Research progress in failure mechanisms and electrolyte modification of <scp>high‐voltage</scp> nickel‐rich layered oxide‐based lithium metal batteries

Liu, Jiandong; Hu, Xinhong; Qi, Shihan; Ren, Yurong; Li, Yong; Ma, Jianmin

doi:10.1002/inf2.12507

Cited by 11 publications

(1 citation statement)

References 108 publications

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“…The studies of clean new energy represent a crucial avenue for realizing the dual-carbon strategy. , Lithium (Li) can be effectively used in lithium–metal batteries (LMBs) for high-density energy storage owing to its high theoretical specific capacity (3860 mAh g –1 ) and low electrochemical potential [−3.04 V vs standard hydrogen electrode (SHE)]. − Apart from inherent safety concerns (flammable and explosive), liquid organic electrolyte-based LMBs suffer from issues such as uneven lithium deposition, a fragile and unstable Li/electrolyte interface leading to dendrite growth, membrane penetration, and low battery lifespan, , which impede the practical application of LMBs. Although strategies such as the careful selection of additives in electrolyte, coating technique for surface construction, and rational design of three-dimensional current collectors can protect the Li anode of liquid electrolyte-based LMBs, the inherent instability and safety concerns of the Li/electrolyte interface owing to liquid electrolytes have not been fundamentally addressed. Hence, the demand for electrochemical energy storage with intrinsic safety has propelled academic and industrial research toward solid electrolyte-based LMBs …”

Section: Introductionmentioning

confidence: 99%

In Situ Polymerized Quasi-Solid Electrolytes Compounded with Ionic Liquid Empowering Long-Life Cycling of 4.45 V Lithium–Metal Battery

Ma,

Zhang,

Tang

et al. 2024

ACS Appl. Mater. Interfaces

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High-voltage resistant quasi-solid-state polymer electrolytes (QSPEs) are promising for enhancing the energy density of lithium−metal batteries in practice. However, side reactions occurring at the interfaces between the anodes or cathodes and QSPEs considerably reduce the lifespan of highvoltage LMBs. In this study, a copolymer of vinyl ethylene carbonate (VEC) and poly(ethylene glycol) diacrylate (PEGDA) was used as the framework, with a cellulose membrane (CE) as the supporting layer. Based on density functional theory calculations, 1butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (Pyr 14 TFSI), an ionic liquid, was screened because of its lowest unoccupied molecular orbital energy level as a modifying agent for the in situ P(VEC x -EG y )/Pyr z /LiTFSI@CE QSPEs synthesis. Pyr 14 + , with a lithiophobic alkyl chain, forms a dense positive ion shielding layer on the protruding tips of deposited lithium, facilitating uniform and smooth lithium deposition. Pyr 14 TFSI assists in constructing a stable solid electrolyte interphase (SEI) layer on the Li surface enriched with LiF, Li 3 N, and RCOOLi. The modulation of lithium deposition behavior on the anode by Pyr 14 TFSI ensures stable Li plating/stripping for >1500 h. A Li−Cu cell exhibits stable cycling for >200 cycles at a current density of 0.05 mA cm −2 , with an average Coulombic efficiency of 92.7%. In situ polymerization ensures that P(VEC x -EG y )/Pyr z /LiTFSI@CE QSPEs exhibit excellent interface compatibility with the anode and the cathode. The CR2032 button cell Li|P(VEC 1 -EG 0.06 )/Pyr 0.4 / LiTFSI@CE|LiCoO 2 demonstrates stable cycling with a negligible capacity decay of 0.083% per cycle for >390 cycles at 25 °C and 0.2 C when using a high-voltage LiCoO 2 (4.45 V) cathode. Furthermore, a 7.1 mAh pouch cell achieves stable charge−discharge cycles, confirming the pronounced stability of the as-fabricated QSPE at the interfaces of the high-voltage LiCoO 2 cathode and Li anode.

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Section: Introductionmentioning

confidence: 99%

In Situ Polymerized Quasi-Solid Electrolytes Compounded with Ionic Liquid Empowering Long-Life Cycling of 4.45 V Lithium–Metal Battery

Ma,

Zhang,

Tang

et al. 2024

ACS Appl. Mater. Interfaces

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Vacancy Remediation in Prussian Blue Analogs for High‐Performance Sodium and Potassium Ion Batteries

Wu,

Ren,

Wang

et al. 2024

Adv Funct Materials

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Sodium‐ion batteries (SIBs) and potassium‐ion batteries (PIBs) have enormous potential for large‐scale energy storage due to their cost‐effectiveness, safety, and environmental compatibility. Developing high‐capacity and highly reliable cathode materials is key to advancing the commercialization of SIBs and PIBs. Low‐cost Prussian blue analogs (PBAs), with their open 3D framework and ease of synthesis, are preferred cathode materials for energy storage applications. However, the unique growth mechanism of PBAs introduces numerous Fe(CN)6 vacancies, which compromise structural integrity and result in capacity decay due to structural collapse during long‐term electrochemical cycling. Additionally, cracking can cause the dissolution of transition metal (TM) ions, undesirable interfacial reactions, and gas generation, which shorten the battery's lifespan and raise safety concerns. In this review, the mechanisms of growth and vacancy formation in PBAs is first clarified, providing a comprehensive overview of current strategies for vacancy remediation based on both bottom‐up and top‐down approaches. It is then elucidate how optimized vacancy remediation mechanisms can enhance lattice and interfacial stability, suppress TM dissolution and mitigate gas generation. Finally, it is discussed future research directions and provide perspectives on the further development of high‐performance cathode materials for SIBs and PIBs.

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In situ evaluation and manipulation of lithium plating morphology enabling safe and long‐life lithium‐ion batteries

Mao,

Wang,

et al. 2024

InfoMat

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The morphology of plated lithium (MPL) metal on graphite anodes, traditionally described as “moss‐like” and “dendrite‐like”, exert a substantial negative influence on the performance of lithium‐ion batteries (LIBs) by modulating the metal‐electrolyte interface and side reaction rates. However, a systematic and quantitative analysis of MPL is lacking, impeding effective evaluation and manipulation of this detrimental issue. In this study, we transition from a qualitative analysis to a quantitative one by conducting a detailed examination of the MPL. Our findings reveal that slender lithium dendrites reduces the lifespan and safety of LIB by increasing the side reaction rates and promoting the formation of dead lithium. To further evaluate the extent of the detrimental effect of MPL, we propose the specific surface area (SSA) as a critical metric, and develop an in situ method integrating expansion force and electrochemical impedance spectroscopy to estimate SSA. Finally, we introduce a pulse current protocol to manipulate hazardous MLP. Phase field model simulations and experiments demonstrate that this protocol significantly enhances the reversibility of plated lithium. This research offers a novel morphological perspective on lithium plating, providing a more detailed fundamental understanding that facilitates effective evaluation and manipulation of plated lithium, thereby enhancing the safety and extending the cycle life of LIBs.image

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Research progress in failure mechanisms and electrolyte modification of high‐voltage nickel‐rich layered oxide‐based lithium metal batteries

Cited by 11 publications

References 108 publications

In Situ Polymerized Quasi-Solid Electrolytes Compounded with Ionic Liquid Empowering Long-Life Cycling of 4.45 V Lithium–Metal Battery

In Situ Polymerized Quasi-Solid Electrolytes Compounded with Ionic Liquid Empowering Long-Life Cycling of 4.45 V Lithium–Metal Battery

Vacancy Remediation in Prussian Blue Analogs for High‐Performance Sodium and Potassium Ion Batteries

In situ evaluation and manipulation of lithium plating morphology enabling safe and long‐life lithium‐ion batteries

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