Closed‐Loop Direct Upcycling of Spent Ni‐Rich Layered Cathodes into High‐Voltage Cathode Materials

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

Published: July 15, 2024

Abstract Facing the resource and environmental pressures brought by retiring wave of lithium‐ion batteries (LIBs), direct recycling methods are considered to be next generation's solution. However, contradiction between limited battery life demand for rapidly iterating technology forces recovery paradigm shift toward “direct upcycling.” Herein, a closed‐loop upcycling strategy that converts waste current collector debris into dopants is proposed, highly inclusive eutectic molten salt system utilized repair structural defects in degraded polycrystalline LiNi 0.83 Co 0.12 Mn 0.05 O 2 cathodes while achieving single‐crystallization transformation introducing Al/Cu dual‐doping. Upcycled materials can effectively overcome two key challenges at high voltages: strain accumulation lattice oxygen evolution. It exhibits comprehensive electrochemical performance far superior commercial 4.6 V, especially its fast charging capability 15 C, an impressive 91.1% capacity retention after 200 cycles 1.2 Ah pouch cell. Importantly, this approach demonstrates broad applicability various spent layered cathodes, particularly showcasing value mixed cathodes. This work bridges gap management material enhancement, offering sustainable path LIBs production next‐generation high‐voltage

Language: Английский

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Unraveling Mechanism for Microstructure Engineering toward High‐Capacity Nickel‐Rich Cathode Materials

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

Published: June 17, 2024

Abstract Microstructural engineering on nickel‐rich layered oxide (NRLO) cathode materials is considered a promising approach to increase both the capacity and lifespan of lithium‐ion batteries by introducing high valence‐state elements. However, rational regulation NRLO microstructures based deep understanding its enhancement mechanism remains challenging. Herein for first time, it demonstrated that an 14 mAh g −1 in reversible at cycle can be achieved via tailoring micro nano structure through tungsten. Aberration‐corrected scanning transmission electron microscopy (STEM) characterization reveals formation modified microstructure featured as coherent spinel twin boundaries. Theoretical modeling electrochemical investigations further demonstrate related such boundaries, which lower Li + diffusion barrier thus allow more participate deeper phase transitions. Meanwhile, surface grain boundaries NRLOs are found generating dense uniform LiW x O y phase, extends life reducing side reactions with electrolytes. This work enables comprehensive capacity‐increased endows remarkable potential microstructural capacity‐ lifespan‐increased NRLOs.

Language: Английский

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Restraining Lattice Oxygen Escape by Bioinspired Antioxidant Enables Thermal Runaway Prevention in Ni−Rich Cathode Based Lithium−Ion Batteries

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(31)

Published: May 21, 2024

Abstract Ni−rich cathodes are hopeful materials for advanced lithium−ion batteries (LIBs) due to high capacity. Nonetheless, the chemical crosstalk triggered by reactive oxygen (O * ) represents a critical factor in thermal runaway (TR). Currently, there few effective means prevent this parasitic reaction. Here, inspired O scavenging effect of β−carotene living organisms, it is innovatively identified that can impede TR restraining escape during decomposition nickel−rich cathodes. Using LiNi 0.6 Co 0.2 Mn 2 as model and extending higher nickel content (LiNi 0.8 0.1 , 0.9 0.05 ), demonstrated undergo an situ copolymerization reaction trapping thereby attenuating crosstalk. Additionally, generated copolymer also adjust band center 2p orbitals delithiated cathode, alleviating charge compensation behavior anions, thus delaying phase transition charged . As result, trigger temperature NCM811∣Graphite pouch cell increased from 131.0 195.0 °C maximum reduced 657.8 412.4 °C. This work introduces new simple strategy designing functional additives block TR, offering promising avenue advancing safety LIBs.

Language: Английский

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Enhancing Chemomechanical Stability and High-Rate Performance of Nickel-Rich Cathodes for Lithium-Ion Batteries through Three-in-One Modification

Energy storage materials, Journal Year: 2024, Volume and Issue: 74, P. 103893 - 103893

Published: Nov. 6, 2024

Language: Английский

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Revolutionizing multifunctional electrolyte additive design and synthesis for high-voltage nickel-rich batteries in diverse climates

Energy storage materials, Journal Year: 2024, Volume and Issue: 71, P. 103642 - 103642

Published: July 14, 2024

Language: Английский

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Promoting Layered Oxide Cathodes Based on Structural Reconstruction for Sodium‐Ion Batteries: Reversible Phase Transition, Stable Interface Regulation, and Multifunctional Intergrowth Structure

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

Published: Oct. 21, 2024

Abstract Layered transition‐metal oxides (Na x TMO 2 ) are one of the most promising cathode materials for sodium‐ion batteries due to their high theoretical specific capacities, good conductivity, and environmental friendliness. However, several key scientific issues Na still persist in practical applications: i) complex phase transitions during charge/discharge process owing slip layer; ii) tendency interface react with electrolyte, resulting structure degradation, iii) reactions between active H O as well CO on exposure air environment form alkaline substances surface. To understand electrochemical storage mechanisms solve these problems, modification strategies have been reported recently, including bulk doping, concentration gradient design, regulation, intergrowth construction. This review focuses reversible transitions, stable multifunctional material from inside outside. The future research directions also analyzed, providing guidance development commercial layered next‐generation energy systems.

Language: Английский

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Layered/Olivine Composite Structure-Induced Stable Gradient Interfacial Chemistry toward High-Temperature Lithium-Ion Batteries

ACS Nano, Journal Year: 2024, Volume and Issue: 18(46), P. 32065 - 32076

Published: Nov. 5, 2024

The state-of-the-art layered oxide as the cathode material for lithium-ion batteries has attracted wide attention; however, harsh operations of high-energy and high-safety energy-storage technology at high temperature is challenging owing to aggravated structural instability parasitic reactions cathodes. Herein, layered/olivine composite structure architecture designed grain surface govern constant electrochemistry in a environment, gradient LiF interlayer developed onto cathodes suppress interfacial degradation. By combination interfacial-sensitive characterizations theoretical analysis cathode/interface, formation mechanism this special interphase induced by revealed. could deliver an excellent high-temperature cycling stability with 90.8% retention 300 cycles half cell 95.6% 1000 pouch simultaneously enhances ∼51% thermal stability, which broadens approaches developing high-stable that work extreme environments.

Language: Английский

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Enhancing the cycling stability of full-concentration-gradient Ni-rich layered cathodes via in-situ Zr doping

Chemical Engineering Journal, Journal Year: 2024, Volume and Issue: 493, P. 152872 - 152872

Published: June 5, 2024

Language: Английский

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Low-Temperature Synthesis of Amorphous Lif/Li3bo3 Interfaces with F, B Co-Doped Subsurface for Long-Cycling and High-Rate Ni-Rich Cathodes

Published: Jan. 1, 2025

Language: Английский

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Surface Engineering Enabling Efficient Upcycling of Highly Degraded Layered Cathodes

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

Published: March 6, 2025

Direct recycling of cathode materials has attracted phenomenal attention due to its economic and eco-friendly advantages. However, existing direct technologies are difficult apply highly degraded layered as the accumulation thick rock-salt phases on their surfaces not only blocks lithiation channels but also is thermodynamically transform into phases. Here, a surface engineering-assisted upcycling strategy that reactivates lithium diffusion at using acid etching explored. Acid can selectively remove electrochemically inert while simultaneously dissociating polycrystalline structure single crystals, thereby reducing thermodynamic barrier relithiation process enhancing stability regenerated cathode. This restore capacity LiNi0.5Co0.2Mn0.3O2 from 59.7 165.4 mAh g-1, comparable commercialized ones. The exhibits excellent electrochemical with retention 80.1% 1 C after 500 cycles within 3.0-4.2 V (vs graphite) in pouch-type full cells. In addition, generality this been validated Ni-rich LiCoO2. work presents promising approach for materials.

Language: Английский

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