Title: Thin Film RuO ₂ Lithiation: Fast Lithium‐Ion Diffusion along the Interface

Abstract

Abstract Although lithium‐ion batteries that run on the conversion reaction have high capacity, their cyclability remains problematic due to large volume changes and material pulverization. Dimensional confinement, such as 2D thin film or nanodots in a conductive matrix, is proposed as a way of improving the cyclic stability, but the lithiation mechanism of such dimensionally controlled materials remains largely unknown. Here, by in situ transmission electron microscopy, lithiation of thin RuO ₂ films with different thicknesses and directions of lithium‐ion diffusion are observed at atomic resolution to monitor the reactions. From the side‐wall diffusion in ≈4 nm RuO ₂ film, the ion‐diffusion and reaction are fast, called “interface‐dominant” mode. In contrast, in ≈12 nm film, the ion diffusion–reaction only occurs at the interface where there is a high density of defects due to misfits between the film and substrate, called the “interface‐to‐film” mode. Compared to the side‐wall diffusion, the reaction along the normal direction of the thin film are found to be sluggish (“layer‐to‐layer” mode). Once lithiation speed is higher, the volume expansion is larger and the intercalation stage becomes shorter. Such observation of preferential lithiation direction in 2D‐like RuO ₂ thin film provides useful insights to develop dimensionally confinedmore » electrodes for lithium‐ion batteries.« less

Authors:

Kim, Sungkyu  ^[1];

• Search DOE PAGES for author "Kim, Sungkyu"
• Search DOE PAGES for ORCID "0000-0002-5371-6964"

Evmenenko, Guennadi ^[2]; Xu, Yaobin ^[3]; Buchholz, Donald Bruce ^[2]; Bedzyk, Michael  ^[2];

• Search DOE PAGES for author "Bedzyk, Michael"
• Search DOE PAGES for ORCID "0000-0002-1026-4558"

He, Kai ^[1]; Wu, Jinsong  ^[4];

• Search DOE PAGES for author "Wu, Jinsong"
• Search DOE PAGES for ORCID "0000-0002-7305-7927"

Dravid, Vinayak P.  ^[3]

• Search DOE PAGES for author "Dravid, Vinayak P."
• Search DOE PAGES for ORCID "0000-0002-6007-3063"

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+ Show Author Affiliations

1. Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA, NUANCE Center Northwestern University Evanston IL 60208 USA, Department of Materials Science and Engineering Clemson University Clemson SC 29634 USA
2. Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA
3. Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA, NUANCE Center Northwestern University Evanston IL 60208 USA
4. Department of Materials Science and Engineering Northwestern University Evanston IL 60208 USA, NUANCE Center Northwestern University Evanston IL 60208 USA, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing Nanostructure Research Centre Wuhan University of Technology Wuhan 430070 China

Publication Date:

Fri Nov 09 00:00:00 EST 2018

Sponsoring Org.:

USDOE

OSTI Identifier:

1481438

Grant/Contract Number:  

DEAC02‐06CH11357

Resource Type:

Publisher's Accepted Manuscript

Journal Name:

Advanced Functional Materials

Additional Journal Information:

Journal Name: Advanced Functional Materials Journal Volume: 28 Journal Issue: 52; Journal ID: ISSN 1616-301X

Publisher:

Wiley Blackwell (John Wiley & Sons)

Country of Publication:

Germany

Language:

English