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Title: Failure mechanisms of single-crystal silicon electrodes in lithium-ion batteries

Journal Article · · Nature Communications
DOI:https://doi.org/10.1038/ncomms11886· OSTI ID:1379398
 [1];  [2];  [3];  [4]; ORCiD logo [5];  [2]
  1. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division; Univ. of California, Berkeley, CA (United States). Dept. of Chemistry
  5. Univ. of California, Berkeley, CA (United States). Dept. of Mechanical Engineering, Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Science Division
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Long-term durability is a major obstacle limiting the widespread use of lithium-ion batteries in heavy-duty applications and others demanding extended lifetime. As one of the root causes of the degradation of battery performance, the electrode failure mechanisms are still unknown. In this paper, we reveal the fundamental fracture mechanisms of single-crystal silicon electrodes over extended lithiation/delithiation cycles, using electrochemical testing, microstructure characterization, fracture mechanics and finite element analysis. Anisotropic lithium invasion causes crack initiation perpendicular to the electrode surface, followed by growth through the electrode thickness. The low fracture energy of the lithiated/unlithiated silicon interface provides a weak microstructural path for crack deflection, accounting for the crack patterns and delamination observed after repeated cycling. On the basis of this physical understanding, we demonstrate how electrolyte additives can heal electrode cracks and provide strategies to enhance the fracture resistance in future lithium-ion batteries from surface chemical, electrochemical and material science perspectives.

Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1379398
Journal Information:
Nature Communications, Vol. 7; ISSN 2041-1723
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 168 works
Citation information provided by
Web of Science

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book October 2010

Cited By (15)

Fabrication of Lamellar Nanosphere Structure for Effective Stress‐Management in Large‐Volume‐Variation Anodes of High‐Energy Lithium‐Ion Batteries journal June 2019
The Impact of Initial SEI Formation Conditions on Strain‐Induced Capacity Losses in Silicon Electrodes journal December 2018
Hierarchical Microspheres of Aggregated Silicon Nanoparticles with Nanometre Gaps as the Anode for Lithium‐Ion Batteries with Excellent Cycling Stability journal January 2019
Reactivating Li 2 O with Nano‐Sn to Achieve Ultrahigh Initial Coulombic Efficiency SiO Anodes for Li‐Ion Batteries journal June 2019
Silicon-Based Anodes for Lithium-Ion Batteries: From Fundamentals to Practical Applications journal January 2018
Recent Progress in Advanced Characterization Methods for Silicon‐Based Lithium‐Ion Batteries journal May 2019
Air-stable and freestanding lithium alloy/graphene foil as an alternative to lithium metal anodes journal July 2017
Towards maximized volumetric capacity via pore-coordinated design for large-volume-change lithium-ion battery anodes journal January 2019
High areal capacity battery electrodes enabled by segregated nanotube networks journal June 2019
Electrochemical Evaluation and Phase-related Impedance Studies on Silicon–Few Layer Graphene (FLG) Composite Electrode Systems journal January 2018
Self-healing SEI enables full-cell cycling of a silicon-majority anode with a coulombic efficiency exceeding 99.9% journal January 2017
Dual or multi carbonaceous coating strategies for next-generation batteries journal January 2018
Dimethylacrylamide, a novel electrolyte additive, can improve the electrochemical performances of silicon anodes in lithium-ion batteries journal January 2019
A study of evolution of residual stress in single crystal silicon electrode using Raman spectroscopy journal August 2017
Understanding the Mechanism of Stress Mitigation in Selenium-Doped Germanium Electrodes journal January 2019

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Related Subjects

36 MATERIALS SCIENCE
25 ENERGY STORAGE
batteries
chemical physics