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Title: Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes

Abstract

High gravimetric/volumetric capacity and low working potential make Si as one of the ideal candidate anode materials for lithium ion batteries. However, the large volume change of Si upon lithiation/delithiation poses a critical challenge for stable battery operations. Here, we introduce a novel designing concept, which takes advantage of such a deformation and ensures the structural stability of the material by developing a 2D Si nanosheet coated with a thin carbon layer (2DSi@C). Upon electrochemical cycling, this 2DSi@C exhibits unique deformation patterns, featuring accommodation of deformation in the thickness direction upon lithiation, while forming ripples upon delithiation, as consistently demonstrated by in-situ TEM observation and chemomechanical simulation. The ripple formation presents a unique mechanism for releasing the cycling induced stress, rendering the 2DSi@C chemomechanically much more stable and durable than the bare 2DSi counterparts. This work demonstrates a general principle as how to take the advantage of the large deformation materials for designing high capacity electrode.

Authors:
ORCiD logo [1]; ORCiD logo [2];  [1];  [1];  [1];  [1]; ORCiD logo [3];  [1];  [1]; ORCiD logo [3];  [2]; ORCiD logo [1]
  1. Ulsan National Inst. of Science and Technology (UNIST), Ulsan (Republic of Korea)
  2. Pennsylvania State Univ., University Park, PA (United States)
  3. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Publication Date:
Research Org.:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
OSTI Identifier:
1578272
Report Number(s):
PNNL-SA-132988
Journal ID: ISSN 2041-1723
Grant/Contract Number:  
AC05-76RL01830; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE

Citation Formats

Ryu, Jaegeon, Chen, Tianwu, Bok, Taesoo, Song, Gyujin, Ma, Jiyoung, Hwang, Chihyun, Luo, Langli, Song, Hyun -Kon, Cho, Jaephil, Wang, Chongmin, Zhang, Sulin, and Park, Soojin. Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes. United States: N. p., 2018. Web. doi:10.1038/s41467-018-05398-9.
Ryu, Jaegeon, Chen, Tianwu, Bok, Taesoo, Song, Gyujin, Ma, Jiyoung, Hwang, Chihyun, Luo, Langli, Song, Hyun -Kon, Cho, Jaephil, Wang, Chongmin, Zhang, Sulin, & Park, Soojin. Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes. United States. doi:10.1038/s41467-018-05398-9.
Ryu, Jaegeon, Chen, Tianwu, Bok, Taesoo, Song, Gyujin, Ma, Jiyoung, Hwang, Chihyun, Luo, Langli, Song, Hyun -Kon, Cho, Jaephil, Wang, Chongmin, Zhang, Sulin, and Park, Soojin. Thu . "Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes". United States. doi:10.1038/s41467-018-05398-9. https://www.osti.gov/servlets/purl/1578272.
@article{osti_1578272,
title = {Mechanical mismatch-driven rippling in carbon-coated silicon sheets for stress-resilient battery anodes},
author = {Ryu, Jaegeon and Chen, Tianwu and Bok, Taesoo and Song, Gyujin and Ma, Jiyoung and Hwang, Chihyun and Luo, Langli and Song, Hyun -Kon and Cho, Jaephil and Wang, Chongmin and Zhang, Sulin and Park, Soojin},
abstractNote = {High gravimetric/volumetric capacity and low working potential make Si as one of the ideal candidate anode materials for lithium ion batteries. However, the large volume change of Si upon lithiation/delithiation poses a critical challenge for stable battery operations. Here, we introduce a novel designing concept, which takes advantage of such a deformation and ensures the structural stability of the material by developing a 2D Si nanosheet coated with a thin carbon layer (2DSi@C). Upon electrochemical cycling, this 2DSi@C exhibits unique deformation patterns, featuring accommodation of deformation in the thickness direction upon lithiation, while forming ripples upon delithiation, as consistently demonstrated by in-situ TEM observation and chemomechanical simulation. The ripple formation presents a unique mechanism for releasing the cycling induced stress, rendering the 2DSi@C chemomechanically much more stable and durable than the bare 2DSi counterparts. This work demonstrates a general principle as how to take the advantage of the large deformation materials for designing high capacity electrode.},
doi = {10.1038/s41467-018-05398-9},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {7}
}

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