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DOE OSTI2023

Evidence of Zintl Intermediate Phase and Its Impacts on Li and Na Storage Performance of Pb-Based Alloying Anodes

Anode materials based on conversion and alloying reactions are promising to achieve high energy density of advanced sodium-ion batteries (SIBs). While the chemical similarities between sodium and lithium as alkali elements make the benchmarking strategy practical in developing new high-performance anodes, simply borrowing the anode material from one system to the other does not always guarantee success unless it is based on sound understanding of both Li- and Na-reaction mechanisms. In this work, we report the Na storage performance of a Pb-based anode and its fundamental reaction dynamics. In contrast to its excellent electrochemical performances in Li cells (reversible ~600 mAh/g), the newly developed Pb@PbO–C nanocomposite anode has limited electrochemical Na reaction properties showing moderate capacity and rate performances (~300 mAh/g at 20 mA/g). Synchrotron-based X-ray diffraction and absorption spectroscopy studies reveal the fundamental differences in the Na and Li reaction mechanism of the Pb-based anode. Further, unlike Li reaction, the unique Na reaction mechanism involves the formation of a highly ionic NaPb Zintl phase, which comprises tetrahedral Pb 4 clusters, as an intermediate phase. The strong covalent character of the Pb 4 Zintl clusters adversely affects the electronic conductivity and thus limits the electrochemical performance of the Pb-based anode in Na cells. These findings provide new insights applicable to developing high-performance alloying anode materials.

25 ENERGY STORAGE↗

DOE OSTI2021

Stress-Dependent Chemo-Mechanical Performance of Amorphous Si Anodes for Li-Ion Batteries upon Lithiation

Alloying-type anodes are significantly governed by their chemo-mechanical performance during the electrochemical cycling. The reaction-induced huge volumetric change of these anodes may cause material degradation and failure under mechanical constraints. Here, we investigate the stress-dependent lithiation behavior of amorphous Si (a-Si) anodes using molecular dynamics simulations. It is indicated that a-Si anodes can sustain higher hydrostatic stress than biaxial/uniaxial ones without the occurrence of mechanical failure. Thermodynamic and electrochemical calculations demonstrate that although the lithiation procedure also affects the thermodynamic stability of a-Si anodes, it is mainly dominated by the external mean stresses. Compressive stress is confirmed to destabilize a-Si anodes and further trigger their capacity fading. Compared with our atomistic simulations, previous continuum models underestimate the open-cell potentials of a-Si anodes, due to their ignored large volumetric deformation at higher stresses and Li concentrations. Finally, this computational study provides the intensive atomic-level understanding of the stress-dependent lithiation behavior of a-Si anodes.

25 ENERGY STORAGE↗

DOE OSTI2025

The Solid Electrolyte Interphase Dispersion Can Predict Cycle and Calendar Lifetimes in Silicon Anodes for Lithium-Ion Batteries

The solid electrolyte interphase (SEI) plays a critical role in lithium-ion battery (LIB) anodes. It is responsible for passivating the reactive surface of lithiated anodes against degradation of the electrolyte which enables long cycle and calendar lifetimes for LIBs. This role is especially important in high energy density anodes like silicon, that undergo massive volumetric changes during electrochemical cycling. The mechanism by which the SEI performs this role, however, is not clear which makes designing an SEI to passivate silicon anodes impossible. Through decades of research, dozens of chemical species have been identified within the SEI ranging from inorganic solids to polymeric coatings all of which simultaneously exist in a 'mosaic' composition at the anode surface. This mosaic creates a highly dispersive environment in which electrostatic screening of the anode surface from the electrolyte is not always complete. Here, we present an electrochemical technique to directly test the dispersion at the anode surface. We use this technique to screen more than 20 different electrolytes against silicon anodes and find correlations between both the cycle life and calendar life. The insights from this study offer a new framework to think about the SEI and a rapid screening method to test novel electrode/electrolyte combinations.

battery↗

DOE OSTI2021

Comparative Techno-Economic and Life Cycle Analysis of Water Oxidation and Hydrogen Oxidation at the Anode in a CO 2 Electrolysis to Ethylene System

We compare the economic viability of employing hydrogen oxidation versus water oxidation at the anode of a commercial-scale electrolysis plant that converts CO 2 to ethylene. We vary the electrolyzer capital cost, membrane lifetime, and renewable electricity price to represent a current and future market scenario. We find that anodic hydrogen oxidation with membraneless reactor design can reduce the electrolyzer capital cost by up to 48% and reduce electricity demand by at least 50% with the current underdeveloped electrolyzer market. These capital and operating cost savings could further lead to a lower ethylene production cost from anodic hydrogen oxidation than the anodic water oxidation system with hydrogen supplied at less than $\$6$ kg. In the future scenario with a fully developed electrolyzer market and cheap renewable electricity, we find that the anodic hydrogen oxidation system requires hydrogen cheaper than $0.7/kg to compete with the anodic water oxidation system. Moreover, hydrogen oxidation at the anode enables extremely low cradle-to-gate emission ethylene by utilizing negative emission hydrogen such as biomass gasification with carbon capture and sequestration, ~240% lower than ethylene produced from the wind/solar electricity-driven water oxidation system. Furthermore, this low carbon footprint ethylene can further boost the economic competitiveness for anodic hydrogen oxidation with a future carbon credit market.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1974

Anode power in a quasi-steady MPD thruster

Local anode heat flux in a quasi-steady MPD thruster is measured by thermocouples attached to the inside surface of a shell anode. Over a range of arc currents J from 5.5 to 44 kiloamperes and argon propellant mass flows m from 1 to 48 g/sec, with the ratio J2/m held constant, the fraction of arc power deposited in the anode is found to decrease with increasing arc power. Specifically, this anode power fraction decreases from 50% at 200 kW arc power, to 10% at 20 MW. In an effort to account for this functional behavior, the current density, plasma potential, and electron temperature in the plasma adjacent to the anode are measured with probes, and the results are used in a theoretical anode heat flux model. The model asserts that energy exchange between electrons and heavy particles in the plasma near the anode occur over distances greater than the anode sheath thickness.

Saber, A. J.↗

NASA NTRS1984

Thermal investigation of an electrical high-current arc with porous gas-cooled anode

The following guantities were measured on a high-intensity electric arc with tungsten cathode and transpiration-cooled graphite anode burning in argon: electric current and voltage, cooling gas flow rate (argon), surface temperature of the anode and of the anode holder, and temperature profile in three cross-sections of the arc are column. The last mentioned values were obtained from spectroscopic photographs. From the measured quantities, the following values were calculated: the heat flux into the anode surface, the heat loss of the anode by radiation and conduction, and the heat which was regeneratively transported by the cooling gas back into the arc space. Heat balances for the anode were also obtained. The anode losses (which are approximately 80% of the total arc power for free burning arcs) were reduced by transpiration cooling to 20%. The physical processes of the energy transfer from the arc to the anode are discussed qualitatively.

Eckert, E. R. G.↗

NASA NTRS1989

Development and testing of a prototype mosaic wedge-and-strip anode detector

A preliminary laboratory study of a prototype mosaic wedge-and-strip anode, a new class of readout system that will furnish large format, high resolution microchannel plate detectors with comparatively simple readout electronics is described. The goals of this study were to demonstrate the linearity of the mosaic anode algorithm, and to verify the predicted resolution performance in a realistic detector configuration. It is found that the nonlinearity introduced at the boundary between two anodes is limited to 50-100 microns. It is also shown that the spatial resolution of the detector is limited mainly by partition noise to about 35 microns (FWHM) at a gain of 2 x 10 to the 7th. A systematic investigation of the charge distribution arriving at the anode is also described. Using the relative charges arriving on the two anodes of the mosaic pattern, the detailed shape of the distribution and its dependence on MCP-anode voltage, MCP voltage, and pulse height are determined. A significant dependence of the profile on pulse height, which can introduce a pulse height dependence to the centroid calculation, particularly near the anode edges is found. Improved anode designs which will achieve the optimal performance are discussed.

Rasmussen, A.↗

NASA NTRS1993

Anodized aluminum on LDEF

A compilation of reported analyses and results obtained for anodized aluminum flown on the Long Duration Exposure Facility (LDEF) was prepared. Chromic acid, sulfuric acid, and dyed sulfuric acid anodized surfaces were exposed to the space environment. The vast majority of the anodized surface on LDEF was chromic acid anodize because of its selection as a thermal control coating for use on the spacecraft primary structure, trays, tray clamps, and space end thermal covers. Reports indicate that the chromic acid anodize was stable in solar absorptance and thermal emittance, but that contamination effects caused increases in absorptance on surfaces exposed to low atomic oxygen fluences. There were some discrepancies, however, in that some chromic acid anodized specimens exhibited significant increases in absorptance. Sulfuric acid anodized surfaces also appeared stable, although very little surface area was available for evaluation. One type of dyed sulfuric acid anodize was assessed as an optical baffle coating and was observed to have improved infrared absorptance characteristics with exposure on LDEF.

Golden, Johnny L.↗

NASA NTRS1995

Circuit for high resolution decoding of multi-anode microchannel array detectors

A circuit for high resolution decoding of multi-anode microchannel array detectors consisting of input registers accepting transient inputs from the anode array; anode encoding logic circuits connected to the input registers; midpoint pipeline registers connected to the anode encoding logic circuits; and pixel decoding logic circuits connected to the midpoint pipeline registers is described. A high resolution algorithm circuit operates in parallel with the pixel decoding logic circuit and computes a high resolution least significant bit to enhance the multianode microchannel array detector's spatial resolution by halving the pixel size and doubling the number of pixels in each axis of the anode array. A multiplexer is connected to the pixel decoding logic circuit and allows a user selectable pixel address output according to the actual multi-anode microchannel array detector anode array size. An output register concatenates the high resolution least significant bit onto the standard ten bit pixel address location to provide an eleven bit pixel address, and also stores the full eleven bit pixel address. A timing and control state machine is connected to the input registers, the anode encoding logic circuits, and the output register for managing the overall operation of the circuit.

Kasle, David B.↗

NASA NTRS1999

High-absorptance high-emittance anodic coating

A colored anodic coating for use on surfaces of substrates, e.g. aluminum substrates in which it is desirable to maintain a high solar absorptance (.alpha.) and a high infrared emittance (.epsilon.), particularly in low earth orbit space environments. This anodic coating is preferably a dark colored coating, and even more preferably a black coating. This coating allows a touch temperature within an acceptable design range to preclude burning of an astronaut in case of contact, but also allows a solar radiation absorption in an amount such that an .alpha./.epsilon. ratio of unity is achieved. The coating of the invention comprises a first layer in the form of an acid anodized colored anodic layer for achieving a high solar absorptance and a second or high emittance layer in the form of a clear acid anodized layer for achieving a high emittance. The entire coating is quite thin, e.g. 1-2 mils and is quite stable in a hostile space environment of the type encountered in a low earth orbit. The coating is obtained by first creating the high emittance clear anodized coating on the metal surface followed by anodizing using a colored anodizing process.

Le, Huong Giang↗

NASA NTRS1998

High-absorptance high-emittance anodic coating

A colored anodic coating for use on surfaces of substrates, e.g. aluminum substrates in which it is desirable to maintain a high solar absorptance (a) and a high infrared emittance (e), particularly in low earth orbit space environments. This anodic coating is preferably a dark colored coating, and even more preferably a black coating. This coating allows a touch temperature within an acceptable design range to preclude burning of an astronaut in case of contact, but also allows a solar radiation absorption in an amount such that an a/e ratio of unity is achieved. The coating of the invention comprises a first layer in the form of an acid anodized colored anodic layer for achieving a high solar absorptance and a second or high emittance layer in the form of a clear acid anodized layer for achieving a high emittance. The entire coating is quite thin, e.g. 1-2 mils and is quite stable in a hostile space environment of the type encountered in a low earth orbit. The coating is obtained by first creating the high emittance clear anodized coating on the metal surface followed by anodizing using a colored anodizing process.

Le, Huong Giang↗

NASA NTRS2006

Electrically Conductive Anodized Aluminum Surfaces

Anodized aluminum components can be treated to make them sufficiently electrically conductive to suppress discharges of static electricity. The treatment was conceived as a means of preventing static electric discharges on exterior satin-anodized aluminum (SAA) surfaces of spacecraft without adversely affecting the thermal-control/optical properties of the SAA and without need to apply electrically conductive paints, which eventually peel off in the harsh environment of outer space. The treatment can also be used to impart electrical conductivity to anodized housings of computers, medical electronic instruments, telephoneexchange equipment, and other terrestrial electronic equipment vulnerable to electrostatic discharge. The electrical resistivity of a typical anodized aluminum surface layer lies between 10(exp 11) and 10(exp 13) Omega-cm. To suppress electrostatic discharge, it is necessary to reduce the electrical resistivity significantly - preferably to < or = 10(exp 9) Omega-cm. The present treatment does this. The treatment is a direct electrodeposition process in which the outer anodized surface becomes covered and the pores in the surface filled with a transparent, electrically conductive metal oxide nanocomposite. Filling the pores with the nanocomposite reduces the transverse electrical resistivity and, in the original intended outer-space application, the exterior covering portion of the nanocomposite would afford the requisite electrical contact with the outer-space plasma. The electrical resistivity of the nanocomposite can be tailored to a value between 10(exp 7) and 10(exp 12) Omega-cm. Unlike electrically conductive paint, the nanocomposite becomes an integral part of the anodized aluminum substrate, without need for adhesive bonding material and without risk of subsequent peeling. The electrodeposition process is compatible with commercial anodizing production lines. At present, the electronics industry uses expensive, exotic, electrostaticdischarge- suppressing finishes: examples include silver impregnated anodized, black electroless nickel, black chrome, and black copper. In comparison with these competing finishes, the present nanocomposite finishes are expected to cost 50 to 20 percent less and to last longer.

Nguyen, Trung Hung↗

NASA NTRS2005

Improved Anode for a Direct Methanol Fuel Cell

A modified chemical composition has been devised to improve the performance of the anode of a direct methanol fuel cell. The main feature of the modified composition is the incorporation of hydrous ruthenium oxide into the anode structure. This modification can reduce the internal electrical resistance of the cell and increase the degree of utilization of the anode catalyst. As a result, a higher anode current density can be sustained with a smaller amount of anode catalyst. These improvements can translate into a smaller fuel-cell system and higher efficiency of conversion. Some background information is helpful for understanding the benefit afforded by the addition of hydrous ruthenium oxide. The anode of a direct methanol fuel cell sustains the electro-oxidation of methanol to carbon dioxide in the reaction CH3OH + H2O--->CO2 + 6H(+) + 6e(-). An electrocatalyst is needed to enable this reaction to occur. The catalyst that offers the highest activity is an alloy of approximately equal numbers of atoms of the noble metals platinum and ruthenium. The anode is made of a composite material that includes high-surface-area Pt/Ru alloy particles and a proton-conducting ionomeric material. This composite is usually deposited onto a polymer-electrolyte (proton-conducting) membrane and onto an anode gas-diffusion/current-collector sheet that is subsequently bonded to the proton-conducting membrane by hot pressing. Heretofore, the areal density of noble-metal catalyst typically needed for high performance has been about 8 mg/cm2. However, not all of the catalyst has been utilized in the catalyzed electro-oxidation reaction. Increasing the degree of utilization of the catalyst would make it possible to improve the performance of the cell for a given catalyst loading and/or reduce the catalyst loading (thereby reducing the cost of the cell). The use of carbon and possibly other electronic conductors in the catalyst layer has been proposed for increasing the utilization of the catalyst by increasing electrical connectivity between catalyst particles. However, the relatively low density of carbon results in thick catalyst layers that impede the mass transport of methanol to the catalytic sites. Also, the electrical conductivity of carbon is less than 1/300th of typical metals. Furthermore, the polymer-electrolyte membrane material is acidic and most metals are not chemically stable in contact with it. Finally, a material that conducts electrons (but not protons) does not contribute to the needed transport of protons produced in the electro-oxidation reaction.

Valdez, Thomas↗

NASA NTRS2012

Fundamental Investigation of Silicon Anode in Lithium-Ion Cells

Silicon is a promising and attractive anode material to replace graphite for high capacity lithium ion cells since its theoretical capacity is ~10 times of graphite and it is an abundant element on Earth. However, there are challenges associated with using silicon as Li-ion anode due to the significant first cycle irreversible capacity loss and subsequent rapid capacity fade during cycling. Understanding solid electrolyte interphase (SEI) formation along with the lithium ion insertion/de-insertion kinetics in silicon anodes will provide greater insight into overcoming these issues, thereby lead to better cycle performance. In this paper, cyclic voltammetry and electrochemical impedance spectroscopy are used to build a fundamental understanding of silicon anodes. The results show that it is difficult to form the SEI film on the surface of a Si anode during the first cycle; the lithium ion insertion and de-insertion kinetics for Si are sluggish, and the cell internal resistance changes with the state of lithiation after electrochemical cycling. These results are compared with those for extensively studied graphite anodes. The understanding gained from this study will help to design better Si anodes, and the combination of cyclic voltammetry with impedance spectroscopy provides a useful tool to evaluate the effectiveness of the design modifications on the Si anode performance.

Wu, James J.↗

DOE OSTI2026

A Holistic Stabilization of the Anode in Lithium‐Sulfur Batteries Through a Ternary Alloy Fusion

The anode in lithium–sulfur batteries (LSBs) is plagued by not only inhomogeneous lithium (Li) deposition, but also by parasitic side-reactions. Often, a thick anode (∼400 µm) is used to compensate for these drawbacks, lowering gravimetric and volumetric energy densities. In this work, we demonstrate a ternary alloy anode fabricated via scalable thermal fusion of Li with aluminum (Al) and tellurium (Te) to cohesively address these issues. The Al–Li skeleton serves to homogenize Li deposition as well as reinforce the anode, allowing it to be rolled down to low thicknesses. Te incorporation suppresses the reaction of Li with polysulfides (Li 2 Sn) to form lithium sulfide (Li 2 S) and electrolyte degradation. It can also facilitate the formation of polytellurosulfides (Li 2 Te x Sy), which are far more conducive to Li + -ion diffusion. Even under a lean electrolyte/sulfur (E/S) ratio of 8 µL mg −1 and a low negative/positive (N/P) ratio of 3, capacities over 900 mA h g −1 at a C/5 rate are obtained in cells with Li–Te–Al anodes with a capacity retention of 80% after 70 cycles. In comparison, the baseline lithium-metal anode retains only 35% after 50 cycles. Furthermore, the Li–Te–Al anodes confer a 24% boost to gravimetric energy density at the pouch cell level.

25 ENERGY STORAGE↗

DOE OSTI2022

Highly Reversible Sodium Metal Battery Anodes via Alloying Heterointerfaces

As a promising pathway toward low-cost, long-duration energy storage, rechargeable sodium batteries are of increasing interest. Batteries that incorporate metallic sodium as anode promise a high theoretical specific capacity of 1166 mAh g –1 , and low reduction potential of –2.71 V. The high reactivity and poor electrochemical reversibility of sodium anodes render sodium metal anode (SMA) cells among the most challenging for practical implementation. Here, the failure mechanisms of Na anodes are investigated and the authors report that loss of morphological control is not the fundamental cause of failure. Rather, it is the inherently poor anchoring/root structure of electrodeposited Na to the electrode substrate that leads to poor reversibility and cell failure. Poorly anchored Na deposits are prone to break away from the current collector, producing orphaning and poor anode utilization. Thin metallic coatings in a range of chemistries are proposed and evaluated as SMA substrates. Based on thermodynamic and ion transport considerations, such substrates undergo reversible alloying reactions with Na and are hypothesized to promote good root growth—regardless of the morphology. Among the various options, Au stands out for its ability to support long Na anode lifetime and high reversibility (Coulombic Efficiency > 98%), for coating thicknesses in the range of 10–1000 nm. Finally, as a first step toward evaluating practical utility of the anodes, their performance in Na||SPAN cells with N:P ratio close to 1:1 is evaluated.

25 ENERGY STORAGE↗

DOE OSTI2023

High performance aluminum-air flow batteries through double-face architecture and laser-modified and friction-stir processed 3D anode

Aluminum-air batteries (AAB) are regarded as one of the most promising beyond-lithium high-energy-density storage candidates. Here, this paper introduces a three-dimensional (3D) Al 7075 anode enabled by femtosecond laser and friction-stir process which, along with a special double-face anode architecture provides world-class performance. Electrochemical characterizations prove that the corrosion resistance of the modified 3D Al 7075 FSP anode was enhanced, and electrochemically active surface area (ECSA) was increased compared with that of normal Al 7075 anode. Friction-stir processing reduced the mean grain size from 30 μm to 3 μm. The discharge performance of 3D Al 7075 FSP anode is shown to be quite stable, and the average values of energy density are significantly increased from 2256 mWh g –1 to 2941 mWh g –1 at 100 mA cm –2 . In a double-face flowing Al-air battery system, the 3D Al 7075 FSP anode exhibited significantly better electrocatalytic performance (discharge voltage of 0.76 V at 400 mA cm –2 , and power density of 337.8 mW cm –2 ) than that of a commercial Al 7075 anode.

25 ENERGY STORAGE↗

DOE OSTI2024

Coal-derived carbon anodes for lithium-ion batteries: Development, challenges, and prospects

Lithium-ion battery (LIB) development has increased rapidly, requiring low-cost anode materials with a high capacity, high-rate performance, and stable lifespan. Carbon-based anodes possess various exceptional morphologies and structures, making them promising candidates for meeting the technical demands; however, conventional synthetic carbon anode processes need expensive feedstocks that increase anode cost and limit commercialization. Coal, the most affordable and abundant carbon resource, has attracted increasing attention as the primary feedstock for producing high-value carbon anode materials. This article reviews the lithium storage mechanisms, characteristics, and productions of some high-valuable carbon anode materials for LIBs from coal and coal derivatives. The high-value carbon anode materials reviewed in this article are graphite, graphene, mesophase microbeads (MCMB), carbon fiber, and hard carbons. Furthermore, the remaining challenges and prospects of using coal-derived carbon materials to create high-performance and low-cost lithium-ion batteries are also discussed.

25 ENERGY STORAGE↗