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Results for “Single Ion Conducting”

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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Optimization of Graphite–SiO blend electrodes for lithium-ion batteries: Stable cycling enabled by single-walled carbon nanotube conductive additive

Lithium-alloying materials are of great interest to improve the gravimetric and volumetric energy density of lithium-ion batteries, though their associated volume fluctuation with cycling often leads to poor cycling performance. Active-inactive alloys and blending alloys with carbon materials are common strategies to accommodate volume fluctuation. Herein we set out to optimize graphite-SiO blend electrode formulations to eliminate rapid capacity fade. Electrodes with highly stable cycling were prepared by simple planetary mixing procedures, enabled by the use of just a fraction of a weight percent of commercial SWCNTs as the only conductive additive, and by the appropriate choice of binder/stabilizing agent. In fact, the use of SWCNTs allowed for graphite-free SiO electrodes with approximately 74% higher volumetric energy density relative to traditional graphite electrodes, and superior capacity retention in coin-type full-cell testing versus NMC532 cathodes.

25 ENERGY STORAGE↗
DOE OSTI2024

Ion concentration polarization causes a nearly pore-length-independent conductance of nanopores

There has been a great amount of interest in nanopores as the basis for sensors and templates for preparation of biomimetic channels as well as model systems to understand transport properties at the nanoscale. The presence of surface charges on the pore walls has been shown to induce ion selectivity as well as enhance ionic conductance compared to uncharged pores. Here, using three-dimensional continuum modeling, we examine the role of the length of charged nanopores as well as applied voltage for controlling ion selectivity and ionic conductance of single nanopores and small nanopore arrays. First, we present conditions where the ion current and ion selectivity of nanopores with homogeneous surface charges remain unchanged, even if the pore length decreases by a factor of 6. This length-independent conductance is explained through the effect of ion concentration polarization (ICP), which modifies local ionic concentrations, not only at the pore entrances but also in the pore in a voltage-dependent manner. We describe how voltage controls the ion selectivity of nanopores with different lengths and present the conditions when charged nanopores conduct less current than uncharged pores of the same geometrical characteristics. The manuscript provides different measures of the extent of the depletion zone induced by ICP in single pores and nanopore arrays, including systems with ionic diodes. In conclusion, the modeling shown here will help design selective nanopores for a variety of applications where single nanopores and nanopore arrays are used.

Cain, DaVante↗
DOE OSTI2024

Water, Solute, and Ion Transport in De Novo-Designed Membrane Protein Channels

Biological organisms engineer peptide sequences to fold into membrane pore proteins capable of performing a wide variety of transport functions. Synthetic de novo-designed membrane pores can mimic this approach to achieve a potentially even larger set of functions. Here, in this work, we explore water, solute, and ion transport in three de novo designed β-barrel membrane channels in the 5–10 Å pore size range. We show that these proteins form passive membrane pores with high water transport efficiencies and size rejection characteristics consistent with the pore size encoded in the protein structure. Ion conductance and ion selectivity measurements also show trends consistent with the pore size, with the two larger pores showing weak cation selectivity. MD simulations of water and ion transport and solute size exclusion are consistent with the experimental trends and provide further insights into structure–function correlations in these membrane pores.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Effect of Tethering Anions in Block Copolymer Electrolytes via Molecular Dynamics Simulations

Ion-containing block copolymers (BCPs) are promising solid-state electrolytes as they can combine ion conduction and mechanical robustness via multiple microphases. However, salt-doped BCPs can have low ion conduction and transference number. One strategy to increase transference number is to tether anions to the polymer backbone (creating a single-ion conductor), though this may impact cation mobility. Leveraging coarse-grained molecular dynamics simulations, we compare the effects of ion concentration and polymer dielectric constant on BCPs with and without bonding anions to the chain (without changing any other chemical properties). We find that single-ion BCPs have higher cation conductivity than analogous salt-doped BCPs, especially at moderate ion concentrations. Furthermore, we also compare several structural features of these systems; notably, tethering anions causes the ions to spread more evenly throughout the conducting phase, which is related to improved cation conduction.

25 ENERGY STORAGE↗
DOE OSTI2020

Mechanisms of activation and desensitization of full-length glycine receptor in lipid nanodiscs

Glycinergic synapses play a central role in motor control and pain processing in the central nervous system. Glycine receptors (GlyRs) are key players in mediating fast inhibitory neurotransmission at these synapses. While previous high-resolution structures have provided insights into the molecular architecture of GlyR, several mechanistic questions pertaining to channel function are still unanswered. Here, we present Cryo-EM structures of the full-length GlyR protein complex reconstituted into lipid nanodiscs that are captured in the unliganded (closed), glycine-bound (open and desensitized), and allosteric modulator-bound conformations. A comparison of these states reveals global conformational changes underlying GlyR channel gating and modulation. The functional state assignments were validated by molecular dynamics simulations, and the observed permeation events are in agreement with the anion selectivity and conductance of GlyR. These studies provide the structural basis for gating, ion selectivity, and single-channel conductance properties of GlyR in a lipid environment.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Ion Transport in Carbon Nanotube Porins with a pH-Switchable Entrance Gate

Molecular transport in nanofluidic channels often differs drastically from conventional bulk transport. Strong confinement in those channels amplifies the roles of surface transport, surface defects, and molecular gates. Here, in this study, we introduce a chemical functionality at the nanotube rim that acts as a pH-triggered molecular gate by forming a movable lid that blocks the pore entrance. We use ion and proton transport measurements to show that these sub-1 nm diameter fluorescent ultrashort carbon nanotube porins (FUNPs) modulate ion transport by switching between the “open” and “closed” conformations of this gate. Specifically, at neutral pH the channel lid is open, allowing unimpeded ion transport through the gate, whereas at acidic pH values the lid forms a “closed” conformation that blocks transport through the nanotube. We also report first-principles MD simulations that confirm this gating mechanism and reveal molecular details of the ion and proton transport processes in these functional nanopores.

Carbon nanotubes↗
DOE OSTI2021

Computational study of Li3BO3 and Li3BN2 I: Electrolyte properties of pure and doped crystals

Both Li3BO3 and Li3BN2 materials have promising properties for use in all-solid-state batteries and other technologies dependent on electrolytes with significant ionic conductivity. As the first of a two-part study, this paper reports the analysis of detailed simulations of Li ion diffusion in the monoclinic forms of these materials. Using both NEB and MD methods, it is clear that Li ion migration via vacancy mechanisms provides the most efficient ion transport in each material. While the results suggest that interstitial defects in these materials do not play a direct role in Li ion migration, their relative stability seems to enhance vacancy production via the formation of Frenkel-type defects. This may partially explain why the Li ion conductivities computed from MD simulations of samples initially containing a single Li ion vacancy are in reasonable agreement with measured values of this work for Li3BO3 and those reported in the literature for poorly crystalline samples of both materials. The possibility of increasing vacancy concentrations by substitutional doping (F for O in Li3BO3 and C for B in Li3BN2) is also examined, finding simulated conductivities comparable to those of the ideal vacancy model.

Li, Yan↗
DOE OSTI2020

Thermal transport across nanoscale damage profile in sapphire irradiated by swift heavy ions

In this work, we studied the degradation of thermal conductivity in single crystal sapphire (α-Al 2 O 3 ) irradiated by 167 MeV Xe swift heavy ions (SHIs) over the multiple fluences in the range of 10 12 –10 14 ions/cm 2 . Thermal conductivity was measured primarily in the cross-plane direction using a noncontact ultrafast optical pump-probe technique called picosecond time domain thermoreflectance (TDTR). Multiple samples with variable ion fluences allowed us to probe distinct regions resulting from different regimes of microstructure evolution caused by electronic energy loss. By tuning the penetration depth of the thermal waves using different modulation frequencies, two regions with distinct conductivities were identified and the values of which were found to be consistent with phonon-mediated thermal transport models while the microstructure was confirmed by electron microscopy characterization. These damaged regions were determined to be a several micrometer thick ion track region and several tens of nanometer-thick amorphous layer present only above 5.0 × 10 13 ions/cm 2 . These results demonstrate the applicability of TDTR to resolve thermal transport behavior in SHI irradiated oxides having nonhomogeneous damage profile on a nanometer scale. The presented approach facilitates future studies aiming at resolving the impact of distinct damage resulting from electronic and nuclear stopping regimes under irradiation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2020

Temperature and processing effects on lithium ion conductivity of solution‐deposited lithium zirconium phosphate (LiZr 2 P 3 O 12 ) thin films

Abstract Lithium zirconium phosphate (LiZr 2 P 3 O 12 ) thin films have been prepared on platinized silicon substrates via a chemical solution deposition approach with processing temperatures between 700°C and 775°C. Films that were subject to a single high‐temperature anneal were found to crystallize at temperatures above 725°C. Crystallization was observed in films annealed after each deposited layer at 700°C and above. In both cases, grain size was found to increase with annealing temperature. Ion conductivity was found to increase with annealing temperature in singly annealed films. In per‐layer annealed films ion conductivity was found to initially increase then decrease with increasing annealing temperature. A maximum ion conductivity of 1.6 × 10 −6 S/cm was observed for the singly annealed 775°C condition, while a maximum ion conductivity of 5.8 × 10 −7 S/cm was observed for the 725°C per‐layer annealed condition. These results are consistent with an increasing influence of cross‐plane, internal interface resistance and vapor phase carrier loss in the per‐layer annealed samples. This work demonstrates that post‐deposition processing methods can strongly affect the ion conducting properties of LiZr 2 P 3 O 12 thin films.

Brummel, Ian A.↗
DOE OSTI2021

Recent performance of the SNS H - ion source with a record long run

The Spallation Neutron Source (SNS) accelerator system includes a 65 keV H - injector, a 2.5 MeV radio frequency quadrupole (RFQ), a 1 GeV linac chain (DTL-CCL-SCL) and an accumulator ring. The H - injector consists of an RF-driven, Cs-enhanced, multi-cusp H - ion source and a compact, two-lens electrostatic low energy beam transport (LEBT). In 2018, a new RFQ was installed in place of the original RFQ along with upgraded ion source support infrastructure. This paper presents the operational performance and some highlights of beam studies with the SNS ion source since the new RFQ was put into operation. SNS routinely operates at 1.4 MW average beam power for three run cycles per year. During the most recently finished run, FY20B, we operated a single source for the entire run spanning ~4 months with a >99.5% availability. A single dose of cesiation was conducted during the ion source startup which yielded ≥54 mA current for the entire run with just few minor adjustments of parameters.

Han, Baoxi↗
DOE OSTI2026

Four-Dimensional Quasielastic Neutron Scattering (4D-QENS) Analysis of Correlated Ionic Conduction in Sr⁢Cl2

Methods of elucidating the mechanisms of fast-ion conduction in solid-state materials are pivotal for advancements in energy technologies such as batteries, fuel cells, sensors, and supercapacitors. In this study, we examine the ionic conduction pathways in single crystal Sr⁢Cl2, which is a fast-ion conductor above 900 K, using four-dimensional quasielastic neutron scattering (4D-QENS). We explore both coherent and incoherent neutron scattering at temperatures above the transition temperature into the superionic phase to explore the correlated motion of hopping anions. Refinements of the incoherent QENS yield residence times and jump probabilities between lattice sites in good agreement with previous studies, confirming that ionic hopping along nearest-neighbor directions is the most probable conduction pathway. However, the coherent QENS reveals evidence of de Gennes narrowing, indicating the importance of ionic correlations in the conduction mechanism. This highlights the need for improvements both in the theory of ionic transport in fluorite compounds and the modeling of coherent 4D-QENS in single crystals.

Coles, Jared [Materials Science Division, Argonne ↗
DOE OSTI2024

Ion transport in composites of binary electrolyte and single ion conductor—A chronoamperometry study

Composite electrolytes for lithium batteries typically combine materials with very different mechanical properties and ionic transport mechanisms and the degree to which these two phases affect each other is not well understood. In this work we used numerical simulations and experiments to investigate the transport in composite electrolytes consisting of polyethylene oxide (PEO) with Lithium bis-triuoromethanesulfonimide (LiTFSI) and Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 (LATP) lithium ion conducting glass-ceramic particles. In particular we are interested in how the introduction of a single ion conductor (SIC) changes the salt concentration gradients in the polymer electrolyte (PE) under applied potential. To study this, we performed numerical simulations and chronoamperometry experiments in electrolytes with different arrangements of the SIC and PE phases, i.e. layers and particulate composites. The results show that the particulate composites have the highest concentration gradients and take the longest time to reach steady state current. Furthermore, the high concentration gradient can be exacerbated by a high SIC/PE interfacial resistance. Finally, the best arrangement appears to have a layer of SIC impenetrable to anions in the polymer phase within the electrolyte membrane.

25 ENERGY STORAGE↗
DOE OSTI2020

Interpenetration and kinetic effects in converging, high-energy plasma jets

In this work, we report on numerical simulations of laser-driven convergent plasma fusion targets. These “inverted corona” fusion targets are useful for the study of counter-streaming and converging rarefied plasma flows, and previous experiments have demonstrated their potential as neutron sources. The scheme consists of a fuel layer lined along the interior surface of a hollow plastic shell that is laser-ablated and expands inward towards the target center. The plasma streams generated in these targets are initially nearly collisionless as they converge, leading to wide interaction length scales and long interaction time scales as the jets interpenetrate. Such kinetic effects impact mixing of constituent ions - a phenomenon not properly captured by single-fluid hydrodynamic simulations. Here we conduct numerical simulations using two different methods: (1) single-fluid simulations in HYDRA, and (2) kinetic-ion, fluid-electron hybrid particle-in-cell (PIC) simulations in the code Chicago. It is shown that the initially nearly collisionless plasma fronts interpenetrate deeply and lead to broader interaction regions in space and time resulting in significant beam-beam fusion. The two approaches make different, testable predictions for the effect of fuel-layer thickness on neutron yield.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Factors Affecting the Electron Conductivity in Single Crystal Li 7 La 3 Zr 2 O 12 and Li 7 P 3 S 11

One of the serious challenges in all solid-state Li ion batteries is neutral Li intrusion into the solid-state electrolyte that can ultimately cause catastrophic failure. One possibility for this is due to n-type electron conductivity that induces the reaction Li + + e – → Li 0 at sites where the potential is less than the Li + /Li potential. This paper reports hybrid density functional theory calculations of the electronic conductivity in two prototype single crystalline solid-state electrolytes, cubic Li 7 La 3 Zr 2 O 12 (c-LLZO) and Li 7 P 3 S 11 (LPS). The formation energies of important point defects that can affect electron conductivity are determined, and we find that the mechanism of n-type electron conductivity for both solid-state electrolytes is via “small” electron polaron hopping, where the quotes signify that substantial Li ion rearrangement is associated with the polaron formation and its migration. In both electrolytes, the formation energies for the small polarons at the Fermi energy are too high to generate measurable electron conductivity at room temperature. For c-LLZO, the concentration of electron polarons necessary to ensure charge neutrality from positively charged oxygen vacancies formed in synthesis can be significantly higher. Hence, the electron conductivity could be significant when measured with ion-blocking metal electrodes, and we discuss how the synthesis conditions could affect this magnitude. However, in the solid-state battery, these polarons are replaced by negatively charged Li vacancies so that the electron conductivity should remain minimal. For LPS single crystals, the inherent minimal electron conductivity is independent of synthesis conditions. Here we also show that the cost of forming Li 0 in bulk c-LLZO is enormous due to strain effects so that it could only potentially form at voids, grain boundaries, or around vacancy defects which relax the lattice strain.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Stationary Oxygen Vacancy Construction toward a Superior-Performance Ultrahigh Nickel Single-Crystal Cathode

Oxygen vacancies exert a complex and profound influence on the layered cathodes, especially those with ultrahigh nickel content. They can facilitate lithium-ion transport and enhance electronic conductivity, while aggressive oxygen vacancy formation causes structural degradation and electrolyte decomposition. Herein, taking ultrahigh nickel single-crystal LiNi 0.92 Co 0.06 Mn 0.02 O 2 (SC-Ni92) as a model material, we propose a pinning strategy to harness the benefits of oxygen vacancies while mitigating their detrimental effects. Through a carefully controlled thermal process, both oxygen vacancies and pinning atoms are successfully introduced into the surface region. The resulting anchored oxygen vacancies, capitalizing on their inherent advantages, improve conductivity and lithium-ion diffusion. Simultaneously, the neighboring pinning atoms effectively increase the migration barrier and suppress the adverse effects of these vacancies, including electrolyte decomposition and structural degradation during long-term electrochemical cycling. Consequently, oxygen vacancy-anchored single-crystal LiNi 0.92 Co 0.06 Mn 0.02 O 2 (SC-Ni92-OV) demonstrates significantly improved high-voltage electrochemical performance, with 86.16% capacity retention after 200 cycles at 4.6 V and 1 C in a half-cell and 90.71% after 300 cycles at 4.5 V and 1 C in a full cell. Furthermore, this study not only provides valuable insights into the chemistry of oxygen vacancy but also introduces a viable strategy for leveraging oxygen vacancies to achieve stable high-voltage performance in ultrahigh nickel single-crystal cathodes.

defects in solids↗
DOE OSTI2021

Cytochrome Nanowire XRD

Microbial metabolism plays an important role in the global cycling of carbon, nutrients, and metals. Recent discovery of microorganisms sharing energy using direct electrical connections might represent a prominent strategy by which anaerobic microorganisms interact with the diversity of environments. The purpose of the proposed research is to apply these newly developed principles of electron exchange in microbial communities to the study of biogeochemical cycling in climate and subsurface systems. Previous studies revealed that soil bacteria Geobacter sulfurreducens produce conductive pili nanofilaments that facilitate long-range electron transport to extracellular electron acceptors and other cells. This discovery has already transformed our understanding of the function of microbial communities in diverse environments, making basic contributions to microbial ecology and helping to improve practical applications such as increasing current output of microbial fuel cells and enhancing the conversion of organic waste to methane. Microbial electron exchange via pili may also contribute to methane production in terrestrial environments that are major sources of atmospheric methane. However, the mechanism of electron transport through pili is not well understood. Initial studies have suggested that pili exhibit metallic-like conductivity similar to conducting polymer polyaniline. However, these studies were limited to electrical measurements. X-ray diffraction studies have suggested that aromatic amino acids tyrosine and phenylalanine are closely packed in pili. But these studies used homology modeling to predict the pilus assembly and information about the number of monomers in each pilus assembly unit and their organization are still lacking. The central hypothesis of this proposal is aromatics in pili enable intermolecular electron delocalization due to pi-stacking that can give rise to metallic-like conductivity. By analyzing pili structure using infrared scattering-scanning near field optical microscope (IR s-SNOM) and combining with solution NMR, Focused Ion Beam (FIB and computational capabilities, this work will provide comprehensive understanding of the conduction mechanism from a structure-function perspective. The specific aims are: 1) With infrared scattering scanning near field optical microscope (IR s-SNOM), image the organization and density of pilin monomers and pH-induced conformational changes in a pilus filament. 2) With solution NMR, resolve pH-induced structural changes in the pilin monomer. 3) Using Focused Ion Beam (FIB), draw electrodes on single pili to measure their conductivity. 4) With computational modeling using the NWChem, simulate the effect of environment on the electronic properties of pili as a function of pH. The proposed work will gain the nanoscale insight into the structure of the pili, as the basis for understanding interspecies electrical communications. The improved understanding will be harnessed to accelerate bioenergy production and bioremediation using pili as well as for predictive modeling of carbon cycling in diverse environments to reach the central goals of DOE-BER to develop sustainable energy sources, regulate the contaminants in the subsurface and understand the effects of greenhouse gas emissions on biosphere. The proposed studies will provide design principles for engineering of electrical interactions among these communities by manipulating the amino acid composition of pili. Moreover, these studies will identify the forces that maintain the function of these communities in the face of environmental perturbation. Therefore, these studies will help to address the need "to incorporate process understanding of biogeochemical cycling into a scalable hierarchy of predictive capabilities" specified in EMSL's Science Themes.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Single Entity Electrochemistry in Nanopore Electrode Arrays: Ion Transport Meets Electron Transfer in Confined Geometries

Electrochemical measurements conducted in confined volumes provide a powerful and direct means to address scientific questions at the nexus of nanoscience, biotechnology, and chemical analysis. How are electron transfer and ion transport coupled in confined volumes and how does understanding them require moving beyond macroscopic theories? Also, how do these coupled processes impact electrochemical detection and processing? We address these questions by studying a special type of confined-volume architecture, the nanopore electrode array, or NEA, which is designed to be commensurate in size with physical scaling lengths, such as the Debye length, a concordance that offers performance characteristics not available in larger scale structures. The experiments described here depend critically on carefully constructed nanoscale architectures that can usefully control molecular transport and electrochemical reactivity. We begin by considering the experimental constraints that guide the design and fabrication of zero-dimensional nanopore arrays with multiple embedded electrodes. These zero-dimensional structures are nearly ideal for exploring how permselectivity and unscreened ion migration can be combined to amplify signals and improve selectivity by enabling highly efficient redox cycling. Our studies also highlight the benefits of arrays, in that molecules escaping from a single nanopore are efficiently captured by neighboring pores and returned to the population of active redox species being measured, benefits that arise from coupling ion accumulation and migration. These tools for manipulating redox species are well-positioned to explore single molecule and single particle electron transfer events through spectroelectrochemistry, studies which are enabled by the electrochemical zero-mode waveguide (ZMW), a special hybrid nanophotonic/nanoelectronic architecture in which the lower ring electrode of an NEA nanopore functions both as a working electrode to initiate electron transfer reactions and as the optical cladding layer of a ZMW. Furthermore, while the work described here is largely exploratory and fundamental, we believe that the development of NEAs will enable important applications that emerge directly from the unique coupled transport and electron-transfer capabilities of NEAs, including in situ molecular separation and detection with external stimuli, redox-based electrochemical rectification in individually encapsulated nanopores, and coupled sorters and analyzers for nanoparticles.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗