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

Journal Article · · Nature Communications

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.

Research Organization:
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)
Grant/Contract Number:
AC05-76RL01830; AC02-05CH11231
OSTI ID:
1578272
Report Number(s):
PNNL-SA--132988
Journal Information:
Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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Silicon Thin Films as Anodes for High-Performance Lithium-Ion Batteries with Effective Stress Relaxation journal December 2011
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Highly elastic binders integrating polyrotaxanes for silicon microparticle anodes in lithium ion batteries journal July 2017
High-performance lithium battery anodes using silicon nanowires
  • Chan, Candace K.; Peng, Hailin; Liu, Gao
  • Materials for Sustainable Energy: A Collection of Peer-Reviewed Research and Review Articles from Nature Publishing Group, p. 187-191 https://doi.org/10.1142/9789814317665_0026
book October 2010
High Capacity, Reversible Silicon Thin-Film Anodes for Lithium-Ion Batteries journal January 2003
Concurrent Reaction and Plasticity during Initial Lithiation of Crystalline Silicon in Lithium-Ion Batteries journal January 2012
The Effect of Stress on Battery-Electrode Capacity journal January 2017

Cited By (14)

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Few‐Layer Bismuthene with Anisotropic Expansion for High‐Areal‐Capacity Sodium‐Ion Batteries journal January 2019
Fabrication of Lamellar Nanosphere Structure for Effective Stress‐Management in Large‐Volume‐Variation Anodes of High‐Energy Lithium‐Ion Batteries journal June 2019
Low‐Temperature Reduction Strategy Synthesized Si/Ti 3 C 2 MXene Composite Anodes for High‐Performance Li‐Ion Batteries journal July 2019
The influence of compact and ordered carbon coating on solid‐state behaviors of silicon during electrochemical processes journal March 2020
Graphene Nanoscrolls with Confined Silicon Nanoparticles as a Durable Anode for Lithium‐Ion Batteries journal May 2019
Ultrasensitive Field‐Effect Biosensors Enabled by the Unique Electronic Properties of Graphene journal October 2019
Infinitesimal sulfur fusion yields quasi-metallic bulk silicon for stable and fast energy storage journal May 2019
Constraint spaces in carbon materials journal January 2019
Compact Si/C anodes fabricated by simultaneously regulating the size and oxidation degree of Si for Li-ion batteries journal January 2019
Scalable Solid-State Synthesis of Self-Assembled Si Nanoparticles in Spherical Carbons through Relative Miscibility for Li-Ion Batteries journal January 2019
Ultrasensitive Field-Effect Biosensors Enabled by the Unique Electronic Properties of Graphene text January 2020

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