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All sources NASA NTRS DOE OSTI

DOE OSTI2015

Self-induced redox cycling coupled luminescence on nanopore recessed disk-multiscale bipolar electrodes

Self-induced redox cycling at nanopore ring-disk electrodes is coupled, through a bipolar electrode, to a remote fluorigenic reporter reaction. We present a new configuration for coupling fluorescence microscopy and voltammetry using self-induced redox cycling for ultrasensitive electrochemical measurements. An array of nanopores, each supporting a recessed disk electrode separated by 100 nm in depth from a planar multiscale bipolar top electrode, was fabricated using multilayer deposition, nanosphere lithography, and reactive-ion etching. Self-induced redox cycling was induced on the disk electrode producing ~30× current amplification, which was independently confirmed by measuring induced electrogenerated chemiluminescence from Ru(bpy) 3 2/3+ /tri-n-propylamine on the floating bipolar electrode. In this design, redox cycling occurs between the recessed disk and the top planar portion of a macroscopic thin film bipolar electrode in each nanopore. Electron transfer also occurs on a remote (mm-distance) portion of the planar bipolar electrode to maintain electroneutrality. This couples the electrochemical reactions of the target redox pair in the nanopore array with a reporter, such as a potential-switchable fluorescent indicator, in the cell at the distal end of the bipolar electrode. Oxidation or reduction of reversible analytes on the disk electrodes were accompanied by reduction or oxidation, respectively, on the nanopore portion of the bipolar electrode and then monitored by the accompanying oxidation of dihydroresorufin or reduction of resorufin at the remote end of the bipolar electrode, respectively. In both cases, changes in fluorescence intensity were triggered by the reaction of the target couple on the disk electrode, while recovery was largely governed by diffusion of the fluorescent indicator. Reduction of 1 nM of Ru(NH 3 ) 6 3+ on the nanoelectrode array was detected by monitoring the fluorescence intensity of resorufin, demonstrating high sensitivity fluorescence-mediated electrochemical sensing coupled to self-induced redox cycling.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2021

Surface processing and discharge-conditioning of high voltage electrodes for the Ra EDM experiment

The Ra EDM experiment uses a pair of high voltage electrodes to search for the atomic electric dipole moment of 225 Ra. We use identical, plane–parallel electrodes with a primary high gradient surface of 200 mm 2 to generate reversible DC electric fields. Our statistical sensitivity is linearly proportional to the electric field strength in the electrode gap. We adapted surface decontamination and processing techniques from accelerator physics literature to chemical polish and clean a suite of newly fabricated large-grain niobium and grade-2 titanium electrodes. Three pairs of niobium electrodes and one pair of titanium electrodes were discharge-conditioned with a custom high voltage test station at electric field strengths as high as +52.5 kV/mm and –51.5 kV/mm over electrode gap sizes ranging from 0.4 mm to 2.5 mm. One pair of large-grain niobium electrodes was discharge-conditioned and validated to operate at ±20 kV/mm with steady-state leakage current ≤ 25 pA (1σ) and a polarity-averaged 98 ± 19 discharges per hour. These electrodes were installed in the Ra EDM experimental apparatus, replacing a copper electrode pair, and were revalidated to ±20 kV/mm. Here, the niobium electrodes perform at an electric field strength 3.1 times larger than the legacy copper electrodes and are ultimately limited by the maximum output of our 30 kV bipolar power supply.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Structure, dynamics, and electrochemistry of choline chloride/ethylene glycol eutectic solvents at an electrode surface explored by molecular dynamics simulations

Choline chloride and ethylene glycol mixtures with 1:2, 1:4, and 1:6 molar ratios on the surfaces of graphite and gold electrodes were studied using classical molecular dynamics simulations. Both neutral and charged electrodes were considered. The liquid composition, solvation structure, molecular orientation, and dynamics at the electrode surface are significantly different from those of the bulk liquid. These properties strongly depend on the electrode material and charge density, whereas they are less sensitive to the overall solvent composition. The effect of the electrode on the composition, structure, and orientation of the liquid fades beyond ∼10 Å from the surface of the electrode. This distance corresponds to about two layers of the structured solvent, despite the fact that the layered structure extends to at least five layers or about 25 Å. However, the electrode influences solvent dynamics over a longer distance. The electrochemical properties of the eutectic solvent at both electrode surfaces were also studied. The simulations captured the experimental differential capacitance shapes for both electrode systems, although the magnitudes and exact shapes differ. The simulations further revealed that the solvent in the first solvation layer can both overscreen and underscreen the electrode charges depending on the electrode material and electrode potential.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Structural Changes during the Conversion Reaction of Tungsten Oxide Electrodes with Tailored, Mesoscale Porosity

In-plane tungsten oxide nanostructures, including hexagonally patterned cylinders and holes in a matrix, were fabricated via sequential infiltration synthesis (SIS) on self-assembled block copolymer templates. Using the tailored morphology and porosity of these model electrodes with in situ grazing incidence small angle X-ray scattering, the intrinsic structural change of nanoscale active materials during the conversion reaction of WO 3 + 6Li ↔ W + 3 Li 2 O was investigated at controlled electrochemical conditions. Reversible electrode volume expansion and contraction was observed during lithiation and delithiation cycles, respectively. The potential where electrode’s thickness expansion started was ~1.6 V, which is close to thermodynamically expected one for conversion reaction of WO 3 with lithium (1.65 V). The temporal evolution of the electrode volume at constant electrode potentials revealed high overpotential for bulk lithiation and slow conversion reaction kinetics, despite the tailored porosity of the SIS electrodes. Oxide cylinders showed smaller overall electrode thickness change, likely due to unconstrained lateral volume change, as compared to a matrix with holes. On the other hand, better connectivity and guided volume change of the latter electrode morphology provided improved cycling stability. Additionally, heterogeneity in an electrode, from internal pores and density gradients, was found to aggravate the fragmentation of the electrode during conversion reaction. Insights into oxide conversion reaction kinetics and the relationship between electrode mesostructure and cycling behavior obtained from this study can help guide the more rational design of conversion electrode for high performing batteries.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Elucidating the assembly of Nanoparticle Organic Hybrid Materials (NOHMs) near an electrode interface with varying potential using Neutron Reflectivity

A critical concern regarding electrolyte formulation in an electrochemical environment is the impact of the interaction of the multiple components (i.e., supporting electrolyte or additive) with the electrode surface. Recently, liquid-like neat Nanoparticle Organic Hybrid Materials (NOHMs) have been considered as an electrolyte component to improve the transport of redox-active species to the electrode surface. However, the structure and assembly of the NOHMs near the electrode surface is unknown and could significantly impact the electrode-electrolyte interface. Hence, we have investigated the depth profile of polyetheramine (HPE) polymer and NOHM-I-HPE (nanoparticles with ionically bonded HPE polymer) in deuterated water (D2O) in the presence of two different salts (KHCO3 and ZnCl2) near two different electrode surfaces using neutron reflectometry. Moreover, the depth profile of the NOHM-I-HPE near the electrode surface in a potential has also been studied with in-situ reflectivity experiments. Our results indicate that a change in the chemical structure/hydrophilicity of the electrode surface does not significantly impact the ordering of HPE polymer or NOHM-I-HPE near the surface. Here, this study also indicates that the NOHM-I-HPE particles form a clear layer near the electrode surface immediately above an adsorbed layer of free polymer on the electrode surface. The addition of salt does not impact the layering of NOHM-I-HPE, though it does alter the conformation of the polymer grafted to the nanoparticle surface and free polymer sequestered near the surface. Finally, the application of negative potential results in an increased amount of free polymer near the electrode surface. Correlating the depth profile of free polymer and NOHM-I-HPE particles with the electrochemical performance indicates that this assembly of free polymer near the electrode surface in NOHM-I-HPE solutions contributes to the higher current density of the system. Therefore, this holistic study offers insight into the importance of the assembly of NOHM-I-HPE electrolyte and free polymer near the electrode surface in an electrochemical milieu on its performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2016

Cycling behavior of NCM523/graphite lithium-ion cells in the 3–4.4 V range: Diagnostic studies of full cells and harvested electrodes

Energy density of full cells containing layered-oxide positive electrodes can be increased by raising the upper cutoff voltage above the current 4.2 V limit. In this article we examine aging behavior of cells, containing LiNi 0.5 Co 0.2 Mn 0.3 O 2 (NCM523)-based positive and graphite-based negative electrodes, which underwent up to ~400 cycles in the 3-4.4 V range. Electrochemistry results from electrodes harvested from the cycled cells were obtained to identify causes of cell performance loss; these results were complemented with data from X-ray photoelectron spectroscopy (XPS) and secondary ion mass spectroscopy (SIMS) measurements. Our experiments indicate that the full cell capacity fade increases linearly with cycle number and results from irreversible lithium loss in the negative electrode solid electrolyte interphase (SEI) layer. The accompanying electrode potential shift reduces utilization of active material in both electrodes and causes the positive electrode to cycle at higher states-of-charge. Here, full cell impedance rise on aging arises primarily at the positive electrode and results mainly from changes at the electrode-electrolyte interface; the small growth in negative electrode impedance reflects changes in the SEI layer. Our results indicate that cell performance loss could be mitigated by modifying the electrode-electrolyte interfaces through use of appropriate electrode coatings and/or electrolyte additives.

30 DIRECT ENERGY CONVERSION↗

DOE OSTI2020

Co-Extrusion (CoEx) for Cost Reduction of Advanced High-Energy-and-Power Battery Electrode Manufacturing

Co-Extrusion (CoEx) is a deposition technology developed at PARC that uses engineered fluidic channels to cause multiple streams of dissimilar fluids to impart shape to one another. Here, we describe the use of CoEx to produce structured cathode electrode films to improve electrochemical performance of thick electrode films. CoEx enables us to create structured electrode films that have periodic regions of enhanced ionic conductivity, enabling higher utilization of thicker cathode films at high discharge rates. While increasing electrode thickness is a known method for increasing energy density of battery electrodes, this increase in energy density typically also results in reduced power density. This project, a collaboration between the Palo Alto Research Center, Oak Ridge National Laboratories, and Ford Motor Company, seeks to first validate the benefits of CoEx at the coin cell level, before performing the necessary R&D effort to scale production up to large (10+ Ah) pouch cells that will show increased energy density without a reduction in power density. We used conventional battery materials (commercially available NMC, PVDF, carbon black, and graphite) to produce structured electrodes via CoEx and compared them to thick and thin conventionally produced (unstructured) battery electrodes. CoEx electrodes show improved high rate performance compared to unstructured electrodes, resulting in higher energy density pouch cells compared to the baseline electrode of 7 and 11% in volumetric and gravimetric energy density, respectively. These electrodes also showed substantially improved electrochemical performance at high discharge rates compared to thick conventional electrodes.

25 ENERGY STORAGE↗

DOE OSTI2021

Assessment of Electrode Contamination Mitigation at 0.5 MA Scale

The Z Machine at Sandia National Laboratories uses current pulses with peaks up to 27 MA to drive target implosions and generate high energy density conditions of interest for stockpile stewardship programs pertinent to the NNSA program portfolio . Physical processes in the region near the Z Machine target create electrode plasmas which seed parasitic current loss that reduce the performance and output of a Z experiment. Electrode surface contaminants (hydrogen, water, hydrocarbons) are thought to be the primary constituent of electrode plasmas which contribute to loss mechanisms. The Sandia team explore d in situ heating and plasma discharge techniques by integrating requisite infrastructure into Sandia's Mykonos LTD accelerator, addressing potential impacts to accelerator operation, and reporting on the impact of these techniques on electrode plasma formation and shot performance. The in situ discharge cleaning utilizes the electrodes of the accelerator to excite an argon-oxygen plasma to sputter and chemically react contaminants from electrode surfaces. Insulating breaks are required to isolate the plasma in electrode regions where loss processes are most likely to occur. The shots on Mykonos validate that these breaks do not perturb experiment performance, reducing the uncertainty on the largest unknown about the in situ cleaning system. Preliminary observations with electrical and optical diagnostics suggest that electrode plasma formation is delayed, and overall inventory has been substantively reduced. In situ heating embeds cartridge heaters into accelerator electrodes and employs a thermal bakeout to rapidly desorb contaminants from electrode surfaces. For the first time, additively manufactured (AM) electrode assemblies were used on a low impedance accelerator to integrate cooling channels and manage thermal gradients. Challenges with poor supplier fabrication to specifications, load alignment, thermal expansion and hardware movement and warpage appears to have introduced large variability in observed loss, though, preventing strong assertions of loss reduction via in situ heating. At this time, an in situ discharge cleaning process offers the lowest risk path to reduce electrode contaminant inventories on Z, though we recommend continuing to develop both approaches. Additional engineering and testing are required to improve the implementation of both systems. .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS2006

Neuro-Prosthetic Implants With Adjustable Electrode Arrays

Brushlike arrays of electrodes packaged with application-specific integrated circuits (ASICs) are undergoing development for use as electronic implants especially as neuro-prosthetic devices that might be implanted in brains to detect weak electrical signals generated by neurons. These implants partly resemble the ones reported in Integrated Electrode Arrays for Neuro-Prosthetic Implants (NPO-21198), NASA Tech Briefs, Vol. 27, No. 2 (February 2003), page 48. The basic idea underlying both the present and previously reported implants is that the electrodes would pick up signals from neurons and the ASICs would amplify and otherwise preprocess the signals for monitoring by external equipment. The figure presents a simplified and partly schematic view of an implant according to the present concept. Whereas the electrodes in an implant according to the previously reported concept would be microscopic wires, the electrodes according to the present concept are in the form of microscopic needles. An even more important difference would be that, unlike the previously reported concept, the present concept calls for the inclusion of microelectromechanical actuators for adjusting the depth of penetration of the electrodes into brain tissue. The prototype implant now under construction includes an array of 100 electrodes and corresponding array of electrode contact pads formed on opposite faces of a plate fabricated by techniques that are established in the art of microelectromechanical systems (MEMS). A mixed-signal ASIC under construction at the time of reporting the information for this article will include 100 analog amplifier channels (one amplifier per electrode). On one face of the mixed-signal ASIC there will be a solder-bump/micro-pad array that will have the same pitch as that of the electrode array, and that will be used to make the electrical and mechanical connections between the electrode array and the ASIC. Once the electrode array and the ASIC are soldered together, the remaining empty space between them will be filled with a biocompatible epoxy, the remaining exposed portions of the ASIC will be covered with micromachined plates for protection against corrosive bodily fluids, and then the ASIC and its covering micromachined plates will be coated with parylene

Whitacre, Jay↗

DOE OSTI2019

Capacitance of coarse-grained carbon electrodes with thickness up to 800 μm

We report that increasing the mass loading of active material in a supercapacitor electrode improves the energy storage capability per electrode area. However, the increase of mass loading is accompanied by the increased electrode thickness, which often causes drops in specific capacitance and counteracts the potential increase in areal capacitance once the electrode thickness exceeds 100 μm. In our previous work, we showed high specific capacitance retention of coarse-grained carbide derived carbon (CDC) with electrode thicknesses up to 1000 μm in organic electrolytes. In this work, we report that this behavior can be extended to coarse-grained activated carbon (AC). AC is the most common commercial supercapacitor electrode material with a much broader pore size distribution and lower electric conductivity compared to CDC. The areal capacitance of the AC electrode is enhanced from 2.3 F/cm 2 to 7.4 F/cm 2 at 5 mV/s, as the electrode thickness increases from 200 to 800 μm. With the increased mass loading of the active electrode material, the mass and volume occupied by current collectors and separators are reduced in the electrode stack, which leads to an increase of the gravimetric and volumetric energy density of the device. Finally, by reporting on this advantageous behavior in thick electrodes using coarse-grained carbons, we hope to garner interest toward an unexplored method for improving the performance of porous carbon-based supercapacitors, without increasing the cost or changing the current used supercapacitor manufacturing process.

36 MATERIALS SCIENCE↗

DOE OSTI2013

Effect of a floating electrode on a plasma jet

Two kinds of floating electrode, floating dielectric barrier covered electrode (FDBCE) and floating pin electrode (FPE), which can enhance the performance of plasma jet are reported. The intense discharge between the floating electrode and power electrode decreased the voltage to trigger the plasma jet substantially. The transition of plasma bullet from ring shape to disk shape in the high helium concentration region happened when the floating electrode was totally inside the powered ring electrode. The enhanced electric field between propagating plasma bullet and ground electrode is the reason for this transition. The double plasma bullets happened when part of the FDBCE was outside the powered ring electrode, which is attributed to the structure and surface charge of FDBCE. As part of the FPE was outside the powered ring electrode, the return stroke resulted in a single intensified plasma channel between FPE and ground electrode.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

High Throughput Solvent-free Manufacturing of Battery Electrodes

The project goal is to develop and demonstrate an advanced solvent-free lithium-ion battery electrode process through proposed Advanced Dry Electrode Process (ADEP) equipment, which is expected to exhibit a better binder fibrillization and high throughput and suitable for high performance electrode manufacturing, and commonize the anode and cathode dry processing equipment, supply chain and operation for lithium-ion battery OEMs for replacing the solvent-based slurry casting. Our proposed approach will facilitate low-cost battery production by addressing the following gaps in present dry electrode processing: • Extend the dry electrode fabrication process to lithium-ion battery anode manufacturing • Increase the active material content for anodes and cathodes • Intensify the process through improved mixing, powder rheology and surface modifications • Enable processing of next-generation electrode materials that are not stable to solvent or ambient air exposure. The project objectives include the development of anode-compatible binder and binder fibrillization promoter for low irreversible capacity loss, low electrode binder content yet higher film mechanical strength, and the optimization of solvent-free anode and cathode process for low cost (>60% electrode cost reduction), high performance (10% increase in energy density without sacrificing cycle life) and high throughput to enable next generation lithium-ion battery electrode production. Solvent-free electrode manufacturing will also enable next-generation cell designs based on prelithiated anodes or solid-state electrolytes.

25 ENERGY STORAGE↗

DOE OSTI2020

Influence of Proton Activity Gaps between Electrodes on Open-Circuit Potential of H 2 /H 2 and H 2 /Air Cells

Polymer -electrolyte-fuel-cell open-circuit voltages (OCVs) are exactly defined by equation (1), where cathode and anode proton activities [(aH+)cathode and (aH+)anode, respectively] usually are identical, so the third term in the right-hand side of equation (2) is ignored. OCV=E0+RT/2F*ln(a1/2 O2*(a2 H+)cathode/aH2O)-RT/2F*ln((a2 H+)anode/aH2) (1) =E0+RT/2F*ln(a1/2 O2*aH2/aH2O)+RT/2F*ln((a2 H+)cathode/(a2 H+)anode) (2) Water vapor pressure is a colligative property that fundamentally correlates to electrolyte concentrations in aqueous solutions. Proton activity is a function of acid concentration, such as pH, when electrolytes are acids. In polymer-electrolyte membranes, water vapor pressure and acid concentration are understood as relative humidity (RH) and water uptake (λ), respectively, where λ represents number of water molecules per sulfonic acid molecule. Several investigations have reported the relationship between RH and λ, meaning that proton activities and associated water uptakes are intimately related to RH. In actual fuel cell operation, cathode RH is determined by ambient-atmosphere and/or humidifier RH(s), and anode RH depends on hydrogen-circulator RH. Therefore, RH is not always identical at both electrodes, and the difference between electrode RHs is considerable during dry operation of polymer electrolyte fuel cells. Therefore, the third term in the right-hand side of equation (2) may be significant for dry operation. We measured OCVs when hydrogen was supplied to both electrodes at 80°C. One electrode (A) was fixed at 30% RH, while RH at the other electrode (B) was varied (0, 5, 10, 20, and 30%). Measured OCVs varied from 0 to 75 mV. For fuel cell tests, electrode A was supplied with hydrogen at 30% RH; electrode B, oxygen at 0, 5, 10, 20, and 30% RH. OCVs deviated from that measured when RH at electrode B was 30%, increasing from 0 to 60 mV with decreasing RH at electrode B. Results are also shown in Figure 1. Proton activities of both electrodes were thermodynamically calculated. The Gibbs–Duhem relation was applied to obtain molar Gibbs free energies of water and sulfonic acid, and proton activity coefficient was calculated using the Gibbs free energy of sulfonic acid and the relationship between RH and λ1–4, assuming that protons and sulfonic anions show identical ionic-activity coefficients. OCVs were estimated using the third term in the right-hand side of equation (2). Results are shown in Figure 1. Fuel-cell current–voltage performance was poor when RHs at the anode and cathode were 30 and 20%, respectively. To determine kinetic current, we measured the oxygen-reduction reaction (ORR) using a rotating-disk electrode (RDE) in concentrated-acid aqueous solutions, which modeled catalyst-layer ionomers. Kinetic currents decreased with acid concentrations. References T. A. Zawodzinski, Jr., C. Derouin, S. Radzinski, R. J. Sherman, V. T. Smith, T. E. Springer and S. Gottesfeld , J. Electrochem. Soc., 140,1041 (1993) P. K. Das and A. Z. Weber, Proceedings of the ASME 2013 11th Fuel Cell Science, Engineering and Technology Conference, Fuel Cell 18010 (2013) V. A. Sethuraman, J. W. Weidner, A. T. Haug, S. Motupally,b and L. V. Protsailo, J. Electrochem. Soc., 155, B50 (2008) A. Kusoglu and A. Z. Weber, Chem. Rev., 117, 987 (2017) Figure 1

Yoshida, Toshihiko↗

NASA NTRS1989

Impedance studies of Ni/Cd and Ni/H cells using the cell case as reference electrode

Many impedance studies were carried out on Ni electrodes and Ni/Cd and Ni/H batteries. In order for impedance to become a diagnostic tool, accurate and reproducible measurements must be made, and some way of separating the contributions of the individual electrodes must be found. Using the PAR and the Solartron impedance equipment, studies have found that consistent measurements can be made if the cells or electrodes are equilibrated at the voltage of interest. In the charged state, equilibration times required are short, on the order of a few hours or less, but the equilibration time required becomes progessively longer as the voltage is lowered. The cell case can be used as a reference electrode during impedance measurements. The voltage of the case with respect to the electrodes is unimportant provided that it does not change appreciably during the course of the measurement. Measurements were made with several uncycled Ni/Cd cells, one from a lot which was known to have faulty Cd electrodes and another from a lot which showed excellent cycle life and presumably had good Cd electrodes. The impedances of the Ni electrodes vs. the case were similar, while the impedance of the poor Cd electrodes vs. the case. A 50 AH Ni/H cell was also investigated. After subtraction of the ohmic resistances, the sums of the impedances of the individual electrodes were very close to the impedance of the total cell. This indicates that the method is valid for examining the characteristics of the individual electrodes in situ.

Reid, Margaret A.↗

NASA NTRS2012

Evaluation of Niobium as Candidate Electrode Material for DC High Voltage Photoelectron Guns

The field emission characteristics of niobium electrodes were compared to those of stainless steel electrodes using a DC high voltage field emission test apparatus. A total of eight electrodes were evaluated: two 304 stainless steel electrodes polished to mirror-like finish with diamond grit and six niobium electrodes (two single-crystal, two large-grain, and two fine-grain) that were chemically polished using a buffered-chemical acid solution. Upon the first application of high voltage, the best large-grain and single-crystal niobium electrodes performed better than the best stainless steel electrodes, exhibiting less field emission at comparable voltage and field strength. In all cases, field emission from electrodes (stainless steel and/or niobium) could be significantly reduced and sometimes completely eliminated, by introducing krypton gas into the vacuum chamber while the electrode was biased at high voltage. Of all the electrodes tested, a large-grain niobium electrode performed the best, exhibiting no measurable field emission (< 10 pA) at 225 kV with 20 mm cathode/anode gap, corresponding to a field strength of 18:7 MV/m.

BastaniNejad, M.↗

DOE OSTI2023

Z-pinch plasma confinement system having intermediate electrode and methods for use

An example method includes directing gas, via one or more first valves, from within an inner electrode to an acceleration region between the inner electrode and an outer electrode that substantially surrounds the inner electrode, directing gas, via two or more second valves, from outside the outer electrode to the acceleration region, and applying, via a power supply, a voltage between the inner electrode and the outer electrode, thereby converting at least a portion of the directed gas into a plasma saving a substantially annular cross section, the plasma flowing axially within the acceleration region toward a first end of the inner electrode and a first end of the outer electrode and, thereafter, establishing a Z-pinch plasma that flows between the first end of the outer electrode and the first end of the inner electrode. Related plasma confinement systems and methods are also disclosed herein.

Shumlak, Uri↗

DOE OSTI2024

Promoting electrochemical rates by concurrent ionic-electronic conductivity enhancement in high mass loading cathode electrode

Enhancing the fast charging capacity of thick electrodes with high mass loading is imperative in expediting the widespread adoption of electric vehicles. Nonetheless, the insufficient charge transfer kinetics of thick electrodes hinder the movement of effective electrons and ions, hence diminishing capacity at high current rates. In this work, we applied sustainable and biodegradable cellulose nanocrystals (CNCs) as electrode additives. It is the first time to simultaneously improve the electronic conductivity by optimizing the carbon dispersion and establishing electron transfer networks, as well as boosting the ionic conductivity of electrodes by shortening the ion transfer pathway. Specifically, the LiNi 0.6 Mn 0.2 Co 0.2 O 2 electrodes incorporating 1% dual functional CNCs additive exhibit improved effective electrical conductivity from 0.11 to 0.16 S/m and risen effective ionic conductivity from 0.36 to 0.62 S/m, in comparison to counterpart electrodes without CNCs. Therefore, the 1% CNC electrode with a high mass loading of 27.0 mg/cm 2 delivers a discharge capacity of 128 mAh/g at 1 C, which is superior to that of the CNC-free electrodes (95 mAh/g). In short, this study presents a novel environmentally friendly, economically viable, and dual-functional electrode additive that enhances both electronic and ionic conductivities with the aim of facilitating the widespread adoption of fast-charging high mass loading electrodes.

25 ENERGY STORAGE↗

DOE OSTI2019

Effects of polymeric binders on the cracking behavior of silicon composite electrodes during electrochemical cycling

Mechanical degradation caused by lithiation/delithiation-induced stress and large volume change is the primary cause of fast capacity fading of silicon (Si)-based electrodes. Although intensive efforts have been devoted to understanding electromechanically induced fractures of electrodes made of Si alone (e.g., Si particles, Si thin films, and Si wafers), the cracking behavior of Si/polymeric binders/carbon black composite electrodes is unclear and poorly understood. Here, we investigate, by in situ and ex situ techniques, the cracking behavior of Si composite electrodes made with different binders, including polyvinylidene fluoride (PVDF), sodium-alginate (SA), sodium-carboxymethyl cellulose (Na-CMC), and Nafion. We found that extensive cracks form during the 1st delithiation process, which periodically open and close during subsequent lithiation/delithiation cycles at the same locations in the Si composite electrodes made with SA, Na-CMC, and Nafion. In contrast, a significantly fewer number of cracks form in the Si/PVDF electrodes after electrochemical cycling. A possible mechanism is proposed to help understand the effects of binders on the cracking behavior (e.g., crack spacing and island size) of Si composite electrodes. We also suggest possible approaches, including reducing the electrode thickness, patterning electrodes, and using highly recoverable binders, to inhibit cracks and improve the mechanical integrity of Si composite electrodes.

25 ENERGY STORAGE↗