The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes

Schroder, Kjell; Li, Juchuan; Dudney, Nancy J.; Meng, Ying Shirley; Stevenson, Keith J.; Alvarado, Judith

doi:10.1021/acs.chemmater.5b01627

Title: The Effect of Fluoroethylene Carbonate as an Additive on the Solid Electrolyte Interphase on Silicon Lithium-Ion Electrodes

Journal Article · Mon Aug 03 00:00:00 UTC 2015 · Chemistry of Materials

DOI: https://doi.org/10.1021/acs.chemmater.5b01627 · OSTI ID:1261351

Schroder, Kjell ^[1]; Li, Juchuan ^[2]; Dudney, Nancy J. ^[2]; Meng, Ying Shirley ^[3]; Stevenson, Keith J. ^[1]; Alvarado, Judith ^[3]

Univ. of Texas, Austin, TX (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of California, San Diego, CA (United States)

Fluoroethylene carbonate (FEC) has become a standard electrolyte additive for use with silicon negative electrodes, but how FEC affects solid electrolyte interphase (SEI) formation on the silicon anode’s surface is still not well understood. Herein, SEI formed from LiPF6-based carbonate electrolytes, with and without FEC, were investigated on 50 nm thick amorphous silicon thin film electrodes to understand the role of FEC on silicon electrode surface reactions. In contrast to previous work, anhydrous and anoxic techniques were used to prevent air and moisture contamination of prepared SEI films. This allowed for accurate characterization of the SEI structure and composition by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry depth profiling. These results show that FEC reduction leads to fluoride ion and LiF formation, consistent with previous computational and experimental results. Surprisingly, we also find that these species decrease lithium-ion solubility and increase the reactivity of the silicon surface. We conclude that the effectiveness of FEC at improving the Coulombic efficiency and capacity retention is due to fluoride ion formation from reduction of the electrolyte, which leads to the chemical attack of any silicon-oxide surface passivation layers and the formation of a kinetically stable SEI comprising predominately lithium fluoride and lithium oxide.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Understanding Charge Separation and Transfer at Interfaces in Energy Materials (CST); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC05-00OR22725; SC0001091

OSTI ID:: 1261351

Journal Information:: Chemistry of Materials, Journal Name: Chemistry of Materials Journal Issue: 27 Vol. 2015; ISSN 0897-4756

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Film-forming electrolyte additives for rechargeable lithium-ion batteries: progress and outlook Zhao, Huajun; Yu, Xueqing; Li, Jianding Journal of Materials Chemistry A, Vol. 7, Issue 15 https://doi.org/10.1039/c9ta00126c	journal	January 2019
An in situ formed graphene oxide–polyacrylic acid composite cage on silicon microparticles for lithium ion batteries via an esterification reaction Jung, Chul-Ho; Kim, Kyeong-Ho; Hong, Seong-Hyeon Journal of Materials Chemistry A, Vol. 7, Issue 20 https://doi.org/10.1039/c9ta02654a	journal	January 2019
Stabilizing a sodium-metal battery with the synergy effects of a sodiophilic matrix and fluorine-rich interface Wang, Qidi; Zhao, Chenglong; Lv, Xiaohui Journal of Materials Chemistry A, Vol. 7, Issue 43 https://doi.org/10.1039/c9ta06877e	journal	January 2019
Fluorine-donating electrolytes enable highly reversible 5-V-class Li metal batteries Suo, Liumin; Xue, Weijiang; Gobet, Mallory Proceedings of the National Academy of Sciences, Vol. 115, Issue 6 https://doi.org/10.1073/pnas.1712895115	journal	January 2018
Improving the electrochemical performance of Si-based anodes by co-compositing LiF and double carbon layer composed of graphite and three-dimensional PM Yuhao, Xu; Xiaogang, Sun; Chengcheng, Wei Materials Research Express, Vol. 6, Issue 11 https://doi.org/10.1088/2053-1591/ab47ca	journal	September 2019
Minimized lithium trapping by isovalent isomorphism for high initial Coulombic efficiency of silicon anodes Zhu, Bin; Liu, Guoliang; Lv, Guangxin Science Advances, Vol. 5, Issue 11 https://doi.org/10.1126/sciadv.aax0651	journal	November 2019
Quantitative Determination of Carbon Dioxide Content in Organic Electrolytes by Infrared Spectroscopy Yu, H.; Obrovac, M. N. Journal of The Electrochemical Society, Vol. 166, Issue 12 https://doi.org/10.1149/2.0291912jes	journal	January 2019
Insights from Studying the Origins of Reversible and Irreversible Capacities on Silicon Electrodes Lee, Pui-Kit; Li, Yingshun; Yu, Denis Y. W. Journal of The Electrochemical Society, Vol. 164, Issue 1 https://doi.org/10.1149/2.0321701jes	journal	December 2016
The Impact of CO ₂ Evolved from VC and FEC during Formation of Graphite Anodes in Lithium-Ion Batteries Schwenke, K. Uta; Solchenbach, Sophie; Demeaux, Julien Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0821910jes	journal	January 2019
Scalable Solid-State Synthesis of Self-Assembled Si Nanoparticles in Spherical Carbons through Relative Miscibility for Li-Ion Batteries Park, Yuwon; Lim, Jaewoong; Mok, Duckgyun Journal of The Electrochemical Society, Vol. 166, Issue 6 https://doi.org/10.1149/2.0891906jes	journal	January 2019
Consumption of Fluoroethylene Carbonate (FEC) on Si-C Composite Electrodes for Li-Ion Batteries Jung, Roland; Metzger, Michael; Haering, Dominik Journal of The Electrochemical Society, Vol. 163, Issue 8 https://doi.org/10.1149/2.0951608jes	journal	January 2016
Effect of Film-Forming Additive in Ionic Liquid Electrolyte on Electrochemical Performance of Si Negative-Electrode for LIBs Yamaguchi, Kazuki; Domi, Yasuhiro; Usui, Hiroyuki Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.0971902jes	journal	January 2019
Electrochemical Stability of Functionalized Cyclic Phosphonium ( CylP ⁺ _n A ⁻ ) Ionic Liquid Based Battery Electrolytes Dathar, Gopi Krishna Phani; Pandian, Shanthi; Raju, Srinivasa G. Journal of The Electrochemical Society, Vol. 163, Issue 6 https://doi.org/10.1149/2.1131606jes	journal	January 2016
Morphological Changes of Silicon Nanoparticles and the Influence of Cutoff Potentials in Silicon-Graphite Electrodes Wetjen, Morten; Solchenbach, Sophie; Pritzl, Daniel Journal of The Electrochemical Society, Vol. 165, Issue 7 https://doi.org/10.1149/2.1261807jes	journal	January 2018
Quantifying the Distribution of Electrolyte Decomposition Products in Silicon-Graphite Electrodes by Neutron Depth Profiling Wetjen, Morten; Trunk, Markus; Werner, Lukas Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.1341810jes	journal	January 2018
Differentiating the Degradation Phenomena in Silicon-Graphite Electrodes for Lithium-Ion Batteries Wetjen, Morten; Pritzl, Daniel; Jung, Roland Journal of The Electrochemical Society, Vol. 164, Issue 12 https://doi.org/10.1149/2.1921712jes	journal	January 2017
Consumption of Fluoroethylene Carbonate (FEC) on Si-C Composite Electrodes for Li-Ion Batteries Jung, Roland; Metzger, Michael; Haering, Dominik ECS Meeting Abstracts, Vol. MA2016-02, Issue 3 https://doi.org/10.1149/ma2016-02/3/284	journal	September 2016
Insights from Studying the Origins of Reversible and Irreversible Capacities on Silicon Electrodes Yu, Denis Yau Wai; Lee, Pui-kit ECS Meeting Abstracts, Vol. MA2016-03, Issue 2, p. 515-515 https://doi.org/10.1149/ma2016-03/2/515	journal	June 2016
Fabrication of Si Nanoparticles@Carbon Fibers Composites from Natural Nanoclay as an Advanced Lithium-Ion Battery Flexible Anode Liu, Sainan; Zhang, Qiang; Yang, Huaming Minerals, Vol. 8, Issue 5 https://doi.org/10.3390/min8050180	journal	April 2018

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