Solid electrolyte interphase formation between the Li 0.29 La 0.57 TiO 3 solid-state electrolyte and a Li-metal anode: an ab initio molecular dynamics study
Abstract
An ab initio molecular dynamics study of an electrochemical interface between a solid-state-electrolyte Li0.29La0.57TiO3 and Li-metal is performed to analyze interphase formation and evolution when external electric fields of 0, 0.5, 1.0 and 2.0 V Å–1 are applied. From this electrochemical stability analysis, it was concluded that lithium-oxide (Li2O) and lanthanum-oxide (La2O3) phases were formed at the electrolyte/anode interphase. As the electric field increased, oxygen from the electrolyte diffused through the Li-metal anode, increasing the amount of O from deeper crystallographic planes of the electrolyte that reacted with Li and La. A strong reduction of Ti was expected from their Bader charge variation from +3.5 in the bulk to +2.5 at the interface. Due to the loss of Li atoms from the anode to form Li-oxide at the interphase, vacancies were created on the Li-metal, causing anode structure amorphization near the Li-oxide phase and keeping the rest of the anode structure as BCC. Therefore, the interface was unstable because of the continuous Li-oxide and La-oxide formation and growth, which were more pronounced when increasing the external electric field.
- Authors:
-
[1]
- Department of Chemical Engineering, Texas A&M University, College Station, USA, Department of Electrical and Computer Engineering
- Publication Date:
- Research Org.:
- Texas A & M Univ., College Station, TX (United States)
- Sponsoring Org.:
- USDOE Office of Energy Efficiency and Renewable Energy (EERE)
- OSTI Identifier:
- 1602324
- Alternate Identifier(s):
- OSTI ID: 1799367
- Grant/Contract Number:
- EE0007766; EE0008210
- Resource Type:
- Published Article
- Journal Name:
- RSC Advances
- Additional Journal Information:
- Journal Name: RSC Advances Journal Volume: 10 Journal Issue: 15; Journal ID: ISSN 2046-2069
- Publisher:
- Royal Society of Chemistry (RSC)
- Country of Publication:
- United Kingdom
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Chemistry
Citation Formats
Galvez-Aranda, Diego E., and Seminario, Jorge M. Solid electrolyte interphase formation between the Li 0.29 La 0.57 TiO 3 solid-state electrolyte and a Li-metal anode: an ab initio molecular dynamics study. United Kingdom: N. p., 2020.
Web. doi:10.1039/C9RA10984F.
Galvez-Aranda, Diego E., & Seminario, Jorge M. Solid electrolyte interphase formation between the Li 0.29 La 0.57 TiO 3 solid-state electrolyte and a Li-metal anode: an ab initio molecular dynamics study. United Kingdom. https://doi.org/10.1039/C9RA10984F
Galvez-Aranda, Diego E., and Seminario, Jorge M. Mon .
"Solid electrolyte interphase formation between the Li 0.29 La 0.57 TiO 3 solid-state electrolyte and a Li-metal anode: an ab initio molecular dynamics study". United Kingdom. https://doi.org/10.1039/C9RA10984F.
@article{osti_1602324,
title = {Solid electrolyte interphase formation between the Li 0.29 La 0.57 TiO 3 solid-state electrolyte and a Li-metal anode: an ab initio molecular dynamics study},
author = {Galvez-Aranda, Diego E. and Seminario, Jorge M.},
abstractNote = {An ab initio molecular dynamics study of an electrochemical interface between a solid-state-electrolyte Li0.29La0.57TiO3 and Li-metal is performed to analyze interphase formation and evolution when external electric fields of 0, 0.5, 1.0 and 2.0 V Å–1 are applied. From this electrochemical stability analysis, it was concluded that lithium-oxide (Li2O) and lanthanum-oxide (La2O3) phases were formed at the electrolyte/anode interphase. As the electric field increased, oxygen from the electrolyte diffused through the Li-metal anode, increasing the amount of O from deeper crystallographic planes of the electrolyte that reacted with Li and La. A strong reduction of Ti was expected from their Bader charge variation from +3.5 in the bulk to +2.5 at the interface. Due to the loss of Li atoms from the anode to form Li-oxide at the interphase, vacancies were created on the Li-metal, causing anode structure amorphization near the Li-oxide phase and keeping the rest of the anode structure as BCC. Therefore, the interface was unstable because of the continuous Li-oxide and La-oxide formation and growth, which were more pronounced when increasing the external electric field.},
doi = {10.1039/C9RA10984F},
journal = {RSC Advances},
number = 15,
volume = 10,
place = {United Kingdom},
year = {Mon Mar 02 00:00:00 EST 2020},
month = {Mon Mar 02 00:00:00 EST 2020}
}
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