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

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

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

OSTI ID:: 1261351

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 319 works

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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
Confronting the Challenges of Next‐Generation Silicon Anode‐Based Lithium‐Ion Batteries: Role of Designer Electrolyte Additives and Polymeric Binders Eshetu, Gebrekidan Gebresilassie; Figgemeier, Egbert ChemSusChem, Vol. 12, Issue 12 https://doi.org/10.1002/cssc.201900209	journal	May 2019
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
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
Embracing high performance potassium-ion batteries with phosphorus-based electrodes: a review Yang, Dan; Liu, Chuntai; Rui, Xianhong Nanoscale, Vol. 11, Issue 33 https://doi.org/10.1039/c9nr05588f	journal	January 2019
In situ synthesis of porous Si dispersed in carbon nanotube intertwined expanded graphite for high-energy lithium-ion batteries Xu, Tao; Wang, Di; Qiu, Ping Nanoscale, Vol. 10, Issue 35 https://doi.org/10.1039/c8nr04587a	journal	January 2018
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
Impact of alginate and fluoroethylene carbonate on the electrochemical performance of SiO–SnCoC anode for lithium-ion batteries Luque, Guillermina L.; Li, Yan; Zeng, Xiaoqiao Journal of Solid State Electrochemistry, Vol. 23, Issue 2 https://doi.org/10.1007/s10008-018-4145-2	journal	November 2018
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
MOF derived ZnCo ₂ O ₄ porous hollow spheres functionalized with Ag nanoparticles for a long-cycle and high-capacity lithium ion battery anode Koo, Won-Tae; Jang, Hye-Yeon; Kim, Chanhoon Journal of Materials Chemistry A, Vol. 5, Issue 43 https://doi.org/10.1039/c7ta07573a	journal	January 2017
Towards maximized volumetric capacity via pore-coordinated design for large-volume-change lithium-ion battery anodes Ma, Jiyoung; Sung, Jaekyung; Hong, Jaehyung Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-018-08233-3	journal	January 2019
Evolving affinity between Coulombic reversibility and hysteretic phase transformations in nano-structured silicon-based lithium-ion batteries Ogata, K.; Jeon, S.; Ko, D. -S. Nature Communications, Vol. 9, Issue 1 https://doi.org/10.1038/s41467-018-02824-w	journal	February 2018

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