylamide-based electrolyte is presented as a promising system for room-temperature REM electrodeposition. Derived from commercially available lithium silylamide precursors, the system enables facile synthesis, broad electrochemical stability, and tunable metal–ligand interactions. Electrochemical analysis reveals high voltammetric stripping reversibility, stable cathodic and anodic potentials, and selective neodymium (Nd) deposition at appreciable current densities (>1 mA/cm 2 ), with minimal parasitic reactions. Bulk experiments produced high-purity Nd with reproducible performance across multiple batches. Scaled deposition yielded over 1 g of Nd with near-theoretical mass efficiency (0.40 mg/C) and >90% purity. Using sacrificial dysprosium (Dy) and Nd metal anodes, the system maintained constant Nd loading during extended deposition and enabled cathodic codeposition of stripped anode material, demonstrating the electrolyte’s dual functionality for REM electrorefining. Collectively, this silylamide platform offers a compelling combination of electrochemical robustness, chemical resilience, and process scalability for sustainable ambient REM recovery.

36 - MATERIALS SCIENCE↗
DOE OSTI2024

Dynamical Janus Interface Design for Reversible and Fast-Charging Zinc–Iodine Battery under Extreme Operating Conditions

Aqueous zinc (Zn) iodine (I 2 ) batteries have emerged as viable alternatives to conventional metal-ion batteries. However, undesirable Zn deposition and irreversible iodine conversion during cycling have impeded their progress. Here, to overcome these concerns, we report a dynamical interface design by cation chemistry that improves the reversibility of Zn deposition and four-electron iodine conversion. Due to this design, we demonstrate an excellent Zn-plating/-stripping behavior in Zn||Cu asymmetric cells over 1000 cycles with an average Coulombic efficiency (CE) of 99.95%. Moreover, the Zn||I 2 full cells achieve a high-rate capability (217.1 mA h g –1 at 40 A g –1 ; C rate of 189.5C) at room temperature and enable stable cycling with a CE of more than 99% at -50 °C at a current density of 0.05 A g –1 . In situ spectroscopic investigations and simulations reveal that introducing tetraethylammonium cations as ion sieves can dynamically modulate the electrode–electrolyte interface environment, forming the unique water-deficient and chloride ion (Cl – )-rich interface. Such Janus interface accounts for the suppression of side reactions, the prevention of ICl decomposition, and the enrichment of reactants, enhancing the reversibility of Zn-stripping/-plating and four-electron iodine chemistry. This fundamental understanding of the intrinsic interplay between the electrode–electrolyte interface and cations offers a rational standpoint for tuning the reversibility of iodine conversion.

25 ENERGY STORAGE↗
DOE OSTI2021

The passivity of lithium electrodes in liquid electrolytes for secondary batteries

Rechargeable Li metal batteries are currently limited by electrolyte decomposition and rapid Li consumption. Li plating and stripping greatly depend on the solid electrolyte interphase formed at the Li metal-liquid electrolyte interface. This Review discusses the reactions occurring at this interface from a corrosion science perspective, highlighting the requirements for an ideal passivation layer. Rechargeable Li metal batteries are currently limited by safety concerns, continuous electrolyte decomposition and rapid consumption of Li. These issues are mainly related to reactions occurring at the Li metal-liquid electrolyte interface. Additionally, the formation of a passivation film (that is, a solid electrolyte interphase) determines ionic diffusion and the structural and morphological evolution of the Li metal electrode upon cycling. In this Review, we discuss spontaneous and operation-induced reactions at the Li metal-electrolyte interface from a corrosion science perspective. We highlight that the instantaneous formation of a thin protective film of corrosion products at the Li surface, which acts as a barrier to further chemical reactions with the electrolyte, precedes film reformation, which occurs during subsequent electrochemical stripping and plating of Li during battery operation. Finally, we discuss solutions to overcoming remaining challenges of Li metal batteries related to Li surface science, electrolyte chemistry, cell engineering and the intrinsic instability of the Li metal-electrolyte interface.

25 ENERGY STORAGE↗
DOE OSTI2019

Quantifying inactive lithium in lithium metal batteries

Lithium metal anodes offer high theoretical capacities (3,860 milliampere-hours per gram)1, but rechargeable batteries built with such anodes suffer from dendrite growth and low Coulombic efficiency (the ratio of charge output to charge input), preventing their commercial adoption. The formation of inactive (‘dead’) lithium— which consists of both (electro)chemically formed Li + compounds in the solid electrolyte interphase and electrically isolated unreacted metallic Li 0 —causes capacity loss and safety hazards. Quantitatively distinguishing between Li + in components of the solid electrolyte interphase and unreacted metallic Li 0 has not been possible, owing to the lack of effective diagnostic tools. Optical microscopy, in situ environmental transmission electron microscopy, X-ray microtomography and magnetic resonance imaging provide a morphological perspective with little chemical information. Nuclear magnetic resonance, X-ray photoelectron spectroscopy and cryogenic transmission electron microscopy can distinguish between Li + in the solid electrolyte interphase and metallic Li 0 , but their detection ranges are limited to surfaces or local regions. Here we establish the analytical method of titration gas chromatography to quantify the contribution of unreacted metallic Li 0 to the total amount of inactive lithium. We identify the unreacted metallic Li 0 , not the (electro)chemically formed Li + in the solid electrolyte interphase, as the dominant source of inactive lithium and capacity loss. By coupling the unreacted metallic Li 0 content to observations of its local microstructure and nanostructure by cryogenic electron microscopy (both scanning and transmission), we also establish the formation mechanism of inactive lithium in different types of electrolytes and determine the underlying cause of low Coulombic efficiency in plating and stripping (the charge and discharge processes, respectively, in a full cell) of lithium metal anodes. Here we propose strategies for making lithium plating and stripping more efficient so that lithium metal anodes can be used for next-generation high-energy batteries.

25 ENERGY STORAGE↗
DOE OSTI2019

Effect of chemical environment on the radiation chemistry of N , N -di-(2-ethylhexyl)butyramide (DEHBA) and plutonium retention

N,N-di-(2-ethylhexyl)butyramide (DEHBA) has been proposed as part of a hydro-reprocessing solvent extraction system for the co-extraction of uranium and plutonium from spent nuclear fuel, owing to its selectivity for hexavalent uranium and tetravalent plutonium. However, there is a critical lack of quantitative understanding regarding the impact of chemical environment on the radiation chemistry of DEHBA, and how this would affect process performance. Here we present a systematic investigation into the radiolytic degradation of DEHBA in a range of n-dodecane solvent system formulations, where we subject DEHBA to gamma irradiation, measure reaction kinetics, ligand integrity, degradation product formation, and investigate solvent system performance through uranium and plutonium extraction and strip distribution ratios. The rate of DEHBA degradation in n-dodecane was found to be slow (G = -0.31 ± 0.02 μmol J -1 ) but enhanced upon contact with the oxidizing conditions of the investigated solvent systems (organic-only, or in contact with either 0.1 or 3.0 M aqueous nitric acid). Two major degradation products were identified in the organic phase, bis-2-ethylhexylamine (b2EHA) and N-(2-ethylhexyl)butyramide (MEHBA), resulting from the cleavage of C–N bonds, and could account for the total loss of DEHBA up to ~300 kGy for organic-only conditions. Both b2EHA and MEHBA were also found to be susceptible to radiolytic degradation, having G-values of -0.12 ± 0.01 and -0.08 ± 0.01 μmol J -1 , respectively. Solvent extraction studies showed: (i) negligible change in uranium extraction and stripping with increasing absorbed dose; and (ii) plutonium extraction and retention exhibits complex dependencies on absorbed dose and chemical environment. Organic-only conditions afforded enhanced plutonium extraction and retention attributed to b2EHA, while acid contacts inhibited this effect and promoted significant plutonium retention for the highest acidity. Overall it has been demonstrated that chemical environment during irradiation has a significant influence on the extent of DEHBA degradation and plutonium retention.

38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEA↗
DOE OSTI2020

Spatial dynamics of lithiation and lithium plating during high-rate operation of graphite electrodes

The principal inhibitor of fast charging lithium ion cells is the graphite negative electrode, where favorable conditions for lithium plating occur at high charge rates, causing accelerated degradation and safety concerns. The local response of graphite, both at the electrode and particle level, when exposed to fast charging conditions of around 6C is not well understood. Consequently, the conditions that lead to the onset of lithium plating, as well as the local dynamics of lithium plating and stripping, have also remained elusive. Here, we use high-speed (100 Hz) pencil-beam X-ray diffraction to repeatedly raster along the depth of a 101 μm thick graphite electrode in 3 μm steps during fast (up to 6C) charge and discharge conditions. Consecutive depth profiles from separator to current collector were each captured in 0.5 seconds, giving an unprecedented spatial and temporal description of the state of the electrode and graphite's staging dynamics during high rate conditions. The electrode is preferentially activated near the separator, and the non-uniformity increases with rate and is influenced by free-energy barriers between graphite's lithiation stages. The onset of lithium plating and stripping was quantified, occurring only within the first 15 μm from the separator. The presence of lithium plating changed the behavior of the underlying graphite, such as causing co-existence of LiC 6 and graphite in the fully discharged state. Finally, the staging behavior of graphite at different rates was quantified, revealing a high dependency on rate and drastic hysteresis between lithiation and delithiation.

25 ENERGY STORAGE↗