Chemical‐Mechanical Robustness of Single‐Crystalline Ni‐Rich Cathode Enabled by Surface Atomic Arrangement Control

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(22)

Опубликована: Апрель 1, 2023

Layered transition metal oxide cathodes have been one of the dominant for lithium-ion batteries with efficient Li+ intercalation chemistry. However, limited by weak layered interaction and unstable surface, mechanical chemical failure plagues their electrochemical performance, especially Ni-rich cathodes. Here, adopting a simultaneous elemental-structural atomic arrangement control based on intrinsic Ni-Co-Mn system, surface role is intensively investigated. Within invariant oxygen sublattice crystal, robust synergistic concentration gradient layered-spinel intertwined structure constructed model single-crystalline cathode. With strain dissipation erosion suppression, cathode exhibits an impressive capacity retention 82 % even at harsh 60 °C after 150 cycles 1 C. This work highlights coupling effect composition chemical-mechanical properties, concept will spur more researches that share same sublattice.

Язык: Английский

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In situ Interweaved Binder Framework Mitigating the Structural and Interphasial Degradations of High‐nickel Cathodes in Lithium‐ion Batteries

Angewandte Chemie International Edition, Год журнала: 2023, Номер 62(15)

Опубликована: Фев. 14, 2023

The practical viability of high-nickel layered oxide cathodes is compromised by the interphasial and structural degradations. Herein, we demonstrate that applying an in situ interweaved binder, cycling stability can be significantly improved. Specifically, results show resilient binder network immobilizes transition-metal ions, suppresses electrolyte oxidative decomposition, mitigates cathode particles pulverization, thus resulting suppressed cathode-to-anode chemical crossover ameliorated chemistry architecture electrode-electrolyte interphases. Pouch full cells with high-mass-loading LiNi0.8 Mn0.1 Co0.1 O2 achieve 0.02 % capacity decay per cycle at 1 C rate over 000 deep cycles 4.4 V (vs. graphite). This work demonstrates a rational compositional design strategy polymer binders to mitigate degradations high-Ni lithium-ion batteries.

Язык: Английский

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Ni-rich cathode materials for stable high-energy lithium-ion batteries

Nano Energy, Год журнала: 2024, Номер 126, С. 109620 - 109620

Опубликована: Апрель 18, 2024

The evolution of modern society demands sustainable rechargeable lithium-ion batteries (LIBs) with higher capacity and improved safety standards. High voltage Ni-rich layered transition metal oxides (i.e., LiNi1-x-yCoxMnyO2, NCM) have emerged as one the most promising cathode materials in meeting this demand. However, instability NCMs cathodes presents challenges large-scale commercialization. This review examines energy storage mechanism, e.g., possible (electro)chemical reactions, occurring at bulk surface degradation mechanism materials. To address challenging issue, we highlight recent advances strategies for engineering NCMs, including lattice, composition, microstructure engineering, electrolyte interfacial engineering. By addressing mechanisms improving overall stability, work sheds lights on potential avenues commercialization cathode-based high-performance LIBs.

Язык: Английский

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Factors Influencing Gas Evolution from High‐Nickel Layered Oxide Cathodes in Lithium‐Based Batteries

Advanced Energy Materials, Год журнала: 2024, Номер 14(8)

Опубликована: Янв. 26, 2024

Abstract Gas evolution from high‐nickel layered oxide cathodes (>90% Ni) remains a major issue for their practical application. Gaseous species, such as CO 2 , O and CO, that are evolved at high states of charge (SOC) worsen the overall safety batteries, pressure build‐up within cell may lead to rupture. Since these gasses produced during cathode degradation, tracking formation is also important in diagnosing failure. Online electrochemical mass spectrometry (OEMS) powerful situ technique study gas high‐voltage charge. However, differences OEMS experimental setups between different groups make it challenging compare results groups. In this perspective, various factors influence based on collected group presented. The focus conditions release, with particular emphasis reactive oxygen subsequent chemical reactions electrolyte. Promising strategies, electrolytes, compositional tuning, surface coatings effective suppressing highlighted. Critical insights into mitigating degradation provided guide development safer, high‐energy batteries.

Язык: Английский

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Recent progress and perspective on lithium metal battery with nickel-rich layered oxide cathode

eScience, Год журнала: 2024, Номер 4(6), С. 100265 - 100265

Опубликована: Март 24, 2024

The pairing of lithium metal anode (LMA) with Ni-rich layered oxide cathodes for constructing batteries (LMBs) to achieve energy density over 500 W h kg−1 receives significant attention from both industry and the scientific community. However, notorious problems are exposed in practical conditions, including lean electrolyte/capacity (E/C) ratio (<3 g (A h)−1), high cathode mass loading (>3 mA cm−2), low negative/positive (N/P) (<3), which creates a disparity between current performance LMBs desired requirements commercial applications. In review, we present summary recent achievements made understanding mechanistic degradation LMA, followed by strategies that utilized address these issues. We also consider detrimental issues cathodes. Furthermore, highlight progresses field coin/pouch cells stimulate further innovation. end, propose prospects development perspective LMBs.

Язык: Английский

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Multi-dimensional, Multi-scale Analysis of Interphase Chemistry for Enhanced Fast-Charging of Lithium-Ion Batteries with Ion Mass Spectrometry

Journal of the American Chemical Society, Год журнала: 2025, Номер unknown

Опубликована: Фев. 6, 2025

Understanding the fundamental properties of electrode–electrolyte interphases (EEIs) is essential for designing electrolytes that support stable operation under high charging rates. In this study, we benchmark our fast-charging electrolyte (FCE) against commercial LP57 to identify EEI characteristics enhance performance. By utilizing latest advances in time-of-flight secondary ion mass spectrometry (TOF-SIMS) and focused-ion beam (FIB) techniques, reveal complex chemical architecture cathode–electrolyte interphase (CEI). Our findings indicate battery conditions requires reduced surface reactivity rather than stabilizing bulk integrity cathode. While inorganic species are often cited as beneficial composition, their distribution within equally critical. Additionally, dynamic interactions between cathode material conductive carbon significantly affect CEI formation alter passivation layer chemistry. A chemically homogeneous components passivating preferentially active particles desired enhanced Notably, amount decomposition solid-electrolyte (SEI) far outweighs SEI determining better electrochemical An inorganic-rich effectively protects graphite particles, suppresses accumulation metallic lithium, prevents lithium dendrites. Overall, an performance can be achieved by tuning chemistry on both anode sides.

Язык: Английский

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Delineating the Roles of Mn, Al, and Co by Comparing Three Layered Oxide Cathodes with the Same Nickel Content of 70% for Lithium-Ion Batteries

Chemistry of Materials, Год журнала: 2022, Номер 34(2), С. 629 - 642

Опубликована: Янв. 10, 2022

High-nickel layered oxides continue to prevail in the energy storage market as frontmost cathode candidates for next-generation lithium-ion batteries. Demand and development of LiNi1–x–yMnxCoyO2 (NMC) LiNi1–x–yCoxAlyO2 (NCA) cathodes are rampantly increasing, particularly electric vehicle (EV) industry. However, continued presence cobalt NMC NCA raises global concerns due geopolitical ethical issues attributed Co sourcing. We herein introduce a novel cobalt-free, high-nickel LiNi0.7Mn0.25Al0.05O2 (NMA70) benchmark it against Co-containing LiNi0.7Mn0.15Co0.15O2 (NMC70) well Co- Al-free LiNi0.7Mn0.3O2 (NM70) with equivalent 70% Ni contents that all synthesized in-house. NMA70 displays high initial C/10 capacity 210 mA h g–1, matching NMC70 half cells cutoff voltage 4.5 V. also exhibits an impressive high-voltage full cell cycling performance 4.4 V nearly identical retention 83% compared 82% after 300 cycles. Postmortem X-ray photoelectron spectroscopy (XPS), high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM), loss (EELS) analyses indicate thinner cathode–electrolyte interface (CEI) developed NM70 unveil more robust solid-electrolyte (SEI) passivation on graphite anode among samples. The benefits Al doping additionally highlighted enhanced CEI thermal stabilities NMA70. This work assesses roles Mn, Al, demonstrate both practicality feasibility synthesizing promising alternatives current NMC- NCA-based cathodes.

Язык: Английский

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Ethylene Carbonate‐Free Electrolytes for Stable, Safer High‐Nickel Lithium‐Ion Batteries

Advanced Energy Materials, Год журнала: 2022, Номер 12(19)

Опубликована: Март 24, 2022

Abstract Ethylene carbonate (EC) is an important component in state‐of‐the‐art electrolytes for lithium‐ion batteries (LIBs). However, EC highly susceptible to oxidation on the surface of high‐nickel layered oxide cathodes, making it undesirable next‐generation high‐energy‐density LIBs. In this study, a simple, yet effective, EC‐free electrolyte (20F1.5M‐1TDI) presented by adding 20 wt% fluoroethylene (FEC) and 1 lithium 4,5‐dicyano‐2‐(trifluoromethyl)imidazole (LiTDI) into 1.5 m LiPF 6 ethyl methyl (EMC) electrolyte. The 20F1.5M‐1TDI found efficiently passivate graphite anode stabilize cathodes synergistic decomposition FEC LiTDI. LiNi 0.9 Mn 0.05 Al O 2 (NMA90)/graphite full cell with electrolyte, therefore, exhibits enhanced cycling stability suppressed voltage hysteresis growth compared that EC‐containing baseline (1 EC:EMC, 3:7 weight, vinyl carbonate). Advanced analytical tools, such as time‐of‐flight secondary ion mass spectrometry X‐ray photoelectron spectroscopy, are employed understand underlying working mechanism present study clearly showcases great potential straightforward, practical approach LIBs cathodes.

Язык: Английский

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High Nickel and No Cobalt─The Pursuit of Next-Generation Layered Oxide Cathodes

ACS Applied Materials & Interfaces, Год журнала: 2022, Номер 14(20), С. 23056 - 23065

Опубликована: Янв. 4, 2022

The prosperity of the electric vehicle industry is driving research and development lithium-ion batteries. As one core components in entire battery system, cathode materials are currently facing major challenges pushing a higher capacity up to materials' theoretical limits transitioning away from unaffordable metals. search for next-generation has shifted high-nickel cobalt-free cathodes meet these requirements. In this review, we distinctly point out shortcomings cobalt stabilizing layered structures systematically summarize recent efforts eliminate achieve nickel content materials. Finally, reasonable prospect put forward further other promising candidates, which likely spur wave toward developing high-performance low-cost Li-ion

Язык: Английский

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Probing the thermal degradation mechanism of polycrystalline and single-crystal Li(Ni0.8Co0.1Mn0.1)O2 cathodes from the perspective of oxygen vacancy diffusion

Energy storage materials, Год журнала: 2023, Номер 56, С. 495 - 505

Опубликована: Янв. 20, 2023

Язык: Английский

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