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Title: In Situ Study of Silicon Electrode Lithiation with X-ray Reflectivity

Journal Article · · Nano Letters
 [1];  [2];  [2];  [2];  [2]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL), Materials Science Division; Stanford Univ., CA (United States). Dept. of Materials Science and Engineering
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States). Stanford Synchrotron Radiation Lightsource (SSRL), Materials Science Division

Surface sensitive X-ray reflectivity (XRR) measurements were performed to investigate the electrochemical lithiation of a native oxide terminated single crystalline silicon (100) electrode in real time during the first galvanostatic discharge cycle. This allows us to gain nanoscale, mechanistic insight into the lithiation of Si and the formation of the solid electrolyte interphase (SEI). We describe an electrochemistry cell specifically designed for in situ XRR studies and have determined the evolution of the electron density profile of the lithiated Si layer (LixSi) and the SEI layer with subnanometer resolution. We propose a three-stage lithiation mechanism with a reaction limited, layer-by-layer lithiation of the Si at the LixSi/Si interface.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1360198
Journal Information:
Nano Letters, Vol. 16, Issue 12; ISSN 1530-6984
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 54 works
Citation information provided by
Web of Science

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The Impact of Initial SEI Formation Conditions on Strain‐Induced Capacity Losses in Silicon Electrodes journal December 2018
Analysis and Simulation of One-Dimensional Transport Models for Lithium Symmetric Cells journal January 2019
In Situ Measurement of Phase Boundary Kinetics during Initial Lithiation of Crystalline Silicon through Picosecond Ultrasonics journal January 2019
The Atomic Scale Electrochemical Lithiation and Delithiation Process of Silicon journal September 2017
Intercalation of Layered Materials from Bulk to 2D journal May 2019
Si nanoflake-assembled blocks towards high initial coulombic efficiency anodes for lithium-ion batteries journal January 2018
Determination of the Solid Electrolyte Interphase Structure Grown on a Silicon Electrode Using a Fluoroethylene Carbonate Additive journal July 2017
Challenges and Recent Progress in the Development of Si Anodes for Lithium-Ion Battery journal September 2017