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At least 955 records · Page 53

Alternate Synthesis Method for High-Performance Manganese Rich Cation Disordered Rocksalt Cathodes

Cation-disordered rocksalt (DRX) cathodes have recently emerged as a promising class of cobalt-free, high-capacity cathodes for lithium-ion batteries. To facilitate their commercialization, the development of scalable synthesis techniques providing control over composition and morphology is critical. To this end, a sol-gel synthesis route to prepare Mn-rich DRX cathodes with high capacities is presented here. Several compositions with varied Mn content and nominal F doping are successfully prepared using this technique. In-situ X-ray diffraction measurements demonstrate that DRX formation proceeds at moderate temperature (800 °C) through the sol-gel route, which enables intimate mixing among reactive intermediate phases that form at lower temperatures. All synthesized compositions possess cation short-range order, as evidenced by neutron pair distribution function and electron diffraction analysis. These DRX materials demonstrate promising electrochemical performance with reversible capacities up to 275 mAh g. Compared to the baseline oxide (Li 1.2 Mn 0.4 Ti 0.4 O 2 ), the Mn-rich compositions exhibit improved cycling stability, with some showing an increase in capacity upon cycling. Finally, this study demonstrates the feasibility of preparing high-capacity DRX cathodes through a sol-gel based synthesis route, which may be further optimized to provide better control over the product morphology compared to traditional synthesis methods.

25 ENERGY STORAGE↗

Utilizing Quantum Cascade Lasers for Ultranarrow Velocity Resolution and Quantum-State Selectivity in Molecular Beam Scattering and Spectroscopy

Here, we demonstrate the capability of a narrow linewidth quantum cascade laser (QCL) to selectively excite a very narrow velocity range of nitric oxide (σ ≤ 7(3) m/s) with a pure ro-vibrational quantum state. By implementing a counter-propagating geometry, the molecules are selectively excited according to the Doppler shift of the ro-vibrational transition frequency such that the velocity width associated with the excited molecules depends only on the QCL linewidth. We demonstrate a velocity distribution limited by the effective linewidth of our free-running QCL (Γ = 3.2 MHz). Our development provides a cost-effective, flexible approach to resolve quantum-state selective chemical dynamics with excellent velocity resolution in a wide variety of molecules with infrared-active transitions. This technique has been formulated to provide ultrahigh collisional energy resolution in molecular beams to delineate final quantum-state product pairs in studies of molecular collisions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Local dynamic responses of magnetic reconnection to three-dimensional perturbations in a laboratory plasma

The dynamic responses of magnetic reconnection to localized three-dimensional (3D) magnetic field perturbations imposed by a pair of figure-8-shaped coils are investigated in the Magnetic Reconnection Experiment (MRX) device. Both the magnetic field geometry and current sheet profiles are altered by external perturbations. For the case when the inductive electric field associated with these perturbations aligns with the preexisting reconnection electric field, O-type magnetic structures appear within an elongated current sheet. When these magnetic structures are ejected downstream at the speed close to the ion outflow velocity, the inductive electric field is enhanced considerably. Despite that the imposed perturbation amplitude is larger than 30% of the original reconnecting magnetic field, the overall reconnection process remains robust without current sheet disruptions. This technique to form O-type magnetic structures can serve as an additional experimental knob for future systematic laboratory investigations of 3D magnetic reconnection and related instabilities without disrupting two-dimensional current sheet.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Observation of flow angle and flow magnitude fluctuations in Pb-Pb collisions at $\sqrt{S_{NN}}$ = 5.02 TeV at the CERN Large Hadron Collider

This Letter reports on the first measurements of transverse momentum dependent flow angle Ψ n and flow magnitude v n fluctuations determined using new four-particle correlators. The measurements are performed for various centralities in Pb–Pb collisions at a center-of-mass energy per nucleon pair of $\sqrt{S_{NN}}$ = 5.02 TeV with ALICE at the CERN Large Hadron Collider. Both flow angle and flow magnitude fluctuations are observed in the presented centrality ranges and are strongest in the most central collisions and for a transverse momentum p T > 2 GeV / c. Comparison with theoretical models, including iEBE-VISHNU, MUSIC, and AMPT, show that the measurements exhibit unique sensitivities to the initial state of heavy-ion collisions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Toward a long-lifetime polarized photoelectron gun for the Ce+BAF positron source

The addition of spin-polarized, continuous-wave (c.w.) positron beams to the 12 GeV Continuous Electron Beam Accelerator Facility (CEBAF) would provide a significant capability to the experimental nuclear physics program at Jefferson Lab. Based on bremsstrahlung and pair-production in a high-Z target, the positron source requires a 120 MeV spin-polarized c.w. electron beam of several milliamperes. While the beam dynamics of the high-current electron beam are tenable, sustaining this current for weeks of user operations requires an unprecedented charge lifetime from a high-polarization GaAs-based photocathode. A promising approach to exceed the kilocoulomb charge lifetime barrier is reducing the ion back-bombardment fluence at the photocathode. By increasing the laser size and managing the emittance growth with an adequate cathode/anode design, significantly enhanced charge lifetime may be achieved. Based upon a new simulation model that qualitatively explains the lifetime data previously measured at different spot sizes, we describe the practical implications on the parameter space available for a kilocoulomb-lifetime polarized photogun design.

Bruker, M.↗

Toward a long-lifetime polarized photoelectron gun for the Ce+BAF positron source

The addition of spin-polarized, continuous-wave (c.w.) positron beams to the 12 GeV Continuous Electron Beam Accelerator Facility (CEBAF) would provide a significant capability to the experimental nuclear physics program at Jefferson Lab. Based on bremsstrahlung and pair-production in a high-Z target, the positron source requires a 120 MeV spin-polarized c.w. electron beam of several milliamperes. While the beam dynamics of the high-current electron beam are tenable, sustaining this current for weeks of user operations requires an unprecedented charge lifetime from a high-polarization GaAs-based photocathode. A promising approach to exceed the kilocoulomb charge lifetime barrier is reducing the ion back-bombardment fluence at the photocathode. By increasing the laser size and managing the emittance growth with an adequate cathode/anode design, significantly enhanced charge lifetime may be achieved. Based upon a new simulation model that qualitatively explains the lifetime data previously measured at different spot sizes, we describe the practical implications on the parameter space available for a kilocoulomb-lifetime polarized photogun design.

Bruker, M.↗

Considerations for Fire Service Response to Residential Battery Energy Storage System Incidents

Renewable energy sources (e.g., rooftop photovoltaics, wind turbines) are capable of addressing our grid-level energy challenges by reducing environmental impacts, increasing resiliency, and increasing the supply of input energy. However, renewable energy sources alone are not a complete solution. The generation of power from major renewable energy sources fluctuates with the weather, creating significant challenges in matching electrical power generation to electrical power consumption. The value of renewable power generation sources is multiplied when paired with battery energy storage systems (ESS), which can store excess power generated from renewable energy sources when it is not consumed and deliver that power later when demand exceeds base power generation. Residential ESS units are frequently installed to support renewable energy initiatives by storing energy from intermittent sources such as photovoltaic panels. Residential ESS units also offer an alternative to gas-powered generators or other backup power means. Lithium-ion batteries are the most common residential ESS technology due to their affordability and energy density. Though lithium-ion systems come with benefits, there is also a risk of thermal runaway within this technology which can result in flammable gas release, fire, and explosion. As the installations of these products increase, the frequency of response to fire incidents involving these products will increase. In response to this new and evolving hazard, UL Solutions (ULS) and UL Fire Safety Research Institute (FSRI) have partnered with the International Association of Fire Fighters (IAFF) to conduct a series of large-scale tests sponsored by the US Department of Energy to characterize the challenges for fire fighters responding to fires involving residential energy storage systems. The project focuses on developing size-up and tactical considerations to support the fire service in navigating the evolving modern fireground.

25 ENERGY STORAGE↗

Qualification of Processing Batches for Tank Closure Cesium Removal Through In-Tank Batch Contact Testing - 20470

The Tank Closure Cesium Removal (TCCR) process at the Savannah River Site (SRS) is currently processing waste from Tank 10H, generating decontaminated salt solution that is sent to Tank 11H. Transfers out of Tank 11H are then disposed of on site as a grout wasteform in the SRS Saltstone Processing Facility. This is a full-scale demonstration of the use of Crystalline Silicotitanate (CST) for the decontamination of aqueous nuclear waste supernate. CST primarily removes cesium from the high sodium alkaline feed, but also adsorbs strontium, actinides, and some other trace metals. The TCCR unit is an at-tank set of four ion exchange columns, with two typically being operated in series during waste processing. Tank 10H is serving a dual function as both the salt dissolution tank as well as the feed tank for the TCCR system. Prior to operation of TCCR, Tank 10H must undergo dissolution campaigns, dissolving the salt cake to form an aqueous salt solution (supernate). After each dissolution campaign, the supernate created must be qualified prior to processing through the TCCR system. Qualification includes detailed characterization of the supernate as well as in-tank batch contact tests to determine the equilibrium loading of Cs-137 on the CST ion exchange media (IONSIV{sup TM} R9120-Ba). In support of the in-tank batch contact testing, Savannah River National Laboratory (SRNL) developed a CST sample holder, also referred to as a 'tea-bag', to hold a measured amount (∼0.1 grams) of pretreated CST between stainless steel screens. The tea-bag fits within a standard stainless steel sample vial that has been modified to allow the flow of supernate to the CST. This sample holder is then immersed in the waste tank allowing free contact between the CST beads and the surrounding liquid, at an effectively infinite liquid-to-solid phase ratio. A pair of tea-bags are deployed in the tank for a period of 10 days for each batch, after which the CST is recovered, digested, and analyzed to determine the loading of cesium isotopes on the CST. This result then supports the TCCR column thermal loading limits for processing as part of the TCCR safety basis. This paper will discuss the design and testing of the CST sample holder, as well as results from the first few batches of waste qualified and subsequently processed through the TCCR system. In addition, results from analyses of Tank 11H samples, showing decontamination of the product will be included. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Unimodal Imaging of Monovalent Metal-Chelator Complexes and Lipids by MALDI Imaging Mass Spectrometry

Careful regulation of monovalent metal ions (M + ) is necessary to maintain a functional cellular system. Of these ions, appropriate sodium (Na + ) and potassium (K + ) concentrations are particularly integral for electrochemical signaling, as well as the secondary transport of nutrients and waste. Dysregulation of M + homeostasis can disrupt these mechanisms, potentially influencing the metabolism of downstream biomolecules such as lipids. Thus, the relationship between M + abundances and related biomolecular distributions must be elucidated to better understand the physiology of healthy and disordered tissues. Traditional techniques for imaging biological metal distributions include SIMS, LA-ICP-MS, and XRF; however, these capabilities are limited to elemental analysis or the analysis of molecular fragments and must be paired with other modalities to visualize distributions of more complex biomolecules within the same or similar samples. Conversely, matrix-assisted laser desorption/ionization imaging mass spectrometry (MALDI IMS) is a powerful tool often used for mapping such biomolecular distributions, but current methods are unable to detect metals within tissue. This study illustrates a novel methodology that adds metal detection to the MALDI IMS repertoire through which the simultaneous detection of M + metals and lipids is achievable. Using a robotic sprayer for homogeneous application, on-tissue deposition of the chelator deferiprone (DEF) enables subsequent detection of the ionizable metal-chelator complex by MALDI without hindering lipid detection. Our work provides proof-of-concept data for the simultaneous detection of K + , Na + , and intact lipids using MALDI IMS.

59 BASIC BIOLOGICAL SCIENCES↗

Water–Hydrocarbon Interactions in Anionic Pyrene Monohydrate

Interactions between water and polycyclic aromatic hydrocarbons are essential in many aspects of chemistry, from interstellar and atmospheric processes to interfacial hydrophobicity and wetting phenomena. Despite their growing importance, the intermolecular potentials of the water-hydrocarbon interactions are underdeveloped compared to water-water potentials, and there are similarly few experimental probes that are sensitive to the details of the water-hydrocarbon potential. We present a combined experimental and computational study of anionic pyrene monohydrate, one of the simplest water/hydrocarbon clusters. The action spectrum in the OH region of the mass-selected cluster ion provides a rigorous benchmark for intermolecular potentials and computational methodologies. We identify missing intermolecular interactions and shortcomings in conventional dynamics calculations by comparing experimental data to density functional theory and classical molecular dynamics calculations. Kinetic trapping is prevalent, even for one water molecule and one pyrene molecule, leading to slow equilibration in conventional molecular dynamics calculations, even on nanosecond timescales and at low temperatures (50 K). At constant energy, temperature fluctuations for the pair of molecules are substantial. Immersing the system in a bath of soft spheres and employing parallel tempering alleviates kinetic trapping and dampens temperature fluctuations, bringing the system closer to the thermodynamic limit. With such augmented sampling, a simple, flexible water model reproduces the linewidth and the asymmetric broadening of the symmetric OH stretching mode, which we assign to spectral diffusion. In the OH stretching region, dynamics calculations predict a more intense antisymmetric peak than experiments observe but do not predict the bimodal split symmetric peak that the experiments show. Furthermore, our work suggests that electronic polarization, missing in the empirical force field, is responsible for the first discrepancy and that quantum nuclear effects, captured neither in density functional theory nor in classical dynamics, may be responsible for the second.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NENCI-2021. I. A large benchmark database of non-equilibrium non-covalent interactions emphasizing close intermolecular contacts

In this work, we present NENCI-2021, a benchmark database of ~8000 Non-Equilibirum Non-Covalent Interaction energies for a large and diverse selection of intermolecular complexes of biological and chemical relevance. To meet the growing demand for large and high-quality quantum mechanical data in the chemical sciences, NENCI-2021 starts with the 101 molecular dimers in the widely used S66 and S101 databases and extends the scope of these works by (i) including 40 cation–π and anion–π complexes, a fundamentally important class of non-covalent interactions that are found throughout nature and pose a substantial challenge to theory, and (ii) systematically sampling all 141 intermolecular potential energy surfaces (PESs) by simultaneously varying the intermolecular distance and intermolecular angle in each dimer. Designed with an emphasis on close contacts, the complexes in NENCI-2021 were generated by sampling seven intermolecular distances along each PES (ranging from 0.7× to 1.1× the equilibrium separation) and nine intermolecular angles per distance (five for each ion–π complex), yielding an extensive database of 7763 benchmark intermolecular interaction energies (E int ) obtained at the coupled-cluster with singles, doubles, and perturbative triples/complete basis set [CCSD(T)/CBS] level of theory. The E int values in NENCI-2021 span a total of 225.3 kcal/mol, ranging from -38.5 to +186.8 kcal/mol, with a mean (median) E int value of -1.06 kcal/mol (-2.39 kcal/mol). In addition, a wide range of intermolecular atom-pair distances are also present in NENCI-2021, where close intermolecular contacts involving atoms that are located within the so-called van der Waals envelope are prevalent—these interactions, in particular, pose an enormous challenge for molecular modeling and are observed in many important chemical and biological systems. A detailed symmetry-adapted perturbation theory (SAPT)- based energy decomposition analysis also confirms the diverse and comprehensive nature of the intermolecular binding motifs present in NENCI-2021, which now includes a significant number of primarily induction-bound dimers (e.g., cation–π complexes). NENCI-2021 thus spans all regions of the SAPT ternary diagram, thereby warranting a new four-category classification scheme that includes complexes primarily bound by electrostatics (3499), induction (700), dispersion (1372), or mixtures thereof (2192). A critical error analysis performed on a representative set of intermolecular complexes in NENCI-2021 demonstrates that the E int values provided herein have an average error of ±0.1 kcal/mol, even for complexes with strongly repulsive E int values, and maximum errors of ±0.2–0.3 kcal/mol (i.e., ~±1.0 kJ/mol) for the most challenging cases. For these reasons, we expect that NENCI-2021 will play an important role in the testing, training, and development of next-generation classical and polarizable force fields, density functional theory approximations, wavefunction theory methods, and machine learning based intra- and inter-molecular potentials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Computational and Experimental Characterization of the Ligand Environment of a Ni-Oxo Catalyst Supported in the Metal–Organic Framework NU-1000

Heterogeneous catalysts exhibit significant changes in composition due to the influence of operating conditions, and these compositional changes can have dramatic effects on catalytic performance. For traditional bulk metal heterogeneous catalysts, relationships between composition and catalytic operating conditions are well documented. However, the influence of operating conditions on the compositions of single-site heterogeneous catalysts remains largely unresolved. To address this, we report a combined computational and experimental characterization of a Ni oxo catalyst under catalytic hydrogenation conditions. Specifically, pair distribution function (PDF) analysis is combined with ab initio thermodynamic modeling to investigate ligand environments present on a Ni oxo cluster supported in the metal–organic framework NU-1000. Comparisons of the experimentally observed and simulated Ni–O coordination numbers and Ni–O, Ni···Ni, and Ni···Zr distances provide insight into the Ni ligand environment under H 2 (g). These comparisons suggest significant OH and H 2 O content and, further, that different Ni ions within the cluster and/or NU-1000 structure may comprise subtly different numbers of these ligands. Further, the observation of significant H 2 O content under H 2 (g) suggests that the NU-1000 support supplies H 2 O to the cluster. Examples of ligand environments that could lead to the observed PDFs are provided. Furthermore, the combination of simulations and experiments provides new insights into the ligand environment for Ni-NU-1000 catalysts that will be useful for understanding the ligand environments of other single-site Ni catalysts as well.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stabilizing lithium-metal electrodes with polymer coatings

Increasing the energy density of batteries can accelerate the deployment of electric vehicles, expand the utilization of renewable energy and, in turn, reduce greenhouse gas emissions. Different from commercially available lithium-ion batteries, high-energy-density lithium-metal batteries use metallic lithium instead of graphite as the negative electrode. Furthermore, the commercialization of lithium-metal batteries is hindered by the electrochemical instability of lithium metal. Polymer coatings have shown promise in addressing issues related to each step of heterogeneous lithium deposition. Here we summarize the current understanding of key design principles and highlight relevant coating compositions. Moreover, we discuss high-performing coating–electrolyte pairs and provide an outlook on interface design for novel electrolytes.

Batteries↗

SN 2010j1: Optical to Hard X-Ray Observations Reveal an Explosion Embedded in a Ten Solar Mass Cocoon

Some supernovae (SNe) may be powered by the interaction of the SN ejecta with a large amount of circumstellar matter (CSM). However, quantitative estimates of the CSM mass around such SNe are missing when the CSM material is optically thick. Specifically, current estimators are sensitive to uncertainties regarding the CSM density profile and the ejecta velocity. Here we outline a method to measure the mass of the optically thick CSM around such SNe. We present new visible-light and X-ray observations of SN 2010jl (PTF 10aaxf), including the first detection of an SN in the hard X-ray band using NuSTAR. The total radiated luminosity of SN 2010jl is extreme atleast 9 1050 erg. By modeling the visible-light data, we robustly show that the mass of the circumstellar material within 1016 cm of the progenitor of SN 2010jl was in excess of 10M_. This mass was likely ejected tens of years prior to the SN explosion. Our modeling suggests that the shock velocity during shock breakout was 6000 km s1, decelerating to 2600 km s1 about 2 yr after maximum light. Furthermore, our late-time NuSTAR and XMM spectra of the SN presumably provide the first direct measurement of SN shock velocity 2 yr after the SN maximum light measured to be in the range of 2000-4500 km s1 if the ions and electrons are in equilibrium, and_2000 km s1 if they are not in equilibrium. This measurement is in agreement with the shock velocity predicted by our modeling of the visible-light data. Our observations also show that the average radial density distribution of the CSM roughly follows an r2 law. A possible explanation for the _10M_ of CSM and the wind-like profile is that they are the result of multiple pulsational pair instability events prior to the SN explosion, separated from each other by years.

circumstellar matter (CSM)↗

Effects of surface vacancy-adatom pair formation on PFC tungsten surface morphological response

Abstract We report a simulation study of the effect of He-irradiation-induced surface vacancy-adatom pair formation on the surface morphological evolution of plasma-facing component (PFC) tungsten and examine a number of factors that impact such evolution. Our analysis is based on self-consistent dynamical simulations according to an atomistically-informed, continuum-scale surface evolution model that has been developed following a hierarchical multiscale modeling strategy and can access the spatiotemporal scales of relevance to fuzz formation. The model accounts for the flux of surface adatoms generated as a result of the surface vacancy-adatom pair formation effect upon He implantation, which contributes to the anisotropic growth of surface nanostructural features due to the different rates of adatom diffusion along and across step edges of islands on the tungsten surface. We have carried out atomic-scale computations of optimal diffusion pathways along and across island step edges on the W(110) surface and calculated Ehrlich–Schwoebel (ES) barriers in adatom diffusion along and across such step edges. This aspect of surface adatom diffusion contributes to anisotropic surface atomic fluxes, terrace and step diffusive currents, and has been incorporated into our PFC surface evolution model, which predicts the formation of preferentially aligned nanoridge stripe patterns on the PFC surface. We establish that these anisotropic diffusive currents accelerate nanotendril growth on the PFC surface and the onset of surface nanostructure pattern formation. We also explore systematically the dependence of the PFC surface morphological response on the surface temperature and He ion incident flux, characterize in detail the resulting surface topographies and growth kinetics, and compare the predicted surface morphologies with experimental observations. Our simulation predictions for the emerging surface nanostructure patterns under certain plasma exposure conditions are consistent with experimental findings in the literature.

36 MATERIALS SCIENCE↗

Colloidal Stability of PFSA-Ionomer Dispersions Part II: Determination of Suspension pH Using Single-Ion Potential Energies

Perfluorosulfonic acid (PFSA) ionomers serve a vital role in the performance and stability of fuel-cell catalyst layers. These properties, in turn, depend on the colloidal processing of precursor inks. Here, to understand the colloidal structure of fuel-cell catalyst layers, we explore the aggregation of PFSA ionomers dissolved in water/alcohol solutions and relate the predicted aggregation to experimental measurements of solution pH. Not all side chains contribute to measured pH because of burying inside particle aggregates. To account for the measured degree of dissociation, a new description is developed for how PFSA aggregates interact with each other. The developed single-counterion electrostatic repulsive pair potential from Part I is incorporated into the Smoluchowski collision-based kinetics of interacting aggregates with buried side chains. We demonstrate that the surrounding solvent mixture affects the degree of aggregation as well as the pH of the system primarily through the solution dielectric permittivity, which drives the strength of the interparticle repulsive energies. Successful pH prediction of Nafion ionomer dispersions in water/n-propanol solutions validates the numerical calculations. Nafion-dispersion pH measurements serve as a surrogate for Nafion particle-size distributions. The model and framework can be leveraged to explore different ink formulations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dusty-Plasma Particle Accelerator

A dusty-plasma apparatus is being investigated as means of accelerating nanometer- and micrometer-sized particles. Applications for the dusty-plasma particle accelerators fall into two classes: Simulation of a variety of rapidly moving dust particles and micrometeoroids in outer-space environments that include micrometeoroid streams, comet tails, planetary rings, and nebulae and Deposition or implantation of nanoparticles on substrates for diverse industrial purposes that could include hardening, increasing thermal insulation, altering optical properties, and/or increasing permittivities of substrate materials. Relative to prior apparatuses used for similar applications, dusty-plasma particle accelerators offer such potential advantages as smaller size, lower cost, less complexity, and increased particle flux densities. A dusty-plasma particle accelerator exploits the fact that an isolated particle immersed in plasma acquires a net electric charge that depends on the relative mobilities of electrons and ions. Typically, a particle that is immersed in a low-temperature, partially ionized gas, wherein the average kinetic energy of electrons exceeds that of ions, causes the particle to become negatively charged. The particle can then be accelerated by applying an appropriate electric field. A dusty-plasma particle accelerator (see figure) includes a plasma source such as a radio-frequency induction discharge apparatus containing (1) a shallow cup with a biasable electrode to hold the particles to be accelerated and (2) a holder for the substrate on which the particles are to impinge. Depending on the specific design, a pair of electrostatic-acceleration grids between the substrate and discharge plasma can be used to both collimate and further accelerate particles exiting the particle holder. Once exposed to the discharge plasma, the particles in the cup quickly acquire a negative charge. Application of a negative voltage pulse to the biasable electrode results in the initiation of a low-current, high-voltage cathode spot. Plasma pressure associated with the cathode spot as well as the large voltage drop at the cathode spot accelerates the charged particles toward the substrate. The ultimate kinetic energy attained by particles exiting the particle holder depends in part on the magnitude of the cathode spot sheath potential difference, which is proportional to the magnitude of the voltage pulse, and the on the electric charge on the dust. The magnitude of the voltage pulse can be controlled directly, whereas the particle s electric charge can be controlled indirectly by controlling the operating parameters of the plasma apparatus.

Foster, John E.↗

Mechanically Robust Bismuth-Embedded Carbon Microspheres for Ultrafast Charging and Ultrastable Sodium-Ion Batteries

Advancements in the development of fast-charging and long-lasting microstructured alloying anodes with high volumetric capacities are essential for enhancing the operational efficiency of sodium-ion batteries (SIBs). These anodes, however, face challenges such as declined cyclability and rate capability, primarily due to mechanical degradation reduced by significant volumetric changes (over 252%) and slow kinetics of sodium-ion storage. Herein, we introduce a novel anode design featuring densely packed bismuth (Bi) embedded within highly conductive carbon microspheres to overcome the aforementioned challenges. Remarkably, the high loading Bi anode within carbon microspheres with a high tap density of 2.59 g cm -3 possesses significant mechanical strength exceeding 590 MPa and limits volume swelling of only 10.9% post-sodiation. This anode demonstrates a high volumetric capacity (908.3 mAh cm -3 ), ultrafast chargeability (200 A g -1 , full charge/discharge in just 5.5 s), and outstanding cyclability over 12,000 cycles and maintains exceptional cycling stability even at -30 °C. The full cell paired with a Na 3 V 2 (PO 4 ) 3 cathode retains over 80% capacity after 600 cycles at 36 C, demonstrating a remarkable rate capability of 126 C (full charge/discharge in 28.6 s). Our comprehensive experimental evaluations and chemo-mechanical simulations shed light on the mechanisms underpinning the anode's superior performance. In conclusion, this development marks a significant advancement in the design of durable and fast-charging anodes for high-performance SIBs.

25 ENERGY STORAGE↗