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Title: Shell-Protective Secondary Silicon Nanostructures as Pressure-Resistant High-Volumetric-Capacity Anodes for Lithium-Ion Batteries

Abstract

Here, the nanostructure design of a prereserved hollow space to accommodate 300% volume change of silicon anodes has created exciting promises for high-energy batteries. However, challenges with weak mechanical stability during the calendering process of electrode fabrication and poor volumetric energy density remain to be solved. Here we fabricated a pressure-resistant silicon structure by designing a dense silicon shell coating on secondary micrometer particles, each consisting of many silicon nanoparticles. The silicon skin layer significantly improves mechanical stability, while the inner porous structure efficiently accommodates the volume expansion. Such a structure can resist a high pressure of over 100 MPa and is well-maintained after the calendering process, demonstrating a high volumetric capacity of 2041 mAh cm–3. In addition, the dense silicon shell decreases the surface area and thus increases the initial Coulombic efficiency. With further encapsulation with a graphene cage, which allows the silicon core to expand within the cage while retaining electrical contact, the silicon hollow structure exhibits a high initial Coulombic efficiency and fast rise of later Coulombic efficiencies to >99.5% and superior stability in a full-cell battery.

Authors:
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
OSTI Identifier:
1490980
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 18; Journal Issue: 11; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; calendering; high-volumetric capacity; lithium-ion batteries; pressure-resistant; shell-protective; Silicon

Citation Formats

Wang, Jiangyan, Liao, Lei, Li, Yuzhang, Zhao, Jie, Shi, Feifei, Yan, Kai, Pei, Allen, Chen, Guangxu, Li, Guodong, Lu, Zhiyi, and Cui, Yi. Shell-Protective Secondary Silicon Nanostructures as Pressure-Resistant High-Volumetric-Capacity Anodes for Lithium-Ion Batteries. United States: N. p., 2018. Web. doi:10.1021/acs.nanolett.8b03065.
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Wang, Jiangyan, Liao, Lei, Li, Yuzhang, Zhao, Jie, Shi, Feifei, Yan, Kai, Pei, Allen, Chen, Guangxu, Li, Guodong, Lu, Zhiyi, & Cui, Yi. Shell-Protective Secondary Silicon Nanostructures as Pressure-Resistant High-Volumetric-Capacity Anodes for Lithium-Ion Batteries. United States. https://doi.org/10.1021/acs.nanolett.8b03065
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Wang, Jiangyan, Liao, Lei, Li, Yuzhang, Zhao, Jie, Shi, Feifei, Yan, Kai, Pei, Allen, Chen, Guangxu, Li, Guodong, Lu, Zhiyi, and Cui, Yi. Fri . "Shell-Protective Secondary Silicon Nanostructures as Pressure-Resistant High-Volumetric-Capacity Anodes for Lithium-Ion Batteries". United States. https://doi.org/10.1021/acs.nanolett.8b03065. https://www.osti.gov/servlets/purl/1490980.
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@article{osti_1490980,
title = {Shell-Protective Secondary Silicon Nanostructures as Pressure-Resistant High-Volumetric-Capacity Anodes for Lithium-Ion Batteries},
author = {Wang, Jiangyan and Liao, Lei and Li, Yuzhang and Zhao, Jie and Shi, Feifei and Yan, Kai and Pei, Allen and Chen, Guangxu and Li, Guodong and Lu, Zhiyi and Cui, Yi},
abstractNote = {Here, the nanostructure design of a prereserved hollow space to accommodate 300% volume change of silicon anodes has created exciting promises for high-energy batteries. However, challenges with weak mechanical stability during the calendering process of electrode fabrication and poor volumetric energy density remain to be solved. Here we fabricated a pressure-resistant silicon structure by designing a dense silicon shell coating on secondary micrometer particles, each consisting of many silicon nanoparticles. The silicon skin layer significantly improves mechanical stability, while the inner porous structure efficiently accommodates the volume expansion. Such a structure can resist a high pressure of over 100 MPa and is well-maintained after the calendering process, demonstrating a high volumetric capacity of 2041 mAh cm–3. In addition, the dense silicon shell decreases the surface area and thus increases the initial Coulombic efficiency. With further encapsulation with a graphene cage, which allows the silicon core to expand within the cage while retaining electrical contact, the silicon hollow structure exhibits a high initial Coulombic efficiency and fast rise of later Coulombic efficiencies to >99.5% and superior stability in a full-cell battery.},
doi = {10.1021/acs.nanolett.8b03065},
journal = {Nano Letters},
number = 11,
volume = 18,
place = {United States},
year = {Fri Oct 19 00:00:00 EDT 2018},
month = {Fri Oct 19 00:00:00 EDT 2018}
}
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Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1021/acs.nanolett.8b03065
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Cited by: 99 works
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Figures / Tables:

Figure 1 Figure 1: Fabrication and merits of shell-protective secondary silicon nanostructures. (a) Scheme of the fabrication process. (b, c) Comparison of the SEI formation and calendering test between uncoated and Si shell coated Si NPs clusters. (b) Uncoated Si NPs cluster. The electrolyte can diffuse into the inner pores, resulting inmore » excessive SEI formation; the structure collapses easily during the calendering process, resulting in electrical contact loss. ( c) After Si shell coating. The electrolyte is prevented from leaking into the interior space, thus restricting SEI formation to the outer surface; more impressively, the structure becomes highly pressure-resistant and maintains intact under 100 MPa.« less
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    Works referencing / citing this record:

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    Scalable Solid-State Synthesis of Self-Assembled Si Nanoparticles in Spherical Carbons through Relative Miscibility for Li-Ion Batteries
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    Investigation of Electrochemical Performance on SnSe 2 and SnSe Nanocrystals as Anodes for Lithium Ions Batteries
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    Space‐Confined Atomic Clusters Catalyze Superassembly of Silicon Nanodots within Carbon Frameworks for Use in Lithium‐Ion Batteries
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    • Chen, Bingjie; Zu, Lianhai; Liu, Yao
    • Angewandte Chemie International Edition, Vol. 59, Issue 8
    • DOI: 10.1002/anie.201915502
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