Influence of Carbonate Solvents on Solid Electrolyte Interphase Composition over Si Electrodes Monitored by In Situ and Ex Situ Spectroscopies
A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and good ionic conductivity. To better understand the influence of carbonate solvents on the SEI composition and mechanism of formation, systemati...
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| Published in | ACS omega Vol. 6; no. 41; pp. 27335 - 27350 |
|---|---|
| Main Authors | , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
American Chemical Society
19.10.2021
ACS Publications |
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| Online Access | Get full text |
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| Abstract | A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and good ionic conductivity. To better understand the influence of carbonate solvents on the SEI composition and mechanism of formation, systematic studies were performed using dimethyl carbonate (DMC) or propylene carbonate (PC) solvent and LiPF6 as a salt. A 1 M LiPF6/EC-DMC was used for comparison. The surface chemical composition of the Si electrode was analyzed at different potentials of lithiation/delithiation and after a few cycles. Ex situ X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results demonstrate that a thinner and more stable SEI layer is formed in LiPF6/DMC. The in situ Fourier transform infrared spectroscopy proves that the coordination between Li+ and DMC is weaker, and fewer DMC molecules take part in the formation of the SEI layer. The higher capacity retention during 60 cycles and less significant morphological modifications of the Si electrode in 1 M LiPF6/DMC compared to other electrolytes were demonstrated, confirming a good and stable interfacial layer. The possible surface reactions are discussed, and the difference in the mechanisms of formation of SEI in these three various electrolytes is proposed. |
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| AbstractList | A solid electrolyte
interphase (SEI) layer on Si-based anodes should
have high mechanical properties to adapt the volume changes of Si
with low thickness and good ionic conductivity. To better understand
the influence of carbonate solvents on the SEI composition and mechanism
of formation, systematic studies were performed using dimethyl carbonate
(DMC) or propylene carbonate (PC) solvent and LiPF
6
as
a salt. A 1 M LiPF
6
/EC-DMC was used for comparison. The
surface chemical composition of the Si electrode was analyzed at different
potentials of lithiation/delithiation and after a few cycles.
Ex situ
X-ray photoelectron spectroscopy and time-of-flight
secondary ion mass spectrometry results demonstrate that a thinner
and more stable SEI layer is formed in LiPF
6
/DMC. The
in situ
Fourier transform infrared spectroscopy proves that
the coordination between Li
+
and DMC is weaker, and fewer
DMC molecules take part in the formation of the SEI layer. The higher
capacity retention during 60 cycles and less significant morphological
modifications of the Si electrode in 1 M LiPF
6
/DMC compared
to other electrolytes were demonstrated, confirming a good and stable
interfacial layer. The possible surface reactions are discussed, and
the difference in the mechanisms of formation of SEI in these three
various electrolytes is proposed. A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and good ionic conductivity. To better understand the influence of carbonate solvents on the SEI composition and mechanism of formation, systematic studies were performed using dimethyl carbonate (DMC) or propylene carbonate (PC) solvent and LiPF6 as a salt. A 1 M LiPF6/EC-DMC was used for comparison. The surface chemical composition of the Si electrode was analyzed at different potentials of lithiation/delithiation and after a few cycles. Ex situ X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results demonstrate that a thinner and more stable SEI layer is formed in LiPF6/DMC. The in situ Fourier transform infrared spectroscopy proves that the coordination between Li+ and DMC is weaker, and fewer DMC molecules take part in the formation of the SEI layer. The higher capacity retention during 60 cycles and less significant morphological modifications of the Si electrode in 1 M LiPF6/DMC compared to other electrolytes were demonstrated, confirming a good and stable interfacial layer. The possible surface reactions are discussed, and the difference in the mechanisms of formation of SEI in these three various electrolytes is proposed.A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and good ionic conductivity. To better understand the influence of carbonate solvents on the SEI composition and mechanism of formation, systematic studies were performed using dimethyl carbonate (DMC) or propylene carbonate (PC) solvent and LiPF6 as a salt. A 1 M LiPF6/EC-DMC was used for comparison. The surface chemical composition of the Si electrode was analyzed at different potentials of lithiation/delithiation and after a few cycles. Ex situ X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results demonstrate that a thinner and more stable SEI layer is formed in LiPF6/DMC. The in situ Fourier transform infrared spectroscopy proves that the coordination between Li+ and DMC is weaker, and fewer DMC molecules take part in the formation of the SEI layer. The higher capacity retention during 60 cycles and less significant morphological modifications of the Si electrode in 1 M LiPF6/DMC compared to other electrolytes were demonstrated, confirming a good and stable interfacial layer. The possible surface reactions are discussed, and the difference in the mechanisms of formation of SEI in these three various electrolytes is proposed. A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and good ionic conductivity. To better understand the influence of carbonate solvents on the SEI composition and mechanism of formation, systematic studies were performed using dimethyl carbonate (DMC) or propylene carbonate (PC) solvent and LiPF6 as a salt. A 1 M LiPF6/EC-DMC was used for comparison. The surface chemical composition of the Si electrode was analyzed at different potentials of lithiation/delithiation and after a few cycles. Ex situ X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectrometry results demonstrate that a thinner and more stable SEI layer is formed in LiPF6/DMC. The in situ Fourier transform infrared spectroscopy proves that the coordination between Li+ and DMC is weaker, and fewer DMC molecules take part in the formation of the SEI layer. The higher capacity retention during 60 cycles and less significant morphological modifications of the Si electrode in 1 M LiPF6/DMC compared to other electrolytes were demonstrated, confirming a good and stable interfacial layer. The possible surface reactions are discussed, and the difference in the mechanisms of formation of SEI in these three various electrolytes is proposed. |
| Author | Światowska, Jolanta Li, Jun-Tao Seyeux, Antoine Huang, Ling Wu, Zhan-Yu Lu, Yan-Qiu Sun, Shi-Gang Marcus, Philippe Zanna, Sandrine |
| AuthorAffiliation | College of Energy State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering |
| AuthorAffiliation_xml | – name: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering – name: College of Energy |
| Author_xml | – sequence: 1 givenname: Zhan-Yu surname: Wu fullname: Wu, Zhan-Yu – sequence: 2 givenname: Yan-Qiu surname: Lu fullname: Lu, Yan-Qiu organization: College of Energy – sequence: 3 givenname: Jun-Tao orcidid: 0000-0002-9650-6385 surname: Li fullname: Li, Jun-Tao email: jtli@xmu.edu.cn organization: College of Energy – sequence: 4 givenname: Sandrine surname: Zanna fullname: Zanna, Sandrine – sequence: 5 givenname: Antoine surname: Seyeux fullname: Seyeux, Antoine – sequence: 6 givenname: Ling orcidid: 0000-0003-1092-5974 surname: Huang fullname: Huang, Ling organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering – sequence: 7 givenname: Shi-Gang orcidid: 0000-0003-2327-4090 surname: Sun fullname: Sun, Shi-Gang organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, College of Chemistry and Chemical Engineering – sequence: 8 givenname: Philippe orcidid: 0000-0002-9140-0047 surname: Marcus fullname: Marcus, Philippe – sequence: 9 givenname: Jolanta orcidid: 0000-0002-3727-0499 surname: Światowska fullname: Światowska, Jolanta email: jolanta.swiatowska@chimieparistech.psl.eu |
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| Snippet | A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and... A solid electrolyte interphase (SEI) layer on Si-based anodes should have high mechanical properties to adapt the volume changes of Si with low thickness and... |
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| Title | Influence of Carbonate Solvents on Solid Electrolyte Interphase Composition over Si Electrodes Monitored by In Situ and Ex Situ Spectroscopies |
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