Decoding Li~+/Na~+ Exchange Route Toward High-erformance Mn-Based Layered Cathodes for Li-Ion Batteries

Bo Cao; Zhefeng Chen; Hongbin CaoChen ZhuHongkai YangTianyi LiWenqian XuFeng PanMingjian Zhang

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Decoding Li~+/Na~+ Exchange Route Toward High-erformance Mn-Based Layered Cathodes for Li-Ion Batteries

机译：Decoding Li~+/Na~+ Exchange Route Toward High-erformance Mn-Based Layered Cathodes for Li-Ion Batteries

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Li~+/Na~+ exchange has been extensively explored as an effective method toprepare high-performance Mn-based layered cathodes for Li-ion batteries,since the first report in 1996 by P. G. Bruce (Nature, 1996. 381, 499–500).Understanding the detailed structural changes during the ion-exchangeprocess is crucial to implement the synthetic control of high-performancelayered Mn-based cathodes, but less studied. Herein, in situ synchrotronX-ray diffraction, density functional theory calculations, and electrochemicaltests are combined to conduct the systemic studies into the structuralchanges during the ion-exchange process of an Mn-only layered cathodeO3-type Li0.67[Li_(0.22)Mn_(0.78)]O_2 (LLMO) from the corresponding counterpartP3-type Na0.67[Li_(0.22)Mn_(0.78)]O_2 (NLMO). The temperature-resolved observationscombined with theoretical calculations reveal that the Li~+/Na~+ exchangeis favorable thermodynamically and composited with two tandem topotacticphase transitions: 1) from NLMO to a layered intermediate through ≈60% ofLi~+/Na~+ exchange. 2) then to the final layered product LLMO through furtherLi insertion. Moreover, the intermediate-dominate composite is obtained byslowing down the exchange kinetics below room temperature, showing betterelectrochemical performance than LLMO obtained by the traditional moltensaltmethod. The findings provide guides for the synthetic control of highperformanceMn-based cathodes under mild conditions.

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来源
《Advanced functional materials》 |2023年第20期|2214921.1-2214921.9|共9页
作者
Bo Cao; Zhefeng Chen; Hongbin CaoChen ZhuHongkai YangTianyi LiWenqian XuFeng PanMingjian Zhang;
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作者单位

School of Advanced MaterialsPeking University Shenzhen Graduate SchoolShenzhen 518055, China;

X-ray Science DivisionAdvanced Photon SourceArgonne National LaboratoryLemont, IL 60439, USA;

School of Science and EngineeringThe Chinese University of Hong KongShenzhen 518172, China;

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layered intermediate; Li~+/Na~+ ion-exchanges; lithium-ion batteries; Mn-based layered cathodes; two-step phase transformations;

Decoding Li~+/Na~+ Exchange Route Toward High-erformance Mn-Based Layered Cathodes for Li-Ion Batteries

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