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

Journal Article · · Nano Letters
ORCiD logo [1];  [1]; ORCiD logo [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1];  [1];  [1];  [1]; ORCiD logo [2]
  1. Stanford Univ., Stanford, CA (United States)
  2. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
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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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1490980
Journal Information:
Nano Letters, Journal Name: Nano Letters Journal Issue: 11 Vol. 18; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Space‐Confined Atomic Clusters Catalyze Superassembly of Silicon Nanodots within Carbon Frameworks for Use in Lithium‐Ion Batteries journal January 2020
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A Facile Strategy to Construct Silver‐Modified, ZnO‐Incorporated and Carbon‐Coated Silicon/Porous‐Carbon Nanofibers with Enhanced Lithium Storage journal March 2019
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Scalable Solid-State Synthesis of Self-Assembled Si Nanoparticles in Spherical Carbons through Relative Miscibility for Li-Ion Batteries journal January 2019

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25 ENERGY STORAGE
Silicon
calendering
high-volumetric capacity
lithium-ion batteries
pressure-resistant
shell-protective