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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Organic Solvent Free Process to Fabricate High Performance Silicon/Graphite Composite Anode

Cycling stability is a key challenge for application of silicon (Si)-based composite anodes as the severe volume fluctuation of Si readily leads to fast capacity fading. The binder is a crucial component of the composite electrodes. Although only occupying a small amount of the total composite mass, the binder has major impact on the long-term electrochemical performance of Si-based anodes. In recent years, water-based binders including styrene-butadiene rubber (SBR) and carboxymethyl cellulose (CMC) have attracted wide research interest as eco-friendly and low-cost alternatives for the conventional poly(vinylidene difluoride) (PVDF) binder in Si anodes. In this study, Si-based composite anodes are fabricated by simple solid mixing of the active materials with subsequent addition of SBR and CMC binders. This approach bypasses the use of toxic and expansive organic solvents. The factors of binder, silicon, and graphite materials have been systematically investigated. It is found that the retained capacities of the anodes are more than 440 mAh/g after 400 cycles. These results indicate that organic solvent free process is a facile strategy for producing high performance silicon/graphite composite anodes.

Fang, Chen (ORCID:0000000321011991)↗
DOE OSTI2022

Hydroxyl Conducting Hydrogels Enable Low-Maintenance Commercially Sized Rechargeable Zn–MnO2 Batteries for Use in Solar Microgrids

Zinc (Zn)–manganese dioxide (MnO2) rechargeable batteries have attracted research interest because of high specific theoretical capacity as well as being environmentally friendly, intrinsically safe and low-cost. Liquid electrolytes, such as potassium hydroxide, are historically used in these batteries; however, many failure mechanisms of the Zn–MnO2 battery chemistry result from the use of liquid electrolytes, including the formation of electrochemically inert phases such as hetaerolite (ZnMn2O4) and the promotion of shape change of the Zn electrode. This manuscript reports on the fundamental and commercial results of gel electrolytes for use in rechargeable Zn–MnO2 batteries as an alternative to liquid electrolytes. The manuscript also reports on novel properties of the gelled electrolyte such as limiting the overdischarge of Zn anodes, which is a problem in liquid electrolyte, and finally its use in solar microgrid applications, which is a first in academic literature. Potentiostatic and galvanostatic tests with the optimized gel electrolyte showed higher capacity retention compared to the tests with the liquid electrolyte, suggesting that gel electrolyte helps reduce Mn3+ dissolution and zincate ion migration from the Zn anode, improving reversibility. Cycling tests for commercially sized prismatic cells showed the gel electrolyte had exceptional cycle life, showing 100% capacity retention for >700 cycles at 9.5 Ah and for >300 cycles at 19 Ah, while the 19 Ah prismatic cell with a liquid electrolyte showed discharge capacity degradation at 100th cycle. We also performed overdischarge protection tests, in which a commercialized prismatic cell with the gel electrolyte was discharged to 0 V and achieved stable discharge capacities, while the liquid electrolyte cell showed discharge capacity fade in the first few cycles. Finally, the gel electrolyte batteries were tested under IEC solar off-grid protocol. It was noted that the gelled Zn–MnO2 batteries outperformed the Pb–acid batteries. Additionally, a designed system nameplated at 2 kWh with a 12 V system with 72 prismatic cells was tested with the same protocol, and it has entered its third year of cycling. This suggests that Zn–MnO2 rechargeable batteries with the gel electrolyte will be an ideal candidate for solar microgrid systems and grid storage in general.

25 ENERGY STORAGE↗
DOE OSTI2024

Use of Hydrogel Electrolyte in Zn-MnO2 Rechargeable Batteries: Characterization of Safety, Performance, and Cu2+ Ion Diffusion

Achieving commercially acceptable Zn-MnO2 rechargeable batteries depends on the reversibility of active zinc and manganese materials, and avoiding side reactions during the second electron reaction of MnO2. Typically, liquid electrolytes such as potassium hydroxide (KOH) are used for Zn-MnO2 rechargeable batteries. However, it is known that using liquid electrolytes causes the formation of electrochemically inactive materials, such as precipitation Mn3O4 or ZnMn2O4 resulting from the uncontrollable reaction of Mn3+ dissolved species with zincate ions. In this paper, hydrogel electrolytes are tested for MnO2 electrodes undergoing two-electron cycling. Improved cell safety is achieved because the hydrogel electrolyte is non-spillable, according to standards from the US Department of Transportation (DOT). The cycling of “half cells” with advanced-formulation MnO2 cathodes paired with commercial NiOOH electrodes is tested with hydrogel and a normal electrolyte, to detect changes to the zincate crossover and reaction from anode to cathode. These half cells achieved ≥700 cycles with 99% coulombic efficiency and 63% energy efficiency at C/3 rates based on the second electron capacity of MnO2. Other cycling tests with “full cells” of Zn anodes with the same MnO2 cathodes achieved ~300 cycles until reaching 50% capacity fade, a comparable performance to cells using liquid electrolyte. Electrodes dissected after cycling showed that the liquid electrolyte allowed Cu ions to migrate more than the hydrogel electrolyte. However, measurements of the Cu diffusion coefficient showed no difference between liquid and gel electrolytes; thus, it was hypothesized that the gel electrolytes reduced the occurrence of Cu short circuits by either (a) reducing electrode physical contact to the separator or (b) reducing electro-convective electrolyte transport that may be as important as diffusive transport.

25 ENERGY STORAGE↗
DOE OSTI2024

Automated Lane Centering: An Off-the-Shelf Computer Vision Product vs. Infrastructure-Based Chip-Enabled Raised Pavement Markers

Safe autonomous vehicle (AV) operations depend on an accurate perception of the driving environment, which necessitates the use of a variety of sensors. Computational algorithms must then process all of this sensor data, which typically results in a high on-vehicle computational load. For example, existing lane markings are designed for human drivers, can fade over time, and can be contradictory in construction zones, which require specialized sensing and computational processing in an AV. But, this standard process can be avoided if the lane information is simply transmitted directly to the AV. High definition maps and road side units (RSUs) can be used for direct data transmission to the AV, but can be prohibitively expensive to establish and maintain. Additionally, to ensure robust and safe AV operations, more redundancy is beneficial. A cost-effective and passive solution is essential to address this need effectively. In this research, we propose a new infrastructure information source (IIS), chip-enabled raised pavement markers (CERPMs), which provide environmental data to the AV while also decreasing the AV compute load and the associated increase in vehicle energy use. CERPMs are installed in place of traditional ubiquitous raised pavement markers along road lane lines to transmit geospatial information along with the speed limit using long range wide area network (LoRaWAN) protocol directly to nearby vehicles. This information is then compared to the Mobileye commercial off-the-shelf traditional system that uses computer vision processing of lane markings. Our perception subsystem processes the raw data from both CEPRMs and Mobileye to generate a viable path required for a lane centering (LC) application. To evaluate the detection performance of both systems, we consider three test routes with varying conditions. Our results show that the Mobileye system failed to detect lane markings when the road curvature exceeded ±0.016 m -1 . For the steep curvature test scenario, it could only detect lane markings on both sides of the road for just 6.7% of the given test route. On the other hand, the CERPMs transmit the programmed geospatial information to the perception subsystem on the vehicle to generate a reference trajectory required for vehicle control. The CERPMs successfully generated the reference trajectory for vehicle control in all test scenarios. Moreover, the CERPMs can be detected up to 340 m from the vehicle’s position. Our overall conclusion is that CERPM technology is viable and that it has the potential to address the operational robustness and energy efficiency concerns plaguing the current generation of AVs.

33 ADVANCED PROPULSION SYSTEMS↗
DOE OSTI2020

Orbital Motion, Variability, and Masses in the T Tauri Triple System

We present results from adaptive optics imaging of the T Tauri triple system obtained at the Keck and Gemini Observatories in 2015−2019. We fit the orbital motion of T Tau Sb relative to Sa and model the astrometric motion of their center of mass relative to T Tau N. Using the distance measured by Gaia, we derived dynamical masses of M{sub Sa}=2.05±0.14 M {sub ⊙} and M {sub Sb} = 0.43 ± 0.06 M{sub ⊙}. The precision in the masses is expected to improve with continued observations that map the motion through a complete orbital period; this is particularly important as the system approaches periastron passage in 2023. Based on published properties and recent evolutionary tracks, we estimate a mass of ∼2 M {sub ⊙} for T Tau N, suggesting that T Tau N is similar in mass to T Tau Sa. Narrowband infrared photometry shows that T Tau N remained relatively constant between late 2017 and early 2019 with an average value of K = 5.54 ± 0.07 mag. Using T Tau N to calibrate relative flux measurements since 2015, we found that T Tau Sa varied dramatically between 7.0 and 8.8 mag in the K band over timescales of a few months, while T Tau Sb faded steadily from 8.5 to 11.1 mag in the K band. Over the 27 yr orbital period of the T Tau S binary, both components have shown 3–4 mag of variability in the K band, relative to T Tau N.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Periodic Eruptive Variability of the Isolated Pre-main-sequence Star V347 Aurigae

V347 Aurigae is associated with the small dark cloud L1438 and appears to be an isolated pre-main-sequence star located at distance d ≈ 200 pc. Multi-epoch, archival photometry reveals periodic brightness variations with amplitude V ≈ 2.0 mag occurring on timescales of ~160 days that have persisted for decades. Regular-cadence, optical imaging of the source with the Zwicky Transient Facility shows that a small reflection nebula illuminated by V347 Aur also fluctuates in brightness, at times fading completely. Multi-epoch, Keck/HIRES data suggests the presence of two distinct spectral components: a prominent emission-line-dominated spectrum with a heavily veiled continuum correlated with the bright photometric state, and an M-type absorption line spectrum associated with quiescence. All spectra exhibit strong Balmer and He i line emission, consistent with accretion, as well as high velocity emission arising from the forbidden transitions of [O i], [N ii], and [S ii] that are generally associated with collimated jets and disk winds. There is no evidence in existing high-dispersion spectroscopy or high-resolution imaging for binarity of V347 Aur. The repeating outburst events are possibly linked to accretion instabilities induced by an undetected companion or a structure within the circumstellar disk that periodically increases the mass accretion rate. V347 Aur is perhaps analogous to an EXor-type variable, though more regularly recurring.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Fermi and Swift Observations of GRB 190114C: Tracing the Evolution of High-energy Emission from Prompt to Afterglow

We report on the observations of gamma-ray burst (GRB) 190114C by the Fermi Gamma-ray Space Telescope and the Neil Gehrels Swift Observatory . The prompt gamma-ray emission was detected by the Fermi GRB Monitor (GBM), the Fermi Large Area Telescope (LAT), and the Swift Burst Alert Telescope (BAT) and the long-lived afterglow emission was subsequently observed by the GBM, LAT, Swift X-ray Telescope (XRT), and Swift UV Optical Telescope. The early-time observations reveal multiple emission components that evolve independently, with a delayed power-law component that exhibits significant spectral attenuation above 40 MeV in the first few seconds of the burst. This power-law component transitions to a harder spectrum that is consistent with the afterglow emission observed by the XRT at later times. This afterglow component is clearly identifiable in the GBM and BAT light curves as a slowly fading emission component on which the rest of the prompt emission is superimposed. As a result, we are able to observe the transition from internal-shock- to external-shock-dominated emission. We find that the temporal and spectral evolution of the broadband afterglow emission can be well modeled as synchrotron emission from a forward shock propagating into a wind-like circumstellar environment. We estimate the initial bulk Lorentz factor using the observed high-energy spectral cutoff. Considering the onset of the afterglow component, we constrain the deceleration radius at which this forward shock begins to radiate in order to estimate the maximum synchrotron energy as a function of time. We find that even in the LAT energy range, there exist high-energy photons that are in tension with the theoretical maximum energy that can be achieved through synchrotron emission from a shock. These violations of the maximum synchrotron energy are further compounded by the detection of very high-energy (VHE) emission above 300 GeV by MAGIC concurrent with our observations. We conclude that the observations of VHE photons from GRB 190114C necessitates either an additional emission mechanism at very high energies that is hidden in the synchrotron component in the LAT energy range, an acceleration mechanism that imparts energy to the particles at a rate that is faster than the electron synchrotron energy-loss rate, or revisions of the fundamental assumptions used in estimating the maximum photon energy attainable through the synchrotron process.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

Radio and X-Ray Observations of the Luminous Fast Blue Optical Transient AT 2020xnd

We present deep X-ray and radio observations of the fast blue optical transient (FBOT) AT 2020xnd/ZTF 20acigmel at z = 0.2433 from 13 days to 269 days after explosion. AT 2020xnd belongs to the category of optically luminous FBOTs with similarities to the archetypal event AT 2018cow. AT 2020xnd shows luminous radio emission reaching L ν ≈ 8 × 10 29 erg s -1 Hz -1 at 20 GHz and 75 days post-explosion, accompanied by luminous and rapidly fading soft X-ray emission peaking at L X ≈ 6 × 10 42 erg s -1 . Interpreting the radio emission in the context of synchrotron radiation from the explosion's shock interaction with the environment, we find that AT 2020xnd launched a high-velocity outflow (v ~ 0.1c–0.2c) propagating into a dense circumstellar medium (effective $\dot{M}\approx {10}^{-3}\,{M}_{\odot }$ yr -1 for an assumed wind velocity of v w = 1000 km s -1 ). Similar to AT 2018cow, the detected X-ray emission is in excess compared to the extrapolated synchrotron spectrum and constitutes a different emission component, possibly powered by accretion onto a newly formed black hole or neutron star. These properties make AT 2020xnd a high-redshift analog to AT 2018cow, and establish AT 2020xnd as the fourth member of the class of optically luminous FBOTs with luminous multiwavelength counterparts.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

DeepZipper: A Novel Deep-learning Architecture for Lensed Supernovae Identification

Large-scale astronomical surveys have the potential to capture data on large numbers of strongly gravitationally lensed supernovae (LSNe). To facilitate timely analysis and spectroscopic follow-up before the supernova fades, an LSN needs to be identified soon after it begins. To quickly identify LSNe in optical survey data sets, we designed ZipperNet, a multibranch deep neural network that combines convolutional layers (traditionally used for images) with long short-term memory layers (traditionally used for time series). We tested ZipperNet on the task of classifying objects from four categories—no lens, galaxy-galaxy lens, lensed Type-Ia supernova, lensed core-collapse supernova—within high-fidelity simulations of three cosmic survey data sets: the Dark Energy Survey, Rubin Observatory’s Legacy Survey of Space and Time (LSST), and a Dark Energy Spectroscopic Instrument (DESI) imaging survey. Among our results, we find that for the LSST-like data set, ZipperNet classifies LSNe with a receiver operating characteristic area under the curve of 0.97, predicts the spectroscopic type of the lensed supernovae with 79% accuracy, and demonstrates similarly high performance for LSNe 1–2 epochs after first detection. We anticipate that a model like ZipperNet, which simultaneously incorporates spatial and temporal information, can play a significant role in the rapid identification of lensed transient systems in cosmic survey experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2023

Merger Signatures are Common, but not Universal, in Massive, Recently Quenched Galaxies at z ~ 0.7

We present visual classifications of merger-induced tidal disturbances in 143 M* ~ 10 11 M ⊙ post-starburst galaxies at z ~ 0.7 identified in the $SQuIGG\vec{L}E$ Sample. This sample spectroscopically selects galaxies from the Sloan Digital Sky Survey that have stopped their primary epoch of star formation within the past ~500 Myr. Visual classifications are performed on Hyper Suprime-Cam imaging. We compare to a control sample of mass- and redshift-matched star-forming and quiescent galaxies from the Large Early Galaxy Census and find that post-starburst galaxies are more likely to be classified as disturbed than either category. This corresponds to a factor of $3.6$$^{+2.9}_{-1.3}$ times the disturbance rate of older quiescent galaxies and $2.1$$^{+1.9}_{-.73}$ times the disturbance rate of star-forming galaxies. Assuming tidal features persist for ≲500 Myr, this suggests merging is coincident with quenching in a significant fraction of these post-starbursts. Galaxies with tidal disturbances are younger on average than undisturbed post-starburst galaxies in our sample, suggesting tidal features from a major merger may have faded over time. This may be exacerbated by the fact that, on average, the undisturbed subset is fainter, rendering low-surface-brightness tidal features harder to identify. However, the presence of 10 young (≲150 Myr since quenching) undisturbed galaxies suggests that major mergers are not the only fast physical mechanism that shut down the primary epoch of star formation in massive galaxies at intermediate redshift.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2024

DESI Massive Poststarburst Galaxies at z ~ 1.2 Have Compact Structures and Dense Cores

Poststarburst galaxies (PSBs) are young quiescent galaxies that have recently experienced a rapid decrease in star formation, allowing us to probe the fast-quenching period of galaxy evolution. In this work, we obtained Hubble Space Telescope (HST)/WFC3 F110W imaging to measure the sizes of 171 massive (log(M $\ast$ /M ⊙ ) ~ 11) spectroscopically identified PSBs at 1 < z 1.3 selected from the DESI Survey Validation luminous red galaxy sample. This statistical sample constitutes an order of magnitude increase from the ~20 PSBs with space-based imaging and deep spectroscopy. We perform structural fitting of the target galaxies with pysersic and compare them to quiescent and star-forming galaxies in the 3D-HST survey. We find that these PSBs are more compact than the general population of quiescent galaxies, lying systematically ~0.1 dex below the established size–mass relation. However, their central surface mass densities are similar to those of their quiescent counterparts (log(Σ 1kpc /(M ⊙ kpc -2 ))~10.1). These findings are easily reconciled by later ex situ growth via minor mergers or a slight progenitor bias. These PSBs are round in projection (b/a median ~ 0.8), suggesting that they are primarily spheroids, not disks, in 3D. We find no correlation between the time since quenching and light-weighted PSB sizes or central densities. This disfavors apparent structural growth due to the fading of centralized starbursts in this galaxy population. Instead, we posit that the fast quenching of massive galaxies at this epoch occurs preferentially in galaxies with preexisting compact structures.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Swift-XRT Follow-up of Gravitational-wave Triggers in the Second Advanced LIGO/Virgo Observing Run

The Neil Gehrels Swift Observatory carried out prompt searches for gravitational-wave (GW) events detected by the LIGO/Virgo Collaboration (LVC) during the second observing run ("O2"). Swift performed extensive tiling of eight LVC triggers, two of which had very low false-alarm rates (GW170814 and the epochal GW170817), indicating a high confidence of being astrophysical in origin; the latter was the first GW event to have an electromagnetic counterpart detected. In this paper we describe the follow-up performed during O2 and the results of our searches. No GW electromagnetic counterparts were detected; this result is expected, as GW170817 remained the only astrophysical event containing at least one neutron star after LVC's later retraction of some events. A number of X-ray sources were detected, with the majority of identified sources being active galactic nuclei. We discuss the detection rate of transient X-ray sources and their implications in the O2 tiling searches. Finally, we describe the lessons learned during O2 and how these are being used to improve the Swift follow-up of GW events. In particular, we simulate a population of gamma-ray burst afterglows to evaluate our source ranking system's ability to differentiate them from unrelated and uncataloged X-ray sources. We find that ≈60%–70% of afterglows whose jets are oriented toward Earth will be given high rank (i.e., "interesting" designation) by the completion of our second follow-up phase (assuming that their location in the sky was observed), but that this fraction can be increased to nearly 100% by performing a third follow-up observation of sources exhibiting fading behavior.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

The Curious Case of PHL 293B: A Long-lived Transient in a Metal-poor Blue Compact Dwarf Galaxy

We report on small-amplitude optical variability and recent dissipation of the unusually persistent broad emission lines in the blue compact dwarf galaxy PHL 293B. The galaxy’s unusual spectral features (P Cygni-like profiles with ~800 km s -1 blueshifted absorption lines) have resulted in conflicting interpretations of the nature of this source in the literature. However, analysis of new Gemini spectroscopy reveals the broad emission has begun to fade after being persistent for over a decade prior. Precise difference imaging light curves constructed with the Sloan Digital Sky Survey and the Dark Energy Survey reveal small-amplitude optical variability of ~0.1 mag in the g band offset by 100 ± 21 pc from the brightest pixel of the host. The light curve is well-described by an active galactic nuclei (AGN)-like damped random walk process. However, we conclude that the origin of the optical variability and spectral features of PHL 293B is due to a long-lived stellar transient, likely a Type IIn supernova or nonterminal outburst, mimicking long-term AGN-like variability. This work highlights the challenges of discriminating between scenarios in such extreme environments, relevant to searches for AGNs in dwarf galaxies. This is the second long-lived transient discovered in a blue compact dwarf, after SDSS1133. Furthermore, our result implies such long-lived stellar transients may be more common in metal-deficient galaxies. Systematic searches for low-level variability in dwarf galaxies will be possible with the upcoming Legacy Survey of Space and Time at the Vera C. Rubin Observatory.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2019

Temperature control to reduce capacity mismatch in parallel-connected lithium ion cells

The temperature and capacity of individual cells affect the current distribution in a battery pack. Non uniform current distribution among parallel-connected cells can lead to capacity imbalance and premature aging. This paper develops models that calculate the current in parallel-connected cells and predict their capacity fade. The model is validated experimentally for a nonuniform battery pack at different temperatures. The paper also proposes and validates the hypothesis that temperature control can reduce capacity mismatch in parallel-connected cells. Three Lithium Iron Phosphate cells, two cells at higher initial capacity than the third cell, are connected in parallel. The pack is cycled for 1500 Hybrid Electric Vehicles cycles with the higher capacity cells regulated at 40 C and the lower capacity cell at 20 C. As predicted by the model, the higher capacity and temperature cells age faster, reducing the capacity mismatch by 48% over the 1500 cycles. A case study shows that cooling of low capacity cells can reduce capacity mismatch and extend pack life.

25 ENERGY STORAGE↗
DOE OSTI2019

Field Aging Testbed for Behind-the-Meter PV + Energy Storage

Small DC-coupled battery test systems are deployed at NREL to evaluate capacity fade models and report on performance parameters such as round-trip efficiency under indoor and outdoor deployment scenarios. Initial commercial battery products include LG Chem RESU Lithium-ion and Avalon vanadium-redox flow batteries. Adapting indoor lab-scale test methods to outdoor systems has challenges, including maintaining constant temperature and fully controlling batteries through standard discharge curves. Initial measurements show the Lithium Ion battery systems performing within expectation, near 85% round-trip efficiency. Initial lifetime modeling and measurements indicate battery capacity may degrade by 20%-35% over 10 years.

25 ENERGY STORAGE↗
DOE OSTI2021

Facile Synthesis of Micrometer-sized Hierarchical Porous Si@C Anodes for High-Performance Lithium-Ion Batteries

Extensive studies have been conducted to determine if replacing graphite anodes with silicon is feasible since silicon possesses a high capacity and is an abundant resource; however, Si anodes suffer significant volume changes during cycling, which pulverizes its structure and subsequently causes rapid capacity fading. We used SiO2 nanoparticles (nSiO2) and low-cost coal-derived humic acid as a feedstock to synthesize high performance Si-C anodes for Li-ion Batteries through spray drying, calcination, and magnesiothermic reductions. Our Si-C anodes features micrometer-sized porous Si coated with a graphitized carbon shell (mpSi@C). The hierarchical graphitized carbon shell and porous silicon structure relieve the mechanical stress of the Si phase upon cycling, which stabilizes the structure. This mpSi@C composite design allows for a high initial discharge capacity of 2199.9 mAh g-1 at 0.1 A g-1 and a cycling performance of 68% capacity retention after 100 cycles at 1.0 A g-1. The multipoint contact between the Si anode and C structure allows for a remarkable performance rate of 566.3 mAh g-1 at 5.0 A g-1.

01 COAL, LIGNITE, AND PEAT↗
DOE OSTI2022

Redox-flow batteries employing oligomeric organic active materials and size-selective microporous polymer membranes

Intermittent energy sources, including solar and wind, require scalable, low-cost, multi-hour energy storage solutions to be effectively incorporated into the grid. Redox-flow batteries offer a solution, but suffer from rapid capacity fade and low Coulombic efficiency due to the high permeability of redox-active species across the battery's membrane. Here we show that active-species crossover can be arrested by scaling the membrane's pore size to molecular dimensions and in turn increasing the size of the active material to be above the membrane's pore-size exclusion limit. When oligomeric redox-active organic molecules were paired with microporous polymer membranes, the rate of active-material crossover was either completely blocked or slowed more than 9,000-fold compared to traditional separators at minimal cost to ionic conductivity. In the case of the latter, this corresponds to an absolute rate of ROM crossover of less than 3 μmol cm−2 day−1 (for a 1.0 M concentration gradient), which exceeds performance targets recently set forth by the battery industry. This strategy was generalizable to both high and low-potential ROMs in a variety of electrolytes, highlighting the importance of macromolecular design in implementing next-generation redox-flow batteries.

Helms, Brett A.↗
DOE OSTI2023

Nanoparticle Surface Passivation Strategies to Improve the Cycle and Calendar Lifetime of Silicon Anodes in Standard Carbonate Electrolytes

Silicon Lithium alloys (SiLix) as the anode active material in a Li-Ion battery configuration offer possible energy densities paralleled only by pure lithium metal. However, the extreme mechanical deformation of alloying and dealloying SiLix through charge/discharge cycles paired with the highly reactive interface of SiLix which generates an interfacial layer known as the solid-electrolyte-interphase are large barriers to industrial adoption of high-silicon-content negative electrodes. Moreover, these challenges are magnified when the thickness of the electrode is brought to relevant levels (>3 mg/cm2). Here, I describe our efforts to address these challenges by utilizing single-nanometer-scale silicon nanoparticles to reduce capacity fade related to mechanical failure. I also detail our efforts to modify the silicon surface through interfacial chemical engineering strategies to passivate the silicon surface. This development three different majority silicon electrodes (50-74 wt%) to achieve cycle capacity retention of greater than 73% through 1000 charge/discharge cycles against capacity-matched NMC-based cathodes and calendar lifetimes greater than one year. This research is a part of the multi-national lab Silicon Consortium Project.

anodes↗