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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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

The effect of ink ball milling time on interparticle interactions and ink microstructure and their influence on crack formation in rod-coated catalyst layers

This work investigates the influence of ballmilling (sometimes also referred to as jar roller milling) time on cathode catalyst layer (CL) inks and electrode properties using formulations and coating methods relevant for industrial manufacturing. Four CL inks with the same composition were milled for 24, 48, 72, or 96 h. Rheological investigation of these inks showed a reduction of elastic moduli and steady-shear viscosity with continuous ink milling, which is correlated to a decrease in particle-particle interactions as well as formation of smaller agglomerates. Optical microscopy (OM) analysis of the fabricated electrodes revealed a trend in surface crack formation; formulations milled for 24 h contained the lowest average surface crack area percentages of 0.370% at heavy-duty loadings of ~0.300 mg Pt cm -2 , compared to 2.418% for the ink milled for 96 h. Further characterization of the CL through transmission electron microscopy (TEM) imaging showed a decrease in the mean agglomerate and pore size with milling time. Furthermore, these smaller electrode features were consistent with reduced fracture resistance and, hence, development of larger stresses during drying. Our results highlight the need to consider ink processing as an important component in defect-free CL manufacturing.

30 DIRECT ENERGY CONVERSION↗
DOE OSTI2021

Tuning Surface Stoichiometry of SOFC Electrodes at the Molecular and Nano-scale for Enhanced Performance and Durability

This project achieved the following objectives. Different cation segregation behaviors of different common SOFC cathodes, including La 0.6 Sr 0.4 Co0.2Fe 0.8 O 3-δ (LSCF), Sr 0.5 Sm 0.5 O 3-δ (SSC), and PrBa 0.5 Sr 0.5 Co 1.5 Fe 0.5 O5 +δ (PBSCF), were determined. We showed how oxygen partial pressure and gas impurities impact the stability of SOFC cathodes. We developed atomic layer deposition (ALD) coating techniques for electrodes and showed that by introducing different elements and different ALD oxidizers, electrode surface chemistry can be altered, resulting in enhanced oxygen reduction kinetics. In addition, we developed solution infiltration technique to enhance performance and durability of electrodes. Different infiltrates as well as different thermal treatment processes were screened to identify the optimal surface modification process that yields both low impedance and high durability. The modified cathode shows excellent stability and has a low area specific resistance (ASR) of only 0.2 Ωcm 2 at 600 °C after over 2000 hours of operation. Further, we developed ceramic anodes, SrFe(Co,Mo)O 3 (SFCM) and SrFe(Ni,Mo)O 3 (SFNM), and enhanced anode oxidation kinetics by solution infiltration or in situ catalyst exsolution from the ceramic anode surface. The modified anodes showed improved performance in full SOFCs, and the optimized anode modification shows high stability for over 400 hours at 550 °C. Moreover, the modified anode also demonstrates high durability in methane. This work provides fundamental understanding of electrode surface chemistry and demonstrates a simple, facile, cost-effective approach to enhance catalytic activity and durability of SOFC electrodes.

20 FOSSIL-FUELED POWER PLANTS↗
DOE OSTI2025

Mitigating Transition Metal Dissolution from Mn-rich Cathodes: Influence of Processing and Testing Methods

Manganese-rich oxides continue to gain interest with respect to the development of Earth-abundant options for lithium-ion cathodes. Of the unique challenges that hinder the respective performance of various classes of such materials, manganese dissolution still stands as a common theme. The work herein explores Li 3 PO 4 as a robust surface protection layer on a prototypical, Co-free, manganese-rich cathode in the way of a lithium- and manganese-rich oxide. The study highlights the critical importance of synthesis and processing in realizing optimal performance of a given surface treatment by comparing sol-gel and atomic layer deposition methods. Furthermore, cycling protocols are emphasized as a critical factor in adequately gauging the efficacy of surface protection strategies to mitigate manganese dissolution and the subsequent electrochemical consequence. Optimized Li 3 PO 4 coatings coatings on lithium- and manganese-rich cathode particles are shown to greatly mitigate capacity fade, impedance rise, pore/void formation and mechanical damage during long-term cycling.

Mallick, Subhadip [Argonne National Laboratory (AN↗
DOE OSTI2023

Rheo-electric measurements of carbon black suspensions containing polyvinylidene difluoride in N -methyl-2-pyrrolidone

Lithium-ion battery cathode slurries have a microstructure that depends sensitively on how they are processed due to carbon black's (CB) evolving structure when subjected coating flows. While polyvinylidene difluoride (PVDF), one of the main components of the cathode slurry, plays an important role in modifying the structure and rheology of CB, a quantitative understanding is lacking. In this work, we explore the role of PVDF in determining the structural evolution of Super C65 CB in N-methyl-2-pyrrolidinone (NMP) with rheo-electric measurements. We find that PVDF enhances the viscosity of NMP resulting in a more extensive structural erosion of CB agglomerates with increasing polymer concentration and molecular weight. We also show that the relative viscosity of all suspensions can be collapsed by the fluid Mason number (Mnf), which compares the hydrodynamic forces imposed by the medium to cohesive forces holding CB agglomerates together. Using simultaneous rheo-electric measurements, we find at high Mnf, the dielectric strength (Δε) scales with Mnf, and the power-law scaling can be quantitatively predicted by considering the self-similar break up of CB agglomerates. The collapse of the relative viscosity and scaling of Δε both suggest that PVDF increases the hydrodynamic force of the suspending medium without directly changing the CB agglomerate structure. These findings are valuable for optimizing the rheology of lithium ion battery cathode slurries. We also anticipate that these findings can be extended to understand the microstructure of similar systems under flow.

Mechanics↗
DOE OSTI2023

Enhanced Electrochemical Performance of Disordered Rocksalt Cathodes Enabled by a Graphite Conductive Additive

Cobalt-free cation-disordered rocksalt (DRX) cathodes are a promising class of materials for next-generation Li-ion batteries. Although they have high theoretical specific capacities (>300 mA h/g) and moderate operating voltages (~3.5 V vs Li/Li + ), DRX cathodes typically require a high carbon content (up to 30 wt %) to fully utilize the active material which has a detrimental impact on cell-level energy density. To assess pathways to reduce the electrode’s carbon content, the present study investigates how the carbon’s microstructure and loading (10–20 wt %) influence the performance of DRX cathodes with the nominal composition Li 1.2 Mn 0.5 Ti 0.3 O 1.9 F 0.1 . While electrodes prepared with conventional disordered carbon additives (C65 and ketjenblack) exhibit rapid capacity fade due to an unstable cathode/electrolyte interface, DRX cathodes containing 10 wt % graphite show superior cycling performance (e.g., reversible capacities ~260 mA h/g with 85% capacity retention after 50 cycles) and rate capability (~135 mA h/g at 1000 mA/g). Furthermore, a suite of characterization tools was employed to evaluate the performance differences among these composite electrodes. Overall, these results indicate that the superior performance of the graphite-based cathodes is largely attributed to the: (i) formation of a uniform graphitic coating on DRX particles which protects the surface from parasitic reactions at high states of charge and (ii) homogeneous dispersion of the active material and carbon throughout the composite cathode which provides a robust electronically conductive network that can withstand repeated charge–discharge cycles. Overall, this study provides key scientific insights on how the carbon microstructure and electrode processing influence the performance of DRX cathodes. Based on these results, exploration of alternative routes to apply graphitic coatings is recommended to further optimize the material performance.

25 ENERGY STORAGE↗
DOE OSTI2025

Developing low-cost rechargeable batteries: beyond traditional layered oxide cathodes for Li-ion and beyond Li-ion batteries

Here, the rising demand for energy storage systems, driven by the rapid adoption of electric vehicles and the global shift toward renewable energy, necessitates continuous efforts to lower the cost of current lithium-ion batteries (LIBs) and enhance the sustainability of existing battery chemistries. This feature article examines the key challenges associated with Ni- and Co-containing LIB cathodes and compares advancements in cathode development for non-traditional Li-ion and beyond Li-ion chemistries. First, a review of earth-abundant element containing disordered rock-salt cathodes is presented, with a discussion of key strategies such as compositional tuning and carbon coating to improve their electrochemical performance. Hurdles in developing oxide-based cathodes for Na- and K-ion batteries are also highlighted, followed by an in-depth overview of polyanion and Prussian blue cathodes for Na- and K-ion systems. Overall, this article provides a systematic perspective on the design of earth-abundant, low-cost, and sustainable cathode materials for both LIB and beyond LIB technologies.

Lohani, Harshita [Lawrence Berkeley National Labor↗
DOE OSTI2021

Deciphering Interfacial Chemical and Electrochemical Reactions of Sulfide-Based All-Solid-State Batteries

Large interfacial resistance resulting from interfacial reactions is widely acknowledged as one of the main challenges in sulfide electrolytes (SEs)-based all-solid-state lithium batteries (ASSLBs). However, the root cause of the large interfacial resistance between the SEs and typical layered oxide cathodes is not fully understood yet. Here we deciphered that interfacial oxygen loss from single-crystal LiNi 0.5 Mn 0.3 Co 0.2 O 2 (SC-NMC532) chemically oxidizes Li 10 GeP 2 S 12 , generating oxygen-containing interfacial species. Meanwhile, the interfacial oxygen loss also induces a structural change of oxide cathodes (layered-to-rocksalt). Besides, the high operation voltage can electrochemically oxidize SEs to form non-oxygen species (e.g. polysulfides). These chemically and electrochemically oxidized species, together with the interfacial structural change, are responsible for the large interfacial resistance at the cathode interface. More importantly, the widely adopted interfacial coating strategy is effective in suppressing chemically oxidized oxygen-containing species and mitigating the coincident interfacial structural change but is unable to prevent electrochemically induced non-oxygen species. These findings provide a deeper insight into the large interfacial resistance between the typical SE and layered oxide cathodes, which may be of assistance for the rational interface design of SE-based ASSLBs in future.

25 ENERGY STORAGE↗
DOE OSTI2025

Selective concentration of multivalent cations via electrodialysis through tandem membranes

Selective electrodialysis is attractive for recovering and recycling valuable ions. However, most studies in this field focus on membranes that are selective for monovalent ions. Multivalent cations preferentially partition into cation-exchange membranes, but low mobilities and concentration polarization limit electrodialysis selectivities for these cations. This work employs electrodialysis through an “in-series” combination of a Nafion membrane and a multilayer polyelectrolyte film (MPF)-coated Nafion membrane to concentrate and isolate La 3+ or Mg 2+ from monovalent ions. The bare Nafion membrane gives a La 3+ /Na + selectivity up to 4 (depending on conditions), which enables concentration of La 3+ with a high current efficiency. The MPF-coated membrane allows selective passage of Na + while rejecting La 3+ to increase the purity of the concentrated multivalent cation. For example, the concentration of La 3+ in the accumulation solution can reach 9 times its original concentration in the feed solution with a purity of 93 mol% (99 wt%) when starting with equimolar mixtures of NaNO 3 and La(NO 3 ) 3 . This study examines how the separation varies with the type of polyelectrolyte, the applied voltage, and the composition of feed, accumulation, and cathode solutions. Here, a high nitric acid concentration (0.5 M) in the cathode compartment allows monovalent anions to pass through the MPF-coated Nafion membrane to maintain the electroneutrality of the accumulation solution. With a low acid concentration (0.04 M) in the cathode chamber, water splitting occurs at the MPF-coated membrane and La(OH) 3 precipitates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Synergy of Graphene Nanoribbons and Graphene Sheets for High-Rate Lithium-Sulfur Batteries

According to the increasing demands for shortening the battery charging time, high current rate (C-rate) performances become more significant in practical applications. With a higher theoretical capacity, lithium-sulfur batteries are treated as promising candidates for the next-generation batteries. In this work, the utilization of graphene nanoribbons (GNRs) exhibits the benefits in conductivity and other electrochemical performances, especially for high-rate applications. With air-controlled electrospray as the method, carbon encapsulated sulfur particles, poly(acrylic acid), reduced graphene oxide (rGO) sheets, and GNRs are mixed and directly deposited onto the carbon coated aluminum collector, to employ as the cathode. The scanning electron microscopy (SEM) imaging exhibits that the two-dimensional structure of GNRs helps construct inter-connected networks. This improved structure of cathode can increase the electroconductivity, confirmed by the electrochemical impedance spectroscopy (EIS), and modify the porosity, indicated through pore size distribution profiles. In this way, the polysulfides can be more efficiently trapped and utilized, realizing the promising behavior with faster charge transfer. In terms of the cycling performance at 0.2 C, the batteries with GNRs can perform 18% higher in capacity than those without GNRs, without decreasing the charge retention. According to the rate-capability tests, systems with GNRs can achieve enhanced performance compared to batteries with precursor carbon nanotubes (CNTs), especially at high C-rates. At 2 C, with 80 wt % of graphene-based materials as GNRs, batteries can achieve an increase in capacity by 78% and 41% compared with systems without GNRs and those with CNTs, respectively. Accordingly, the results testify the synergy of GNRs and rGO sheets in Li-S batteries.

25 ENERGY STORAGE↗
DOE OSTI2024

Corrosion of Zinc Cold Spray Coatings in a Wet Sweet and Sour Gas Environment

Internal corrosion is a problem for steel pipelines transporting natural gas or CO 2 containing water and partial pressures of H 2 S higher than 0.3 kPa (0.05 psi). This work aims to mitigate internal corrosion in steel pipelines transporting natural gas containing H 2 S using cold spray coatings. Two types of the cold spray binary metallic coatings (zinc chromium [ZnCr]. zinc niobium [ZnNb]) were studied using electrochemical techniques: potentiodynamic polarization, linear polarization resistance, and electrochemical impedance spectroscopy. The corrosion resistance of cold spray coatings (ZnCr, ZnNb) was evaluated in an environment containing 4 bar CO 2 pressure, simulating the partial pressures found in gas transmission lines over a solution of 3.5 wt% NaCl heated to 40°C. A concentration of 0.003 M Na 2 S 2 O 3 ·5H 2 O, corresponding to H 2 S partial pressures around 0.079 bar (1.146 psi), was used to simulate sour conditions. Postcorrosion surface characterization was performed using a scanning electron microscope (SEM) equipped with an energy-dispersive x-ray spectroscope (EDS) and x-ray diffraction analysis. The data showed that the presence of 0.003 M Na 2 S 2 O 3 ·5H 2 O shifted the corrosion potential to more anodic values and decreased the corrosion current density. Both coatings showed similar behavior after 1 h of exposure in the CO 2 /H 2 S environment, indicating that similar electrochemical reactions were occurring on ZnNb and ZnCr. SEM images and EDS surface analyses for specimens showed a significant change in the surface chemical composition of carbon steel coated with ZnNb and ZnCr after 24 h of immersion. In the presence of thiosulfate (under sour conditions), the formation of corrosion product layers (ZnCO 3 and ZnS) on top of ZnNb and ZnCr coatings increased their corrosion resistance, which helped to reduce their corrosion by a factor of 2. Under a sweet environment, the corrosion rates for steel coated with cold spray coatings after 14 d of exposure are lower than that for galvanized steel by a factor of 5 due to the ZnCO 3 layer formed on top of the coatings. The ZnCO 3 layer formed on the steel surface acts as a physical barrier against corrosion by blocking the diffusion of corrosive species to the surface. No localized attack was observed. ZnCr Cold spray coating with defect showed promising corrosion protection against CO 2 corrosion (sweet corrosion) after 14 d of exposure to a CO 2 environment. Here, the scratch on the coating simulated damage created in service, and it was deep enough to expose the substrate material (steel). The formation of zinc oxide (ZnO) and zinc carbonate (ZnCO 3 ) on the scratch confirmed the cathodic protection of the steel by ZnCr and ZnNb coatings.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Unravelling electro-chemo-mechanical interplay in layered oxide cathode degradation in solid-state batteries

Solid-state batteries (SSBs) hold notable promise for advancing energy storage technologies. However, their commercial viability is limited by the poor cycle stability and complex degradation mechanism. This study underscores the pivotal role of electro-chemo-mechanical interactions in driving the failure of SSBs. Leveraging advanced x-ray imaging and spectroscopy techniques, we analyzed LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) cathodes from cycled Li x In||Li 6 PS 5 Cl (LPSC)||NMC811 SSBs, uncovering the interplay between microstructure, chemical heterogeneity, mechanical characteristics, and electrochemical performance. Our results show that revealing electro-chemo-mechanical interactions is essential to develop strategies to suppress the degradation of SSBs. Particularly, we revisit a LiNbO 3 (LNO) coating layer to mitigate electrochemical degradation. The LNO@NMC811 cathode retains 116 milliampere-hours per gram after 200 cycles, showing excellent stability, while the uncoated NMC811 cathode keeps degrading over time, with suppressed chemical heterogeneity and mechanical failure. This work highlights the importance of synergizing advanced material design with coating techniques, ensuring uniform lithium flux and improving mechanical properties to achieve stable, high-performance SSBs.

Zheng, Xueli [SLAC National Accelerator Laboratory↗
DOE OSTI2022

Precision surface modification of solid oxide fuel cells via layer-by-layer surface sol–gel deposition

While solid oxide fuel cells (SOFCs) are a promising technology for a clean and sustainable future, their commercialization is hindered by limited durability and performance. Here, we report our findings on the application of a layer-by-layer surface sol–gel (SSG) coating of catalysts to dramatically enhance the electro-catalytic activity and durability of SOFC cathodes. The SSG process is capable of penetrating and preserving complex backbone microstructures of porous electrodes, creating highly conformal coatings of controlled morphology, while tailoring the composition of the surface to improve catalytic properties and durability. For example, the application of an SSG coating of PrO x to a La 0.6 Sr 0.4 Co 0.2 Fe 0.8 O 3–δ (LSCF) cathode has reduced the polarization resistance from 1.136 to 0.117 Ω cm 2 at 600 °C and the degradation rate from 1.13 × 10 –3 to 2.67 × 10 –4 Ω cm 2 h –1 at 650 °C. In addition, a continuous improvement in electrode performance is demonstrated as the thickness of the coating is increased, corresponding to the linear addition of catalyst. Furthermore, this first application of the SSG technique to SOFC systems opens the door for the controlled surface modification of porous components in electrochemical systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Reduction of Methane Leaks through Corrosion Mitigation Pre-treatments for Pipelines with Field Applied Coatings

Corrosion of buried, coated steel pipelines transporting natural gas is a significant source of methane emissions, from pipeline venting required for maintenance and repairs and from pipeline leaks and incidents. Corrosion of steel under field applied coatings is an important safety concern for the pipeline industry. This project investigates the application of a field applied alloy over girth welds to mitigate external corrosion of buried coated steel pipelines. Various metallic coating options were considered, which were required to meet several criteria: (1) it must resist corrosion under open-circuit or mild cathodic protection conditions, (2) it must protect the substrate steel, and (3) it must not negatively affect the adhesion of the field coating. Finite element models and lab testing were performed of alloy coating compositions to identify promising alloy types underneath disbonded coatings. Polarization curves of coating alloys were generated to provide the boundary conditions for the COMSOL model to compute potential and current distributions around coated areas. Sacrificial and corrosion-resistant metal alloy coatings were evaluated and optimized using corrosion modeling and laboratory electrochemical testing, where aluminum alloy 5356 (5% Mg) and steel alloy B9 (9% Cr) were selected. Corrosion test coupons were designed and fabricated using thermal spray aluminum 5356 and welded B9 steel overlays on API 5L grade X42 line pipe steel. The corrosion test coupons, with simulated pipe coating damage, were tested in a laboratory soil box and a field pipeline site in Texas for 3-months. Corrosion test coupons were then tested for 6-months at field pipeline sites in Texas and Tennessee to quantify corrosion rates and performance of the aluminum and steel alloys under polyethylene tape and 2-part epoxy coatings, various coating holidays, and with and without cathodic protection.

03 NATURAL GAS↗
DOE OSTI2023

On the Electrochemical Properties of Carbon-Coated NaCrO 2 for Na-Ion Batteries

NaCrO 2 is a promising cathode for Na-ion batteries. However, further studies of the mechanisms controlling its specific capacities and cycle stability are needed for real-world applications in the future. This study reveals, for the first time, that the typical specific capacity of ~110 mAh/g reported by many researchers when the charge/discharge voltage window is set between 2.0 and 3.6 V vs. Na/Na + is actually controlled by the low electronic conductivity at the electrode/electrolyte interface. Through wet solution mixing of NaCrO 2 particles with carbon precursors, uniform carbon coating can be formed on the surface of NaCrO 2 particles, leading to unprecedented specific capacities at 140 mAh/g, which is the highest specific capacity ever reported in the literature with the lower and upper cutoff voltages at the aforementioned values. However, such carbon-coated NaCrO 2 with ultrahigh specific capacity does not improve cycle stability because with the specific capacity at 140 mAh/g the Na deintercalation during charge is more than 50% Na ions per formula unit of NaCrO 2 which leads to irreversible redox reactions. The insights from this study provide a future direction to enhance the long-term cycle stability of NaCrO 2 through integrating carbon coating and doping.

25 ENERGY STORAGE↗
DOE OSTI2022

Surface Stabilization with Fluorine of Layered Ultrahigh-Nickel Oxide Cathodes for Lithium-Ion Batteries

High-nickel layered oxide cathodes are key to meet the demands of the electric vehicle industry because of their high specific capacity. However, commercialization of these materials is hindered by critical challenges, such as phase transitions, particle cracking, aggressive surface reactivity, and thermal instability. Cation doping along with surface coating has proven to be an effective way to circumvent some of these issues to a large extent. Herein, fluorine coating is employed on a high-nickel Li[Ni 0.95 Mn 0.015 Co 0.02 Al 0.01 Mg 0.005 ]O 2 (NMCAM) cathode via a solution route. Detailed structural and electrochemical analyses indicate fluorine largely decorates the surface at low enough calcination temperatures. The cathode with 1 mol % fluorine coating exhibits a capacity retention of 71% after 500 cycles as compared to 59% for the control sample when cycled to a high cutoff voltage of 4.3 V in a full cell configuration with graphite anode. Post-mortem analysis of cycled electrodes reveals that surface reactivity is a major contributor to capacity fade as compared to particle cracking. Fluorine coating reduces surface reactivity and the depth to which rock-salt phase is formed on the surface during cycling. The thermal stability is also enhanced after fluorine coating as the material shows less heat release at high states of charge. Furthermore, this work demonstrates an effective, economical, and scalable way to stabilize the surface with fluorine and enhance the electrochemical performance of high-nickel cathodes.

25 ENERGY STORAGE↗
DOE OSTI2021

An ultrathin solid-state electrolyte film coated on LiNi 0.8 Co 0.1 Mn 0.1 O 2 electrode surface for enhanced performance of lithium-ion batteries

We report layered Ni-rich oxide is a promising cathode material for lithium-ion batteries (LIBs) of high energy density, yet its poor electrochemical stability induced by electrode-electrolyte interfacial degradation has still needed to be addressed. Surface coating is one of the powerful techniques to tackle this issue, nevertheless, it has been extensively used on particle but not electrode regarding a larger area of protection. Herein, we have covered a nano-scaled layer of lithium phosphorus oxynitride (LiPON) on the electrode level of LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM) surface and found lower impedance, longer cycle life, and better safety for treated battery. Most notably, such an NCM-LiPON based 1.3 Ah pouch cell delivers an energy density of 364.4 Wh kg -1 (based on positive and negative materials), along with the retention of 80.0% over 745 cycles at 0.5 C-rate, which is 1.3 times longer than the bare one. This results from modification of both superficial cathode-electrolyte interphase (CEI) and structure stabilization of general particle surface, therefore, role of conformal coating upon electrode surface should be highlighted.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Solvent‐Phobic and Ionophilic Carboxylated Polythiophene Layer for Fluoride‐Rich Cathode Electrolyte Interphase

Abstract One focal area of contemporary organic mixed ionic‐electronic conductor (OMIEC) research relates to utilization of dual‐conductive properties to enhance the ion/electron transfer kinetics for energy storage applications. Insight regarding OMIEC response toward the electrolyte anion and solvent used in lithium‐ion batteries (LIBs), however, is limited. Here, for the first time, the solvent‐phobic and ionophilic (SP‐IP) properties of the OMIEC, poly[3‐(potassium‐4‐butanoate)thiophene‐2,5‐diyl] (P3KBT), are revealed through comprehensive evaluation and characterization. The solvent‐phobic characteristics arise from the cooperation of dispersive interaction, polar interaction, and hydrogen‐bonding between P3KBT and electrolyte solvent. The ionophilic nature is driven by electrostatic interactions between P3KBT side chain carboxylate groups and LiPF 6 , and the reversible electrochemical doping/de‐doping of the polythiophene backbone with PF 6 ⁻ . The SP‐IP properties induce formation of a LiF‐ rich , Li 2 CO 3 ‐ limited cathode electrolyte interphase (CEI) layer when a P3KBT coating layer is applied to the active material surface, significantly improving half‐cell life to over 1500 cycles at 2C.

Ren, Haoze [Department of Chemical and Bimolecular↗
DOE OSTI2021

Enabling aqueous processing for LiNi 0.80 Co 0.15 Al 0.05 O 2 (NCA)-based lithium-ion battery cathodes using polyacrylic acid

Replacing N-methyl-2-pyrrolidone (NMP) with water in the production of lithium-ion battery cathodes is critical to realizing process cost savings and improved worker safety. LiNi 0.80 Co 0.15 Al 0.05 O 2 (NCA) is a poor fit for aqueous processing due to destructive Al current collector corrosion resulting from highly basic slurries and detrimental surface reconstruction reactions that occur in water. In this study, polyacrylic acid (PAA, MW = 450,000 g·mol -1 ) is examined as a corrosion-mitigating and surface-stabilizing agent. Adding PAA to an aqueous NCA slurry can provide a stable pH (4.0–8.5) for at least 4 h, since the carboxyl groups from PAA dissociate and increase the proton concentration in the slurry. Further, these groups can also adsorb to the surface of NCA particles and provide electrostatic stability from active material particle agglomeration, as revealed by zeta potential measurements. Minor cracking does occur at the electrode surface; this cracking likely caused poorer adhesion to the Al current collector in the aqueous-processed film when compared to the NMP-processed baseline. Electrochemically, the leached Li does cause a lower initial capacity for the aqueous-processed cathode, though the capacity retention of the aqueous-processed cathode is better than the baseline. The cracks in the coating led to a rise in charge transfer resistance that hindered rate capability above 1C.

25 ENERGY STORAGE↗