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Title: Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries

Abstract

Due to the high lithium capacity of silicon, the composite (blended) electrodes containing silicon (Si) and graphite (Gr) particles are attractive alternatives to the all-Gr electrodes used in conventional lithium-ion batteries. In this Communication, the lithiation and delithiation in the Si and Gr particles in a 15 wt% Si composite electrode is quantified for each component using energy dispersive X-ray diffraction. This quantification is important as the components cycle in different potential regimes, and interpretation of cycling behavior is complicated by the potential hysteresis displayed by Si. The lithiation begins with Li alloying with Si; lithiation of Gr occurs at later stages when the potential dips below 0.2 V (all potentials are given vs. Li/Li+). In the 0.2 – 0.01 V range, the relative lithiation of Si and Gr is ~58% and 42%, respectively. During delithiation, Li+ ion extraction occurs preferentially from Gr in the 0.01 – 0.23 V range and from Si in the 0.23 – 1.0 V range; that is, the delithiation current is carried sequentially, first by graphite and then by silicon. Furthermore, these trends can be used for rational selection of electrochemical cycling windows that limits volumetric expansion in Si particles, thereby extending cell life.

Authors:
 [1];  [2];  [2];  [2]; ORCiD logo [2]
  1. Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Delaware, Newark, DE (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); USDOE
OSTI Identifier:
1496633
Alternate Identifier(s):
OSTI ID: 1489418
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Energy Materials
Additional Journal Information:
Journal Volume: 9; Journal Issue: 8; Journal ID: ISSN 1614-6832
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; X-ray diffraction; capacity quantification; electrochemistry; graphite silicon

Citation Formats

Yao, Koffi Pierre Claver, Okasinski, John S., Kalaga, Kaushik, Almer, Jonathan D., and Abraham, Daniel P. Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries. United States: N. p., 2019. Web. doi:10.1002/aenm.201803380.
Yao, Koffi Pierre Claver, Okasinski, John S., Kalaga, Kaushik, Almer, Jonathan D., & Abraham, Daniel P. Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries. United States. doi:10.1002/aenm.201803380.
Yao, Koffi Pierre Claver, Okasinski, John S., Kalaga, Kaushik, Almer, Jonathan D., and Abraham, Daniel P. Thu . "Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries". United States. doi:10.1002/aenm.201803380. https://www.osti.gov/servlets/purl/1496633.
@article{osti_1496633,
title = {Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries},
author = {Yao, Koffi Pierre Claver and Okasinski, John S. and Kalaga, Kaushik and Almer, Jonathan D. and Abraham, Daniel P.},
abstractNote = {Due to the high lithium capacity of silicon, the composite (blended) electrodes containing silicon (Si) and graphite (Gr) particles are attractive alternatives to the all-Gr electrodes used in conventional lithium-ion batteries. In this Communication, the lithiation and delithiation in the Si and Gr particles in a 15 wt% Si composite electrode is quantified for each component using energy dispersive X-ray diffraction. This quantification is important as the components cycle in different potential regimes, and interpretation of cycling behavior is complicated by the potential hysteresis displayed by Si. The lithiation begins with Li alloying with Si; lithiation of Gr occurs at later stages when the potential dips below 0.2 V (all potentials are given vs. Li/Li+). In the 0.2 – 0.01 V range, the relative lithiation of Si and Gr is ~58% and 42%, respectively. During delithiation, Li+ ion extraction occurs preferentially from Gr in the 0.01 – 0.23 V range and from Si in the 0.23 – 1.0 V range; that is, the delithiation current is carried sequentially, first by graphite and then by silicon. Furthermore, these trends can be used for rational selection of electrochemical cycling windows that limits volumetric expansion in Si particles, thereby extending cell life.},
doi = {10.1002/aenm.201803380},
journal = {Advanced Energy Materials},
number = 8,
volume = 9,
place = {United States},
year = {2019},
month = {1}
}

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