Chemical Interplay of Silicon and Graphite in a Composite Electrode in SEI Formation

Yang, Zhenzhen; Kim, Minkyu; Yu, Lei; Trask, Stephen E.; Bloom, Ira

doi:10.1021/acsami.1c15727

Chemical Interplay of Silicon and Graphite in a Composite Electrode in SEI Formation

Journal Article · Tue Nov 16 00:00:00 EST 2021 · ACS Applied Materials and Interfaces

DOI:https://doi.org/10.1021/acsami.1c15727· OSTI ID:1878228

Yang, Zhenzhen ^[1]; ^[1]; Yu, Lei ^[1]; ^[1]; ^[1]

Argonne National Lab. (ANL), Lemont, IL (United States)

In this study, we investigated the effect of the Si/graphite weight ratio in half-cells on the solid electrolyte interphase (SEI) layer's chemistry. The nominal concentrations of active materials were (wt % Si/wt % Gr) 15/73, 30/58, 60/28, and 80/0. The electrolyte in the cells consisted of either 1.2 M LiPF₆ in ethylene carbonate/ethyl methyl carbonate (3:7 by wt) or 1.2 M LiPF₆ in ethylene carbonate:ethyl methyl carbonate (3:7 by wt) + 10 wt % fluoroethylene carbonate. These coin cells were cycled five times at the C/10 rate. As expected, the addition of silicon to the electrode significantly increased the measured capacity. Examination of the aged composite material showed that the electrolyte influenced the concentration of chemical environments on the surface. Depth profiling revealed that these concentrations of surface environments changed with sputtering time. A statistics-of-mixtures model was used to deconvolute how silicon and graphite interacted during the formation of these species and how the interaction changed with depth.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL); Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Vehicle Technologies Office

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1878228

Journal Information:: ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 47 Vol. 13; ISSN 1944-8244

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (38)

25th Anniversary Article: Understanding the Lithiation of Silicon and Other Alloying Anodes for Lithium-Ion Batteries McDowell, Matthew T.; Lee, Seok Woo; Nix, William D. Advanced Materials, Vol. 25, Issue 36 https://doi.org/10.1002/adma.201301795	journal	August 2013
Silicon-Based Nanomaterials for Lithium-Ion Batteries: A Review Su, Xin; Wu, Qingliu; Li, Juchuan Advanced Energy Materials, Vol. 4, Issue 1 https://doi.org/10.1002/aenm.201300882	journal	October 2013
Operando Quantification of (De)Lithiation Behavior of Silicon-Graphite Blended Electrodes for Lithium-Ion Batteries Yao, Koffi P. C.; Okasinski, John S.; Kalaga, Kaushik Advanced Energy Materials, Vol. 9, Issue 8 https://doi.org/10.1002/aenm.201803380	journal	January 2019
Integration of Graphite and Silicon Anodes for the Commercialization of High‐Energy Lithium‐Ion Batteries Chae, Sujong; Choi, Seong‐Hyeon; Kim, Namhyung Angewandte Chemie International Edition, Vol. 59, Issue 1 https://doi.org/10.1002/anie.201902085	journal	January 2020
Understanding Component‐Specific Contributions and Internal Dynamics in Silicon/Graphite Blended Electrodes for High‐Energy Lithium‐Ion Batteries Heubner, Christian; Liebmann, Tobias; Lohrberg, Oliver Batteries & Supercaps, Vol. 5, Issue 1 https://doi.org/10.1002/batt.202100182	journal	October 2021
Surface film formation on a graphite electrode in Li-ion batteries: AFM and XPS study Leroy, S.; Blanchard, F.; Dedryvère, R. Surface and Interface Analysis, Vol. 37, Issue 10 https://doi.org/10.1002/sia.2072	journal	January 2005
Filming mechanism of lithium-carbon anodes in organic and inorganic electrolytes Besenhard, J. O.; Winter, M.; Yang, J. Journal of Power Sources, Vol. 54, Issue 2 https://doi.org/10.1016/0378-7753(94)02073-C	journal	April 1995
A short review of failure mechanisms of lithium metal and lithiated graphite anodes in liquid electrolyte solutions Aurbach, D. Solid State Ionics, Vol. 148, Issue 3-4 https://doi.org/10.1016/S0167-2738(02)00080-2	journal	June 2002
XPS studies of graphite electrode materials for lithium ion batteries Blyth, R. I. R.; Buqa, H.; Netzer, F. P. Applied Surface Science, Vol. 167, Issue 1-2 https://doi.org/10.1016/S0169-4332(00)00525-0	journal	October 2000
Review of selected electrode–solution interactions which determine the performance of Li and Li ion batteries Aurbach, Doron Journal of Power Sources, Vol. 89, Issue 2 https://doi.org/10.1016/S0378-7753(00)00431-6	journal	August 2000
Recent studies on the correlation between surface chemistry, morphology, three-dimensional structures and performance of Li and Li-C intercalation anodes in several important electrolyte systems Aurbach, D.; Zaban, A.; Ein-Eli, Y. Journal of Power Sources, Vol. 68, Issue 1 https://doi.org/10.1016/S0378-7753(97)02575-5	journal	September 1997
Comparative study of the solid electrolyte interphase on graphite in full Li-ion battery cells using X-ray photoelectron spectroscopy, secondary ion mass spectrometry, and electron microscopy Lee, Jung Tae; Nitta, Naoki; Benson, James Carbon, Vol. 52 https://doi.org/10.1016/j.carbon.2012.09.049	journal	February 2013
Calendar-life versus cycle-life aging of lithium-ion cells with silicon-graphite composite electrodes Kalaga, Kaushik; Rodrigues, Marco-Tulio F.; Trask, Stephen E. Electrochimica Acta, Vol. 280 https://doi.org/10.1016/j.electacta.2018.05.101	journal	August 2018
Electrochemistry and morphology of graphite negative electrodes containing silicon as capacity-enhancing electrode additive Jeschull, Fabian; Surace, Yuri; Zürcher, Simone Electrochimica Acta, Vol. 320 https://doi.org/10.1016/j.electacta.2019.134602	journal	October 2019
Modelling capacity fade in silicon-graphite composite electrodes for lithium-ion batteries Dhillon, Shweta; Hernández, Guiomar; Wagner, Nils P. Electrochimica Acta, Vol. 377 https://doi.org/10.1016/j.electacta.2021.138067	journal	May 2021
Generation and Evolution of the Solid Electrolyte Interphase of Lithium-Ion Batteries Heiskanen, Satu Kristiina; Kim, Jongjung; Lucht, Brett L. Joule, Vol. 3, Issue 10 https://doi.org/10.1016/j.joule.2019.08.018	journal	October 2019
Nano- and bulk-silicon-based insertion anodes for lithium-ion secondary cells Kasavajjula, Uday; Wang, Chunsheng; Appleby, A. John Journal of Power Sources, Vol. 163, Issue 2, p. 1003-1039 https://doi.org/10.1016/j.jpowsour.2006.09.084	journal	January 2007
High capacity graphite–silicon composite anode material for lithium-ion batteries Fuchsbichler, B.; Stangl, C.; Kren, H. Journal of Power Sources, Vol. 196, Issue 5 https://doi.org/10.1016/j.jpowsour.2010.10.081	journal	March 2011
Quantifying capacity loss due to solid-electrolyte-interphase layer formation on silicon negative electrodes in lithium-ion batteries Nadimpalli, Siva P. V.; Sethuraman, Vijay A.; Dalavi, Swapnil Journal of Power Sources, Vol. 215 https://doi.org/10.1016/j.jpowsour.2012.05.004	journal	October 2012
Mass Spectrometry Investigations on Electrolyte Degradation Products for the Development of Nanocomposite Electrodes in Lithium Ion Batteries Gireaud, Laurent; Grugeon, Sylvie; Pilard, Serge Analytical Chemistry, Vol. 78, Issue 11 https://doi.org/10.1021/ac051987w	journal	June 2006
Cycling Behavior of Silicon-Containing Graphite Electrodes, Part A: Effect of the Lithiation Protocol Schott, Tiphaine; Robert, Rosa; Ulmann, Pirmin A. The Journal of Physical Chemistry C, Vol. 121, Issue 34 https://doi.org/10.1021/acs.jpcc.7b05919	journal	August 2017
Capacity Fade and Its Mitigation in Li-Ion Cells with Silicon-Graphite Electrodes Bareño, Javier; Shkrob, Ilya A.; Gilbert, James A. The Journal of Physical Chemistry C, Vol. 121, Issue 38 https://doi.org/10.1021/acs.jpcc.7b06118	journal	September 2017
Electrode–Electrolyte Interface in Li-Ion Batteries: Current Understanding and New Insights Gauthier, Magali; Carney, Thomas J.; Grimaud, Alexis The Journal of Physical Chemistry Letters, Vol. 6, Issue 22 https://doi.org/10.1021/acs.jpclett.5b01727	journal	October 2015
Chemical Evolution in Silicon–Graphite Composite Anodes Investigated by Vibrational Spectroscopy Ruther, Rose E.; Hays, Kevin A.; An, Seong Jin ACS Applied Materials & Interfaces, Vol. 10, Issue 22 https://doi.org/10.1021/acsami.8b02197	journal	May 2018
Nano/Microstructured Silicon–Graphite Composite Anode for High-Energy-Density Li-Ion Battery Li, Peng; Hwang, Jang-Yeon; Sun, Yang-Kook ACS Nano https://doi.org/10.1021/acsnano.9b00169	journal	February 2019
Elimination of Fluorination: The Influence of Fluorine-Free Electrolytes on the Performance of LiNi _1/3 Mn _1/3 Co _1/3 O ₂ /Silicon–Graphite Li-Ion Battery Cells Hernández, Guiomar; Naylor, Andrew J.; Chien, Yu-Chuan ACS Sustainable Chemistry & Engineering, Vol. 8, Issue 27 https://doi.org/10.1021/acssuschemeng.0c01733	journal	June 2020
Principles and procedures of exploratory data analysis. Behrens, John T. Psychological Methods, Vol. 2, Issue 2 https://doi.org/10.1037/1082-989X.2.2.131	journal	January 1997
Interplay between electrochemical reactions and mechanical responses in silicon–graphite anodes and its impact on degradation Moon, Junhyuk; Lee, Heung Chan; Jung, Heechul Nature Communications, Vol. 12, Issue 1 https://doi.org/10.1038/s41467-021-22662-7	journal	May 2021
Design-Considerations regarding Silicon/Graphite and Tin/Graphite Composite Electrodes for Lithium-Ion Batteries Otero, Manuel; Heim, Christopher; Leiva, Ezequiel P. M. Scientific Reports, Vol. 8, Issue 1 https://doi.org/10.1038/s41598-018-33405-y	journal	October 2018
An XPS/AES comparative study of the surface behaviour of nano-silicon anodes for Li-ion batteries Radvanyi, Etienne; De Vito, Eric; Porcher, Willy J. Anal. At. Spectrom., Vol. 29, Issue 6 https://doi.org/10.1039/C3JA50362C	journal	January 2014
Capacity fade in high energy silicon-graphite electrodes for lithium-ion batteries Dose, W. M.; Piernas-Muñoz, M. J.; Maroni, V. A. Chemical Communications, Vol. 54, Issue 29 https://doi.org/10.1039/C8CC00456K	journal	January 2018
Fracture of crystalline silicon nanopillars during electrochemical lithium insertion Lee, S. W.; McDowell, M. T.; Berla, L. A. Proceedings of the National Academy of Sciences, Vol. 109, Issue 11 https://doi.org/10.1073/pnas.1201088109	journal	February 2012
Robust regression using iteratively reweighted least-squares Holland, Paul W.; Welsch, Roy E. Communications in Statistics - Theory and Methods, Vol. 6, Issue 9 https://doi.org/10.1080/03610927708827533	journal	January 1977
Experiments with Mixtures Scheffé, Henry Journal of the Royal Statistical Society: Series B (Methodological), Vol. 20, Issue 2 https://doi.org/10.1111/j.2517-6161.1958.tb00299.x	journal	July 1958
The Simplex‐Centroid Design for Experiments with Mixtures Scheffé, Henry Journal of the Royal Statistical Society: Series B (Methodological), Vol. 25, Issue 2 https://doi.org/10.1111/j.2517-6161.1963.tb00506.x	journal	July 1963
Structural Changes in Silicon Anodes during Lithium Insertion/Extraction Obrovac, M. N.; Christensen, Leif Electrochemical and Solid-State Letters, Vol. 7, Issue 5 https://doi.org/10.1149/1.1652421	journal	January 2004
A Comparative Study of Synthetic Graphite and Li Electrodes in Electrolyte Solutions Based on Ethylene Carbonate-Dimethyl Carbonate Mixtures Aurbach, D. Journal of The Electrochemical Society, Vol. 143, Issue 12 https://doi.org/10.1149/1.1837300	journal	January 1996
Evaluation Residual Moisture in Lithium-Ion Battery Electrodes and Its Effect on Electrode Performance Li, Jianlin; Daniel, Claus; An, Seong Jin MRS Advances, Vol. 1, Issue 15 https://doi.org/10.1557/adv.2016.6	journal	January 2016

Similar Records

Investigating the Chemical Reactivity of Lithium Silicate Model SEI Layers

Journal Article · Wed Mar 18 20:00:00 EDT 2020 · Journal of Physical Chemistry. C · OSTI ID:1616815

Effect of Vinylene Carbonate and Fluoroethylene Carbonate on SEI Formation on Graphitic Anodes in Li-Ion Batteries

Journal Article · Wed Jul 22 20:00:00 EDT 2015 · Journal of the Electrochemical Society · OSTI ID:1454692

Capacity Fade and Its Mitigation in Li-Ion Cells with Silicon-Graphite Electrodes

Journal Article · Tue Sep 05 20:00:00 EDT 2017 · Journal of Physical Chemistry. C · OSTI ID:1405319

Related Subjects

25 ENERGY STORAGE
X-ray photoelectron spectroscopy
anode materials
carbon
composite electrode
electrodes
electrolytes
lithium-ion battery
silicon
silicon-graphite electrode
solid electrolyte interphase layer
surface chemistry

Chemical Interplay of Silicon and Graphite in a Composite Electrode in SEI Formation

Citation Formats

References (38)

Similar Records

Related Subjects