Redox Reversible Materials for EV Batteries

A method to prepare high quality monolithic lithium-nickel-manganese-cobalt oxide (NMC) positive electrode materials for batteries with improved performance and processability compared to conventional polycrystalline NMC. The method involves a solid-state reaction followed by wet milling and heat treatment to produce NMC particles with single crystal monolithic morphology. The wet milling step separates primary particles from agglomerated secondary particles. The heat treatment heals any cracks formed during milling. This allows controlling the particle size and morphology for optimal battery performance. The resulting monolithic NMC has uniform particle size distribution with D50 between 2-8 um and span less than 1.5.

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Cathode material for lithium-ion batteries with improved stability and cycling performance compared to traditional lithium iron phosphate (LFP) cathodes. The new cathode has a fluoride-doped olivine crystal structure formed by a specific process. It involves calcining a mixture of fluoride-containing lithium source and fluoride-free lithium source at intermediate temperatures. The calcined material is then heated in a reducing atmosphere to form the fluoride-doped olivine cathode active material. The process provides a cathode with uniform fluoride distribution, small particle size, and carbon coating for stability.

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Fluorinated lithium-rich and manganese-based oxide (LMR) for high capacity, stable lithium-ion battery positive electrodes. The fluorinated LMR has the formula Li1+xMe1−xO2−yFy, where Me is mainly Mn, x is 0-0.33, and y is 0-0.1. The fluorine ions in the crystal structure improve capacity and cycling stability compared to non-fluorinated LMR. The fluorinated LMR can be made by mixing non-fluorinated LMR with a fluorine-containing solution, removing the solvent, and coating the fluorinated LMR onto a substrate to form the electrode.

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Cathode material for lithium-ion batteries that has improved cycle life and safety compared to conventional disordered rocksalt cathodes. The cathode material is a disordered rocksalt oxide with a lithium-containing cation and an anion comprising oxygen, fluorine, and optionally phosphorus, sulfur, and nitrogen. The composition has a higher fluorine content compared to just oxygen, which improves cycle life and reduces oxygen redox voltage for safer batteries. The cation can be lithium and another metal. The anion ratio is desirably oxygen-majority with minor fluorine and optionally P, S, N.

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Air-stable organic crystal-based metal ion batteries (MIBs) are important for cost-effective renewable energy storage. In the dearth of such crystalline organic reservoirs, a family porphyrin-fused extended conjugated sulfonamide compounds (ECSA) has been demonstrated here MIBs lithium (LIBs). The ECSA forms class metalloporphyrins (M4ZnSOTAPP) having different possibilities (M = Li+/Na+/K+) with four redox meso positions. discharge voltage Li4ZnSOTAPP LIB is found to be 2.5 V vs Li/Li+, in line theoretical calculations, capacity ~100 mAhg-1 cell constructed practically relevant conditions 1M electrolyte. Further demonstration stable performance (83 % retention till 500 cycles), its crystal structure and charge-discharge mechanism have unraveled. extension this synthetic strategy K4ZnSOTAPP crystals further establishes avenue -extended structures innate conductivity high as next-generation battery cathodes batteries.

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Bipolar redox active materials for electrochemical devices like redox flow batteries and lithium-ion batteries. The materials are derivatives of isatin, a natural compound, that exhibit reversible redox behavior in non-aqueous solvents. They can be used as bipolar redox materials in redox flow batteries or as redox shuttle additives in lithium-ion and other batteries to prevent overcharging and overdischarging. The bipolar redox behavior allows using the same isatin derivative compound as both the catholyte and anolyte in redox flow batteries, simplifying the design compared to using separate materials for each electrode.

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Lithiumrich manganesebased oxides (LRMOs) materials are considered to be the nextgeneration cathode for highenergy Liion/metal batteries owing their superior specific capacity, high operation voltage and low cost. However, commercial application of LRMOs is constrained by surface structure degradation lattice oxygen release, resulting in initial coulombic efficiency (ICE) rapid capacity decay. Herein, we propose a facile sorbic acidassisted treatment strategy construct homogeneous multifunctional interface layers composed layeredspinel heterogeneous vacancies on LRMOs, which enhance stability improve activity reversibility anionic redox reactions. The interfacial effectively suppress irreversible release alleviate unfavorable phase transformation. As consequence, treated displays improved ICE 88.3%, retention rate (87.9% at 1 C after 150 cycles) decay ratio (1.26 mV per cycle). These findings provide valuable new idea comprehensive electrochemical performance through multistrategy synergistic engineering techniques.

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Lithiumrich manganesebased oxides (LRMOs) materials are considered to be the nextgeneration cathode for highenergy Liion/metal batteries owing their superior specific capacity, high operation voltage and low cost. However, commercial application of LRMOs is constrained by surface structure degradation lattice oxygen release, resulting in initial coulombic efficiency (ICE) rapid capacity decay. Herein, we propose a facile sorbic acidassisted treatment strategy construct homogeneous multifunctional interface layers composed layeredspinel heterogeneous vacancies on LRMOs, which enhance stability improve activity reversibility anionic redox reactions. The interfacial effectively suppress irreversible release alleviate unfavorable phase transformation. As consequence, treated displays improved ICE 88.3%, retention rate (87.9% at 1 C after 150 cycles) decay ratio (1.26 mV per cycle). These findings provide valuable new idea comprehensive electrochemical performance through multistrategy synergistic engineering techniques.

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LiMn0.6Fe0.4PO4 is limited in practical applications due to its low electronic conductivity and slow Li+ diffusion rate. Therefore, Cu doping was applied modify LiMn0.6Fe0.4PO4, the mechanism of Cu2+ "three-function" synergistic enhancement cathode material performance explored. Compared undoped sample (LMFP), Cu-doped (LMFP-Cu 1%) exhibited significantly improved coefficient. First-principles calculations also confirmed high barrier LiMn0.6Fe0.4PO4@C. Additionally, LiMn0.6Fe0.39Cu0.01PO4@C demonstrated excellent rate cycling stability, with discharge capacities 160.3 mA h g-1 121.2 at 0.1 2C rates, respectively. After 200 cycles 1C rate, capacity retention 92.5%. The first principle calculation DFT can help show that introduction effectively reduce intrinsic Li+, situ XRD analysis revealed good structural stability reversibility. incorporation represents a promising approach improving lithium storage capabilities materials.

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Abstract Lithium-manganese-rich (LMR) oxides are regarded as one of the most promising cathode materials for next-generation batteries. However, their poor rate capability and performance degradation during cycling present significant challenges practical applications. Understanding how to optimize microscopic structures synthesis may provide critical insights enhancing performance. In this work, we investigated structural evolution solid-state sintering Li1.2Ni0.2Mn0.6O2 from Li-/Mn-/Ni-carbonate precursors. Combining X-ray diffraction transmission electron microscopy (TEM) techniques, observed nucleation a nanoscaled solid-solution phase at 550C, accompanied by secondary phases spinel-like, layered rocksalt. At 800C, relatively pure R3 m is formed. Notably, uncovered, first time, transition structure chemically separated two-phase when annealing sample 850C 900C. Atomic resolution scanning-TEM (STEM) imaging clearly distinguished C2/m phase, coherent grain boundary, confirmed STEM-energy-dispersion spectroscopy (STEM-EDS) mapping. Our calculations indicate that diffusion N... Read More

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Abstract The kinetics difference of sulfur reduction reaction (SRR) results in the shuttle effect issue lithiumsulfur (LiS) batteries, challenging their commercial use. electrocatalytic polysulfide conversion is regarded as a proactive strategy for suppressing such shuttling. Here, phase engineering proposed constructing highperformance crystal catalysts, using 2D TaTe 2 typical example to demonstrate rational catalyst design principle that urgent need developing right push forward practical use LiS batteries. Teenriched edges facilitate formation thinlayer LiTe x analogs, thereby accelerating ratedetermining step SRR, evidenced by activation energy from 0.96 0.76 eV. presence dynamic catalytic intermediates (LiTe ) and mitigation shuttle effect are confirmed through situ Raman spectroscopy. Consequently, catalyzed battery delivers an outstanding cycleability with low capacity degradation rate 0.035% per cycle over 1500 cycles at 2.0 C, even ultrahigh retention 94.9% 100 achieved pouch cell high areal loading 9.4 mg cm 2 .

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Covalent organic frameworks (COFs) have emerged as promising cathode materials for highperformance lithiumion batteries (LIBs) due to their welldefined topologies and tunable pore architectures. However, practical application is often limited by intrinsically sluggish charge transfer inferior reaction kinetics. To address these challenges, we develop an ionic quinolinelinked COF (iQCOF) via a onepot Povarov with triazole liquid. The iQCOF architecture achieves synergistic enhancement integrating bridgeinduced delocalization facilitate transport, the specific adsorption effect gain fast atmosphere dissociation rate, polar triazine units enable uniform ion flux stable interfaces. As result, delivers high capacity of 407 mAh g1 701 Wh kg1, exceptional rate capability (121 at 10 A g1) 0.0027% per cycle over 10000 cycles, further highlighting its potential cathode. This work provides convenient strategy advanced COFbased cathodes kinetics highrate performance, paving way nextgeneration energy storage technologies.

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Abstract Lithiumcarbon dioxide (LiCO 2 ) batteries have recently emerged as an innovative solution for energy storage and CO capture, storage, utilization. However, LiCO chemistry exhibits poor reversibility limited cycle life due to the cathode passivation caused by insulating discharge productLi 3 . Herein, a liquid metal (LM)based catalyst anchored on reduced graphene oxide (rGO@LM@Ru) is introduced mitigate thus enhance electrochemical performance of batteries. These findings indicate that LM plays critical role in improving charge transfer stabilizing Ru its surface. The rGO@LM@Ru offers low charge/discharge voltage gap 1.0 V, extended over 500 h, well enhanced capacity rate This work proposes novel design redox, which suggests promising application nextgeneration

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Mixing electroactive materials, solid-state electrolytes, and conductive carbon to fabricate composite electrodes is the most practiced but least understood process in all-solid-state batteries, which strongly dictates interfacial stability charge transport. We report on universal halide segregation at interfaces across various halogen-containing electrolytes a family of high-energy chalcogen cathodes enabled by mechanochemical reaction during ultrahigh-speed mixing. Bulk interface characterizations multimodal synchrotron x-ray probes cryotransmission electron microscopy show that situ segregated lithium layers substantially boost effective ion transport suppress volume change bulk cathodes. Various lithium-chalcogen cells demonstrate utilization close 100% extraordinary cycling commercial-level areal capacities.

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Lithium-ion (Li-ion) batteries that can be recharged, store energy in the form of chemical electrode materials, which may then converted into electrical when battery is discharged. A lot effort has been put improving performance via screening electroactive materials and assessing their structural integrity cycle reversibility. In order to effectively deal with issues like large volume variation, unstable interface, limited cyclability, rate capability, this chapter discusses recent advances oxide utilization for Li rechargeable both anode cathode, through nano-engineering active materials. Future research efforts will focus on enhancing materials stability, strength, cycle, various performances.

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Abstract ZnS batteries have garnered widespread attention in recent years due to their higher safety and low cost. However, challenges such as incomplete sulfur redox reactions the tendency of ZnS agglomerate impeded continued advancement highperformance batteries. Hollow hierarchical porous carbon spheres (HCs) are designed efficient hosts for The tailored HCs, featuring optimized shell thickness, porosity, facilitate uniform nanoZnS deposition, improve ion/electron transport, which revealed by situ impedance technology. This nano reactor design ensures highly reversible SZnS conversion, reducing internal polarization mitigating structural degradation. Electrochemical tests demonstrate outstanding cycling stability, with minimal capacity decay (0.068%) over 500 cycles, 463 mAh g 1 at 5 A . Finite element simulations further confirm effective stress dispersion preserving electrode integrity. work provides a promising strategy developing

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Abstract Fluoropolymers promise all-solid-state lithium metal batteries (ASLMBs) but suffer from two critical challenges. The first is the trade-off between ionic conductivity ( ) and anode reactions, closely related to high-content residual solvents. second, usually consciously overlooked, fluoropolymers inherent instability against alkaline anodes. Here, we propose indium-based metalorganic frameworks (In-MOFs) as a multifunctional promoter simultaneously address these challenges, using poly(vinylidene fluoridehexafluoropropylene) (PVH) typical fluoropolymer. In-MOF plays trio: (1) adsorbing converting free solvents into bonded states prevent their side reactions with anodes while retaining advantages on Li + transport; (2) forming inorganic-rich solid electrolyte interphase layers PVH reacting promote uniform deposition without dendrite growth; (3) reducing crystallinity promoting Li-salt dissociation. Therefore, resulting PVH/In-MOF (PVH-IM) showcases excellent electrochemical stability anodes, delivering 5550 h cycling at 0.2 mA cm 2 remarkable cumulative capacity... Read More

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Organic ionic plastic crystal (OIPC) materials exhibit soft solid phases within a specific temperature range, making them promising candidates for various electrochemical devices due to their intrinsic conductivity and stability. In this study, series of linear trispyrrolidinium salts with different alkyl side chain lengths counteranions were synthesized systematically characterized in terms structural, thermal, properties. Among the compounds, N,Nbis(4(Nundecylpyrrolidinium)butyl)pyrrolidinium trishexafluorophosphate (11PF6) exhibited two solidsolid phase transitions, low fusion entropy (Sf) 13 JK1mol1 at 210 C. Similarly, N,Nbis(4(Ndodecylpyrrolidinium)butyl)pyrrolidinium (12PF6) showed multiple transitions Sfof 18 206 The temperaturedependent crystalline 11PF6 identified as using polarized optical microscopy 1D wideangle Xray scattering (WAXS). was measured be 2.04106 Scm1 70 Upon blending 80 mol% LiTf2N, significantly increased 1.16104 Scm1. Electrochemical stability evaluated via sweep ... Read More

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ABSTRACT Highnickel ternary cathode (HNCM) materials are regarded as the primary choice for lithiumion batteries (LIBs) due to their high energy density. However, development is limited by lithiumnickel mixing, microcrack generation, and surface side reactions. Herein, a combined rolltoroll vacuum vapor deposition process used prepare LiNi 0.9 Co 0.05 Mn O 2 (NCM9055) material with dense, ultrathin, robust lithium fluoride (LiF) protective layer. Compared traditional methods, this approach allows precise control over thickness rate of deposited LiF layer, producing uniform layer that enhances stability. This not only effectively reduces direct contact between electrolyte electrode surface, mitigating corrosion reactions, but also strengthens structural integrity cathode, thereby significantly improving cycling The NCM9055 10 nm exhibits enhanced electrochemical performance, especially at cutoff voltages 4.3 4.5 V, excellent performance 1 C. Additionally, introduction improves thermal stability NCM9055, further enhancing safety highnickel batteries. study demonstr... Read More

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Lithium-ion battery cathode material with improved cycling life and capacity retention for electric vehicle applications. The cathode active material is a high nickel-manganese-cobalt oxide composition with a surface layer containing aluminum. The aluminum-doped surface layer improves cycling stability compared to uncoated high nickel cathodes. The aluminum content in the surface is 0.04-0.15 wt% of the total cathode material. The coated particles have median sizes of 3-15 um and surface layer thicknesses of 5-200 nm.

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