TY - JOUR
T1 - Connecting the irreversible capacity loss in Li-ion batteries with the electronic insulating properties of solid electrolyte interphase (SEI) components
AU - Lin, Yu Xiao
AU - Liu, Zhe
AU - Leung, Kevin
AU - Chen, Long Qing
AU - Lu, Peng
AU - Qi, Yue
N1 - Funding Information:
YXL, KL, and YQ acknowledge the support for degradation mechanism modeling as part of Nanostructures for Electrical Energy Storage (NEES) , an Energy Frontier Research Center funded by the U.S. Department of Energy , Office of Science , Basic Energy Sciences under Award number DESC0001160 . ZL, LQC, PL, and YQ are grateful for the financial support by NSF GOALI under CMMI-1235092 . The computer simulations were carried out at MSU High Performance Computer Center (HPCC). Sandia National Laboratories is a multiprogram laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000 .
Publisher Copyright:
© 2016 Elsevier Ltd. All rights reserved.
PY - 2016/3/31
Y1 - 2016/3/31
N2 - The formation and continuous growth of a solid electrolyte interphase (SEI) layer are responsible for the irreversible capacity loss of batteries in the initial and subsequent cycles, respectively. In this article, the electron tunneling barriers from Li metal through three insulating SEI components, namely Li2CO3, LiF and Li3PO4, are computed by density function theory (DFT) approaches. Based on electron tunneling theory, it is estimated that sufficient to block electron tunneling. It is also found that the band gap decreases under tension while the work function remains the same, and thus the tunneling barrier decreases under tension and increases under compression. A new parameter, η, characterizing the average distances between anions, is proposed to unify the variation of band gap with strain under different loading conditions into a single linear function of η. An analytical model based on the tunneling results is developed to connect the irreversible capacity loss, due to the Li ions consumed in forming these SEI component layers on the surface of negative electrodes. The agreement between the model predictions and experimental results suggests that only the initial irreversible capacity loss is due to the self-limiting electron tunneling property of the SEI.
AB - The formation and continuous growth of a solid electrolyte interphase (SEI) layer are responsible for the irreversible capacity loss of batteries in the initial and subsequent cycles, respectively. In this article, the electron tunneling barriers from Li metal through three insulating SEI components, namely Li2CO3, LiF and Li3PO4, are computed by density function theory (DFT) approaches. Based on electron tunneling theory, it is estimated that sufficient to block electron tunneling. It is also found that the band gap decreases under tension while the work function remains the same, and thus the tunneling barrier decreases under tension and increases under compression. A new parameter, η, characterizing the average distances between anions, is proposed to unify the variation of band gap with strain under different loading conditions into a single linear function of η. An analytical model based on the tunneling results is developed to connect the irreversible capacity loss, due to the Li ions consumed in forming these SEI component layers on the surface of negative electrodes. The agreement between the model predictions and experimental results suggests that only the initial irreversible capacity loss is due to the self-limiting electron tunneling property of the SEI.
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U2 - 10.1016/j.jpowsour.2016.01.078
DO - 10.1016/j.jpowsour.2016.01.078
M3 - Article
AN - SCOPUS:84957068038
VL - 309
SP - 221
EP - 230
JO - Journal of Power Sources
JF - Journal of Power Sources
SN - 0378-7753
ER -