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At least 19 records

From Materials to Cell: State-of-the-Art and Prospective Technologies for Lithium-Ion Battery Electrode Processing

Electrode processing plays an important role in advancing lithium-ion battery technologies and has a significant impact on cell energy density, manufacturing cost, and throughput. Compared to the extensive research on materials development, however, there has been much less effort in this area. In this Review, we outline each step in the electrode processing of lithium-ion batteries from materials to cell assembly, summarize the recent progress in individual steps, deconvolute the interplays between those steps, discuss the underlying constraints, and share some prospective technologies. Finally, this Review aims to provide an overview of the whole process in lithium-ion battery fabrication from powder to cell formation and bridge the gap between academic development and industrial manufacturing.

25 ENERGY STORAGE↗

Correlation among porosity, mechanical properties, morphology, electronic conductivity and electrochemical kinetics of dry-processed electrodes

Dry processing (DP) has received great interest recently, which poses many advantages over the conventional slurry-based processing. Here, this work investigates the effect of compression on electrode mechanical properties, morphology, electronic conductivity, and electrochemical kinetics. Similar to the slurry-based electrodes, LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC) cathodes with intermediate porosity (i.e., 32%) demonstrate lowest charge transfer resistance, highest electronic conductivity and best rate performance. Fracture of NMC secondary particles is observed in the dry processed NMC cathodes. Reducing electrode porosity results in more fracture in the NMC secondary particles.

25 ENERGY STORAGE↗

High‐Loading Lithium‐Sulfur Batteries with Solvent‐Free Dry‐Electrode Processing

Abstract Lithium‐sulfur (Li‐S) batteries, with their high energy density, nontoxicity, and the natural abundance of sulfur, hold immense potential as the next‐generation energy storage technology. To maximize the actual energy density of the Li‐S batteries for practical applications, it is crucial to escalate the areal capacity of the sulfur cathode by fabricating an electrode with high sulfur loading. Herein, ultra‐high sulfur loading (up to 12 mg cm −2 ) cathodes are fabricated through an industrially viable and sustainable solvent‐free dry‐processing method that utilizes a polytetrafluoroethylene binder fibrillation. Due to its low porosity cathode architecture formed by the binder fibrillation process, the dry‐processed electrodes exhibit a relatively lower initial capacity compared to the slurry‐processed electrode. However, its mechanical stability is well maintained throughout the cycling without the formation of electrode cracking, demonstrating significantly superior cycling stability. Additionally, through the optimization of the dry‐processing, a single‐layer pouch cell with a loading of 9 mg cm −2 and a novel multi‐layer pouch cell that uses an aluminum mesh as its current collector with a total loading of 14 mg cm −2 are introduced. To address the reduced initial capacity of dry‐processed electrodes, strategies such as incorporating electrocatalysts or employing prelithiated active materials are suggested.

Chemistry↗

Micron Size NaCrO 2 Particles Enable High‐loading Dry‐processed Electrode for Sodium Ion Batteries

Dry-process fabrication using fibrillatable binder is emerging as a promising method to produce high-loading electrodes for energy storage applications, favored by its cost-efficiency and eco-friendliness. While previous studies have demonstrated the advantages of dry process over the traditional slurry method, there remains a gap in understanding how the particle size of active materials influences the mechanical and electrochemical performance of dry electrodes. In this study, four different particle size NaCrO 2 materials (Average size, S-NCO: 0.6 µm, M1-NCO 1.5 µm, M2-NCO: 4.4 µm, and L-NCO: 9.9 µm) are synthesized to investigate the effect of particle size on dry-processed high-loading electrodes. The findings reveal that the larger micron-sized (>4.4 µm) NCO dry films exhibit significantly improved tensile strength and electrochemical performance, primarily ascribed to the low film porosity, abundant inter-particle connection by the binder, comprehensive carbon coverage, and efficient percolation of the conductive pathway. Notably, a full cell incorporated with a high loading (5.2 mAh cm −2 ) and high active material ratio (96.5 wt.%) L-NCO film electrode demonstrates promising cycling stability and rate capability. Furthermore, these results provide valuable insights regarding the design and fabrication of dry-processed electrodes for future energy storage applications.

25 ENERGY STORAGE↗

Understanding and Enhancing Silicon Nanoparticle Distribution during Electrode Processing

Silicon-dominant anodes are of great interest because of their potential to boost the cell-level energy of state-of-the-art Li-ion batteries. While silicon materials have been extensively studied, understanding interactions at the electrode level has recieved little attention, especially the coating process of Si particles, which plays an equally important role in unlocking the full potential of silicon anodes. Herein, the electrode processing of a Si-dominated anode (52.8 wt%, 3.5–4.5 mAh cm −2 ) is being investigated to understand the relationship of processing on the morphology and properties of Si anodes at the electrode level. It has been found that almost-undetectable Si agglomerates easily form during electrode processing, which grow into largeprotrusions after lithiation and trigger potential internal shorting and self-discharge problems. A facile slurry filtration step is proposed to homogenize the particle distribution within Si-dominant electrodes which improves the electrochemical performance and storage stability of Si-based Li ion batteries.

Wu, Bingbin↗

Advanced electrode processing for lithium-ion battery manufacturing

Lithium-ion batteries (LIBs) need to be manufactured at speed and scale for their use in electric vehicles and devices. However, LIB electrode manufacturing via conventional wet slurry processing is energy-intensive and costly, challenging the goal to achieve sustainable, affordable and facile manufacturing of high-performance LIBs. Here, in this Review, we discuss advanced electrode processing routes (dry processing, radiation curing processing, advanced wet processing and 3D-printing processing) that could reduce energy usage and material waste. Maxwell-type dry processing is a scalable alternative to conventional processing and has relatively low manufacturing cost and energy consumption. Radiation curing processing could enable high-throughput manufacturing, but binder selection is limited to certain radiation curable chemistries. 3D-printing processing can produce electrodes with diverse architectures and improved rate performance, but scalability is yet to be demonstrated. 3D-printing processing is good for special applications where throughput and cost can be compromised for performance.

25 ENERGY STORAGE↗

Exploring the potential and impact of single-crystal active materials on dry-processed electrodes for high-performance lithium-ion batteries

Roll-to-roll powder-to-film dry processing (DP) and single-crystal (SC) active materials (AMs) with many advantages are two hot topics of lithium-ion batteries (LIBs). However, DP of SC AMs for LIBs is rarely reported. Consequently, the impact of SC AMs on dry-processed LIBs is not well understood. Herein, for the first time, via a set of experimental and theoretical studies of the conventional polycrystalline-AM- and SC-AM-based DPed electrodes (DPEs), this work not only reports a high-performance dry SC-AM cathode for LIB manufacturing, but also establishes some fundamental understanding of SC-based dry-processed electrodes, including their morphology, structure, mechanical strength, electronic conductivity and LIB electrochemical behavior. Further, the results suggest that DP of SC AMs is promising, which can dramatically improve the electrochemical kinetics at electrode level and particle level. Specifically, for the rate capability and long-term cyclability in full cells, SC DPEs exhibit a discharge specific capacity of 152.1 mAh g -1 at 1C and a capacity retention rate of 79.9 % at C/3 over 500 cycles, which are superior to those of PC DPEs (135.6 mAh g -1 and 68.3 %) at the same conditions and are further confirmed by the simulation data from the theoretical modelling study. Therefore, this comprehensive work marks a significant milestone for DP strategy and SC AMs, enlightening future research and development of LIB manufacturing.

25 ENERGY STORAGE↗

Dry-processed electrodes enabled by polytetrafluoroethylene fibrillation for high-performance lithium-ion batteries

The dry processing technique of polytetrafluoroethylene (PTFE) fibrillation offers significant advancements in cost reduction, environmental impact, and electrochemical performance. Dry processing alone allows for ∼ 20–60% cost reduction and increases of up to 40 mg cm⁻2 of areal loading – it typically comes at a reduction of rate capability. By leveraging the network structure of fibers, this method enhances rate capability and cycling performance, providing a compelling alternative to the conventional and currently predominant wet processing. The review delves into PTFE fibrillation mechanisms and examines critical influencing factors including material properties and processing parameters. It also discusses challenges associated with the electrodes fabricated by PTFE fibrillation, including structural instability due to insufficient PTFE fibrillization, compromised electrical conductivity from an insufficient conductive network, inhomogeneous dispersion resulting from the absence of solvents, restricted ionic transport due to increased electrode thickness, inadequate adhesion to current collector because of low surface energy of PTFE, electrochemical degradation due to low lowest unoccupied molecular orbital (LUMO) level of PTFE, particle damage during processing and environmental concerns related PTFE being a perfluoroalkyl and polyfluoroalkyl substances (PFAS). Recent research innovations aimed at mitigating these issues, their application in beyond-lithium batteries, and future research directions are thoroughly discussed.

Park, Hyunji↗

Effect of Fluoride Anions on Nd(III) Electrode Processes and Nd Metal Recovery in LiCl–KCl–NdCl 3

Here, this work investigated the impact of fluoride anions on Nd metal recovery in LiCl–KCl–NdCl 3 electrolytes by introducing LiF at a molar F/Nd ratio of 9 at 773 K. The voltammetric measurements confirmed that the fluoride ions facilitated single-step Nd(III)/Nd reduction by promoting the stability of the Nd(III) state compared to two-step reduction (Nd(III)/Nd(II) and Nd(II)/Nd) in all-chloride electrolytes. The stabilized Nd(III) state in the LiF-containing electrolyte effectively suppressed partial Nd(III)/Nd(II) reduction and the back-dissolution of Nd metal via comproportionation. By suppressing these reactions, high round-trip Coulombic efficiencies of 77–86% were achieved in the LiF-containing electrolyte during selective Nd deposition–removal cycles compared to 53–59% in all-chloride electrolytes. The Faradaic yield for Nd metal recovery was estimated at 38.6% in the LiF-containing electrolyte following long-term electrolysis, more than three times higher than 11.3% in all-chloride electrolytes. These results confirm the beneficial effect of fluoride ions on Nd metal recovery in low-melting chloride-based electrolytes, promising efficient Nd recovery at low temperatures.

11 - NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Positive electrode processing for Hughes NiH2 cells

The basic procedures were developed for the manufacture of nickel cadmium batteries. An electrochemical impregnation in an aqueous ethanol solution is used in this process. Several additional controls were instituted for production of flight electrodes, including a Hughes controlled MCD, a solution reserved exclusively for the impregnation of Hughes positive electrodes a system of complete traceability for individual electrodes, an electrical characterization test to provide information on weight and capacity at the plaque level, and a stress test to provide data on capacity, weight, and physical parameters at the electrode level.

Bleser, C. A.↗

Probing Anion Exchange Membrane Fuel Cell Cathodes by Varying Electrocatalysts and Electrode Processing

To date, several high-performing anion exchange membrane fuel cells (AEMFCs) have been demonstrated, but most these studies have focused on Pt containing cathodes with high loadings. Here, we explore and compare the performance and perform electrochemical diagnostics on three leading AEMFC cathode electrocatalysts: Pt/C, Ag/C, and Fe–N–C with electrodes that have been processed with either powder or dispersion-based ionomers using perfluorinated anion exchange polymers. Pt/C had the highest performance but also showed a strong dependence on ionomer type, with powder ionomer exhibiting much higher performance. These results were consistent with the observations for Ag/C but did not hold for the Fe–N–C catalyst where almost no change was observed between powder and dispersion-based ionomers. This is the first-time the impact of powder and dispersion ionomer with different classes of cathode electrocatalysts on the fuel cell performance have been compared, and the results have strong implications for the ability to achieve high performance at low loadings and for better understanding catalyst-ionomer interactions within AEMFCs.

30 DIRECT ENERGY CONVERSION↗

Implementing hydrogen oxidation reaction on Pt for controlling counter electrode processes

The search for active, stable, and durable materials for electrochemical energy technologies requires increasing levels of precision to establish true structure-function relationships and guide materials design from atomic and molecular scale. This increases the level of control required over the experimental system for proper materials evaluation. The choice of counter electrode material become crucial, as Pt dissolution at high voltages may cause contamination to the working electrode, especially when studying reductive processes in reactions such as oxygen reduction reaction (ORR), H 2 evolution reaction (HER), and the CO 2 reduction reaction. The learnings from “old school” electrochemistry groups lead us to leverage H 2 reactions over Pt to construct a counter electrode system with controlled potential that eliminates Pt ion contamination concerns. In here we discuss the construction of such Pt|H 2 counter electrode where key experimental aspects such as the H 2 flow rate and effective distribution determines the maximum current this counter electrode can accommodate before switching to high voltage and triggering Pt dissolution. Lastly, we demonstrate the use of the Pt|H 2 counter electrode in aqueous electrolytes during HER occurring on the working electrode at varying currents, showing that the Pt content in the cell remains below parts per trillion (ppt) up to 10 mA, and below 50 ppt at 100 mA up to 1 h of constant current hold. This work provides a guide to the implementation of Pt|H 2 counter electrodes to improve the precision of electrochemical experiments in search of highly active, selective, and durable materials for energy technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Green Electrode Processing Enabled by Fluoro-Free Multifunctional Binders for Lithium-Ion Batteries

The eco-friendly processing of conjugated polymer binder for lithium-ion batteries demands improved polymer solubility by introducing functional moieties, while this strategy will concurrently sacrifice polymer conductivity. Employing the polyfluorene-based binder poly(2,7-9,9 (di(oxy-2,5,8-trioxadecane))fluorene) (PFO), soluble in water-ethanol mixtures, a novel approach is presented to solve this trade-off, which features integration of aqueous solution processing with subsequent controlled thermal-induced cleavage of solubilizing side chains, to produce hierarchically ordered structures (HOS). The thermal processing can enhance the intermolecular π–π stacking of polyfluorene backbone for better electrochemical performance. Notably, HOS-PFO demonstrated a substantial 6–7 orders of magnitude enhancement in electronic conductivity, showcasing its potential as a functional binder for lithium-ion batteries. As an illustration, HOS-PFO protected SiOx anodes, utilizing in situ side chain decomposition of PFO surrounding SiOx particles after aqueous processing are fabricated. HOS-PFO contributed to the stable cycling and high-capacity retention of practical SiOx anodes (3.0 mAh cm -2 ), without the use of any conducting carbon additives or fluorinated electrolyte additives. It is proposed that this technique represents a universal approach for fabricating electrodes with conjugated polymer binders from aqueous solutions without compromising conductivity.

25 ENERGY STORAGE↗

To Pave the Way for Large-Scale Electrode Processing of Moisture-Sensitive Ni-Rich Cathodes

High-capacity Ni-rich cathode such as LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NMC811) has a great potential to enable high energy lithium-ion batteries (LIBs) for long-range electrical vehicles. However, the utilization of NMC 811 in large-scale application is still challenging. While many published papers on NMC811 focus on materials modification, the moisture sensitivity of NMC811 and its implications in storage and large-scale electrode coating are not well explored, not to mention how to overcome those challenges for industry application. This work discusses the key parameters impacting the rheological properties of NMC811 slurries and their correlations to the properties of dried electrodes. Effective solutions are proposed to address the gelation issue of NMC811 slurry during large-scale coating to hopefully inspire more effective and practical approaches to tackle the grand challenges in electrochemical energy storage.

25 ENERGY STORAGE↗

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↗

Performance Comparison Between NiH2 Dry Sinter and Slurry Electrode Cells

The electrical and thermal performance of dry sinter and slurry process electrode cells manufactured for the Hubble Space Telescope (HST) batteries have been characterized for a matrix of operating conditions over the temperature range from 14 to 86 F at various charge control levels. The dry sinter process electrode cells tested are similar to the onboard HST NiH2 cells. The slurry process electrode cells were developed to be less susceptible to electrode expansion and impedance changes with life. Both cell types were impregnated by the aqueous electrochemical process. Test conditions included standard capacity tests and electrical cycling using 96-minute cycling regimens incorporating gr depth-of-discharge (DOD) cycles. The dry sinter process electrodes have higher operating capacities to 1.20V/cell, but both electrode types have similar heat dissipation for the conditions tested. The results of the testing included cyclic heat generation during a typical 96-minute cycle, operating capacity data vs. cutoff voltage to generate a temperature-compensated voltage curve, and voltage characteristics suitable to develop a voltage prediction model. Analysis of data shows differences in the discharge voltage plateaus operating conditions evaluated. This is the basis for recommended changes in the battery charge control.

Armantrout, J. D.↗

Unraveling the impact of the degree of dry mixing on dry-processed lithium-ion battery electrodes

Dry processing of lithium-ion battery electrodes facilely realizes the powder-to-film manner, which is thus regarded as a highly promising strategy for lithium-ion battery manufacturing. However, a fundamental understanding of the impact of the involved dry mixing is still rarely reported. In this work, the degree of dry mixing is monitored by the dry mixing time, and a set of dry-processed electrodes with different degree of dry mixing is accordingly prepared and comprehensively studied. This work novelly reveals that the degree of dry mixing exhibits pronounced impact on the morphology, the homogeneity of electrode components and the degree of PTFE fiberization, which leads to difference in the mechanical strength and electrochemical performance of dry-processed electrodes. Accordingly, it is suggested that a moderate degree of dry mixing is preferred for high-performance dry-processed lithium-ion battery electrodes.

25 ENERGY STORAGE↗