Reversible Configurations of 3‐Coordinate and 4‐Coordinate Boron Stabilize Ultrahigh‐Ni Cathodes with Superior Cycling Stability for Practical Li‐Ion Batteries

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 30, 2024

Abstract Ultrahigh‐Ni layered oxide cathodes are the leading candidate for next‐generation high‐energy Li‐ion batteries owing to their cost‐effectiveness and ultrahigh capacity. However, increased Ni content causes larger volume variations worse lattice oxygen stability during cycling, resulting in capacity attenuation kinetics hysteresis. Herein, a Li 2 SiO 3 ‐coated Li(Ni 0.95 Co 0.04 Mn 0.01 ) 0.99 B O ultrahigh‐Ni cathode that well‐addresses all above issues, which is also first time realize real doping of ions demonstrated. The as‐obtained delivers reversible up 237.4 mAh g −1 (924 Wh kg superior retention 84.2% after 500 cycles at 1C pouch‐type full‐cells. Advanced characterizations calculations verify boron‐doping existed terms 3‐coordinate 4‐coordinate configurations high electrochemical reversibility de‐/lithiation, greatly stabilizes anions impedes Ni‐ion migration layer. Furthermore, B‐doping engineers primary particle microstructure better relaxing strain accelerating diffusion. This work advances energy density materials into domain 900 , concept will inspire more intensive study on cathodes.

Language: Английский

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Compositional Gradient Design of Ni-Rich Co-Poor Cathodes Enhanced Cyclability and Safety in High-Voltage Li-Ion Batteries

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 20, 2025

Developing cost-effective high-voltage Ni-rich cathodes has reached a consensus to replace conventional ultrahigh Ni counterparts for high-energy Li-ion batteries, but more rigorous requirements are put forward their mechanical and chemical stability. Herein, we report the design synthesis of full concentration gradient LiNi0.75Mn0.20Co0.05O2 cathode with Mn-rich Ni-poor surface, which been realized by in situ forming PO43- distribution retard transition-metal ions' interdiffusion during high-temperature lithiation process. This mitigates stress at source high morphological integrity refrains lattice oxygen loss under 4.5 V operation. After Li0.1B0.967PO4 is coated, surface parasitic reactions further ameliorated stable interface chemistry. The resultant deliver reversible capacity as 212.6 mAh g-1 2.7-4.5 an energy density >800 Wh kg-1cathode, almost equivalent state-of-the-art Ni-content 90% 2.7-4.3 V. In commercial-grade cells, superior cycle life 80.5% retention achieved 1C within after 1700 cycles, exhibiting promising opportunities compositional cathodes.

Language: Английский

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In Situ Interphasial Engineering Enabling High‐Rate and Long‐Cycling Li Metal Batteries

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: June 10, 2024

Abstract The practical implementation of Li metal anode has long been hindered by the significant challenges notorious dendritic growth and severe interphase instability during repeated cycling. Herein, a highly lithiophilic NiSe‐modified host rationally constructed to stabilize facile mechanical rolling strategy. in situ configurated high‐flux 2 Se‐enriched layer can facilitate fast interfacial charge transfer, high plating/stripping reversibility homogeneous nucleation/growth. Consequently, achieved modified demonstrates ultrahigh rate capability (10 mA cm −2 ) ultralong‐term cycling stability (6600 cycles) with dendrite‐free deposition. Li|LiFePO 4 (LFP) cell exhibits an extraordinarily lifespan over 500 cycles ultra‐low decay only ≈0.0092% per cycle at 1 C. Furthermore, 4.5 V high‐voltage Li|LiCoO pouch areal capacity (≈1.9 mAh still reveals impressively prolonged cyclability 200 even under harsh test condition low negative‐to‐positive‐capacity (N/P) ratio ≈3.4 lean electrolyte ≈5.5 µL −1 . This work provides scalable strategy toward stable for reliable usage.

Language: Английский

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Electrochemical reactivity of PZT materials in Li-ion and Na-ion batteries

Discover Electrochemistry., Journal Year: 2025, Volume and Issue: 2(1)

Published: March 31, 2025

Language: Английский

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Electrochemical Self‐Assembly of Boron‐Based Cathode‐Electrolyte Interphase to Stabilize 4.65 V LiCoO₂

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 26, 2025

Abstract The cathode‐electrolyte interphase (CEI) is vital for the stability of LiCoO 2 (LCO) beyond 4.55 V (vs Li/Li + ). Herein, full coverage boron‐based CEI achieved on LCO surface via utilizing self‐wetting synthesis boric acid (i.e., B‐LCO), accompanying with subsequent electrochemical self‐assembly process upon cycles. Initially, B‐LCO coated borate deposits (size 10–20 nm), then it melts and fully covers sintering, leading to artificial CEI, which directly reduces side reactions induced by highly oxidative Co 4+ /O n− (0 < n 2). Significantly, during cycling, in situ interfacial between species LiF promote formation crystalline LiB 6 O 9 F components, showing mechanically robust Li conductive characteristics. Due synergism structurally tough rocksalt (RS) phase, not only more reversible phase transition uniform (de)lithiation are achieved, but also particle cracks deterioration issues effectively inhibited. As a result, B‐LCO||Li cells show excellent cycle stability, high retention 84.0% 500 cycles 3–4.65 V.

Language: Английский

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High Rate Performance of Single‐Crystalline NCM Upcycled from Spent Lithium‐Ion Batteries Via Direct Recovery and Modification

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Dec. 17, 2024

Abstract The global expansion of spent lithium‐ion batteries (LIBs) presents both an urgent environmental issue and a significant economic opportunity, driving the development diverse recycling processes worldwide. Direct regeneration is promising method for recovering materials from LIBs. However, most existing direct methods focus solely on cathodes without addressing further improvements in their performance. Herein, reported to upcycle single‐crystalline lithium nickel manganese cobalt oxides (NCM) polycrystalline NCM based facile phosphoric acid etching approach. Moreover, Li 3 PO 4 coating 3− polyanion doping are simultaneously achieved surface single‐crystal during upcycling process. enlarged lattice spacing fast ionic conductor layer enhance + diffusion mitigate phase transformations delithiation/lithiation. Benefiting synergistic effect single crystal structure modification, upcycled LiNi 0.65 Co 0.2 Mn 0.15 O 2 demonstrates excellent electrochemical performances, including large reversible capacity (≈186 mAh g −1 at 0.1C), high‐rate capability (≈142 10C), cycling stability (≈99% retention 100 cycles). This approach provides novel effective pathway transform LIBs into value‐added cathode materials, achieving win–win situation protection resource conservation.

Language: Английский

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Unraveling Inherent Degradation Mechanism of Electrolyte at High-Voltage and the d2sp3 Hybridization Strategy for Non-Flammable 4.8 V LiCoO2 Battery

Published: Jan. 1, 2025

The potential risk of transition metal (TM) ion dissolution is a prevalent issue in nearly all layered oxide cathodes. While the detrimental effects this are widely discussed context cathode material design, implications for electrolyte design receive comparatively less attention. In fact, severe decomposition frequently occurs after TM ions. This phenomenon typically attributed to catalytic However, there lack research that clearly explains destabilization electrolyte. study delves into different interface behaviors between Co3+ and Li+. Near anode surface, significant proportion solvent molecules PF6- ions escape from Li+ solvation sheath, with only small portion contributing formation electrode/electrolyte interface. Subsequently, free reduced, interpolated or deposited anode. contrast, exhibit stronger binding ability than ions, leading challenges desolvation. sheaths demonstrate reduction instability, trapped must be reduced. order mitigate hazard dissolution, fluorinated cathode/electrolyte was applied inhibit Isobutyronitrile (IBN) used capture harmful electrolyte, resulting d2sp3 hybrid orbitals when IBN combines Co3+. stable chelated complex effectively eliminated associated sheaths. developed through hybridization strategy addresses dissolved Co, even 0.1M Co intentionally added LCO batteries utilizing an impressive increase capacity retention, rising 56.6% 84.5% 300 cycles at 4.7 V. Additionally, retention battery 73.3% 200 4.8

Language: Английский

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Enhanced electrochemical properties of hard carbon anode derived from phenolic resin modified via an oxygen-induced plasma surface treatment for lithium-ion batteries

Surfaces and Interfaces, Journal Year: 2025, Volume and Issue: unknown, P. 106282 - 106282

Published: March 1, 2025

Language: Английский

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Research progress on cathode materials for lithium-ion batteries

Journal of Solid State Electrochemistry, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Language: Английский

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Enhanced Structural Stability of Single-Crystalline Ni-Rich Cathode Enables Improved Cyclability in Pouch Cells

ACS Nano, Journal Year: 2025, Volume and Issue: unknown

Published: April 4, 2025

Single-crystalline LiNi0.9Co0.05Mn0.05O2 (SCNCM90) cathode materials experience continuous capacity degradation during cycling, primarily due to irreversible structural transformations and oxygen loss. These alterations are driven by the local adjustment of in-layer interlayer transition metal ions as a result anionic cationic redox reactions. In this study, selenium (Se) titanium (Ti) were simultaneously incorporated into SCNCM90 structure enhance stability, inhibit reactions lattice oxygen, mitigate severe internal strain induced phase near end charge. Moreover, Se/Ti regulation in reduces Li+ migration barrier, suppresses Li/Ni cation mixing further stabilizes SCNCM90. The formation O-transition -Se bonds deep charging can reduce outward Oα- (α < 2) increase vacancy energy, thereby improving stability processes within Ti4+ promotes nanoscale mixed-phase layer on surface SCNCM90, enhancing reversibility H2-H3 transition. Additionally, alleviation enhanced significantly contribute long-term cyclic cathodes. Hence, modification material achieves retention 87.6% after 500 cycles at 1 C with 2.8-4.5 V, compared only 61.4% for undoped cathode. A 2.83 Ah pouch cell SCNCM90-0.6ST||graphite electrodes demonstrates long cycle life over cycles, 3.1% loss 3-4.25 V. This work reveals that mitigation particle cracking suppression release crucial improvements Ni-rich layered materials.

Language: Английский

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