Effect of Water Concentration in LiPF6‑Based Electrolytes on the Formation, Evolution, and Properties of the Solid Electrolyte Interphase on Si Anodes
A trace amount of water in an electrolyte is one of the factors detrimental to the electrochemical performance of silicon (Si)-based lithium-ion batteries that adversely affect the formation and evolution of the solid electrolyte interphase (SEI) on Si-based anodes and change its properties. Thus fa...
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| Veröffentlicht in: | ACS applied materials & interfaces 2020-11, Vol.12 (44), p.49563-49573 |
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| creator | Ha, Yeyoung Stetson, Caleb Harvey, Steven P Teeter, Glenn Tremolet de Villers, Bertrand J Jiang, Chun-Sheng Schnabel, Manuel Stradins, Paul Burrell, Anthony Han, Sang-Don |
| description | A trace amount of water in an electrolyte is one of the factors detrimental to the electrochemical performance of silicon (Si)-based lithium-ion batteries that adversely affect the formation and evolution of the solid electrolyte interphase (SEI) on Si-based anodes and change its properties. Thus far, a lack of fundamental and mechanistic understanding of SEI formation, evolution, and properties in the presence of water has inhibited efforts to stabilize the SEI for improved electrochemical performance. Thus, we investigated the SEI formed in a Gen2 electrolyte (1.2 M LiPF6 in ethylene carbonate/ethyl methyl carbonate, 3:7 wt %, water content: |
| doi_str_mv | 10.1021/acsami.0c12884 |
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(NREL), Golden, CO (United States)</creatorcontrib><description>A trace amount of water in an electrolyte is one of the factors detrimental to the electrochemical performance of silicon (Si)-based lithium-ion batteries that adversely affect the formation and evolution of the solid electrolyte interphase (SEI) on Si-based anodes and change its properties. Thus far, a lack of fundamental and mechanistic understanding of SEI formation, evolution, and properties in the presence of water has inhibited efforts to stabilize the SEI for improved electrochemical performance. Thus, we investigated the SEI formed in a Gen2 electrolyte (1.2 M LiPF6 in ethylene carbonate/ethyl methyl carbonate, 3:7 wt %, water content: <10 ppm) with and without additional water (50 ppm) at varying potentials (1.0, 0.5, 0.2, and 0.01 V vs Li/Li+). The impact of additional water on the morphological, (electro)chemical, and structural properties of SEI was studied using microscopic (atomic force microscopy and scanning spreading resistance microscopy) and spectroscopic (X-ray photoelectron spectroscopy, attenuated total reflection Fourier-transform infrared spectroscopy, and time-of-flight secondary ion mass spectrometry) techniques. The SEI exhibits both potential- and water concentration-dependent trends in its morphology and chemical composition. The presence of additional water in the electrolyte causes parasitic reactions, which onset at ∼1.0 V, resulting in a reduction of electrolyte components and result in the formation of an insulating, fluorophosphate-rich SEI. In addition, hydrolysis of LiPF6 creates hydrofluoric acid, which reacts with the surface oxide layer on the Si electrode, leading to a pitted and inhomogeneous SEI structure.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.0c12884</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>electrolyte water concentration ; Energy, Environmental, and Catalysis Applications ; fluorophosphates ; hydrolysis of LiPF6 ; MATERIALS SCIENCE ; silicon-electrolyte interphase (SiEI) ; surface pitting</subject><ispartof>ACS applied materials & interfaces, 2020-11, Vol.12 (44), p.49563-49573</ispartof><rights>2020 American Chemical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><orcidid>0000-0003-0729-1261 ; 0000-0003-0230-7500 ; 0000-0002-2931-659X ; 0000-0003-2679-2539 ; 0000-0001-6120-7062 ; 000000018685539X ; 0000000326792539 ; 0000000161207062 ; 0000000302307500 ; 0000000307291261 ; 000000022931659X</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acsami.0c12884$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsami.0c12884$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,778,782,883,27063,27911,27912,56725,56775</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1726072$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Ha, Yeyoung</creatorcontrib><creatorcontrib>Stetson, Caleb</creatorcontrib><creatorcontrib>Harvey, Steven P</creatorcontrib><creatorcontrib>Teeter, Glenn</creatorcontrib><creatorcontrib>Tremolet de Villers, Bertrand J</creatorcontrib><creatorcontrib>Jiang, Chun-Sheng</creatorcontrib><creatorcontrib>Schnabel, Manuel</creatorcontrib><creatorcontrib>Stradins, Paul</creatorcontrib><creatorcontrib>Burrell, Anthony</creatorcontrib><creatorcontrib>Han, Sang-Don</creatorcontrib><creatorcontrib>National Renewable Energy Lab. (NREL), Golden, CO (United States)</creatorcontrib><title>Effect of Water Concentration in LiPF6‑Based Electrolytes on the Formation, Evolution, and Properties of the Solid Electrolyte Interphase on Si Anodes</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>A trace amount of water in an electrolyte is one of the factors detrimental to the electrochemical performance of silicon (Si)-based lithium-ion batteries that adversely affect the formation and evolution of the solid electrolyte interphase (SEI) on Si-based anodes and change its properties. Thus far, a lack of fundamental and mechanistic understanding of SEI formation, evolution, and properties in the presence of water has inhibited efforts to stabilize the SEI for improved electrochemical performance. Thus, we investigated the SEI formed in a Gen2 electrolyte (1.2 M LiPF6 in ethylene carbonate/ethyl methyl carbonate, 3:7 wt %, water content: <10 ppm) with and without additional water (50 ppm) at varying potentials (1.0, 0.5, 0.2, and 0.01 V vs Li/Li+). The impact of additional water on the morphological, (electro)chemical, and structural properties of SEI was studied using microscopic (atomic force microscopy and scanning spreading resistance microscopy) and spectroscopic (X-ray photoelectron spectroscopy, attenuated total reflection Fourier-transform infrared spectroscopy, and time-of-flight secondary ion mass spectrometry) techniques. The SEI exhibits both potential- and water concentration-dependent trends in its morphology and chemical composition. The presence of additional water in the electrolyte causes parasitic reactions, which onset at ∼1.0 V, resulting in a reduction of electrolyte components and result in the formation of an insulating, fluorophosphate-rich SEI. In addition, hydrolysis of LiPF6 creates hydrofluoric acid, which reacts with the surface oxide layer on the Si electrode, leading to a pitted and inhomogeneous SEI structure.</description><subject>electrolyte water concentration</subject><subject>Energy, Environmental, and Catalysis Applications</subject><subject>fluorophosphates</subject><subject>hydrolysis of LiPF6</subject><subject>MATERIALS SCIENCE</subject><subject>silicon-electrolyte interphase (SiEI)</subject><subject>surface pitting</subject><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNpVkUFLwzAYhosoOKdXz8GTiJvJ16RNj3N0Ohg4mOIxZGnKMrpkNqngzb_gzd_nL7Fbh-Dpew8Pz_fCG0WXBA8JBnInlZcbM8SKAOf0KOqRjNIBBwbHf5nS0-jM-zXGSQyY9aLvvCy1CsiV6FUGXaOxs0rbUMtgnEXGopmZT5Kfz6976XWB8qqla1d9BO1RC4SVRhNXb_b4LcrfXdV0UdoCzWu31XUwO7bcswtXmX8WNLXt2-2qte98C4NG1hXan0cnpay8vjjcfvQyyZ_Hj4PZ08N0PJoNJDAcBkrDMqOlSnHMEwqKM0azAgrIKGepknxJCJVcgtKkiGWBIWVFBiBVVjIpWdyPrjqv88EIr0zQaqWctW1DQVJIcAotdN1B29q9NdoHsTFe6aqSVrvGC6CMEsxjtvPddGg7h1i7prZte0Gw2G0kuo3EYaP4F5lLh7A</recordid><startdate>20201104</startdate><enddate>20201104</enddate><creator>Ha, Yeyoung</creator><creator>Stetson, Caleb</creator><creator>Harvey, Steven P</creator><creator>Teeter, Glenn</creator><creator>Tremolet de Villers, Bertrand J</creator><creator>Jiang, Chun-Sheng</creator><creator>Schnabel, Manuel</creator><creator>Stradins, Paul</creator><creator>Burrell, Anthony</creator><creator>Han, Sang-Don</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0003-0729-1261</orcidid><orcidid>https://orcid.org/0000-0003-0230-7500</orcidid><orcidid>https://orcid.org/0000-0002-2931-659X</orcidid><orcidid>https://orcid.org/0000-0003-2679-2539</orcidid><orcidid>https://orcid.org/0000-0001-6120-7062</orcidid><orcidid>https://orcid.org/000000018685539X</orcidid><orcidid>https://orcid.org/0000000326792539</orcidid><orcidid>https://orcid.org/0000000161207062</orcidid><orcidid>https://orcid.org/0000000302307500</orcidid><orcidid>https://orcid.org/0000000307291261</orcidid><orcidid>https://orcid.org/000000022931659X</orcidid></search><sort><creationdate>20201104</creationdate><title>Effect of Water Concentration in LiPF6‑Based Electrolytes on the Formation, Evolution, and Properties of the Solid Electrolyte Interphase on Si Anodes</title><author>Ha, Yeyoung ; Stetson, Caleb ; Harvey, Steven P ; Teeter, Glenn ; Tremolet de Villers, Bertrand J ; Jiang, Chun-Sheng ; Schnabel, Manuel ; Stradins, Paul ; Burrell, Anthony ; Han, Sang-Don</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a250t-ce2b94fc7038642c85549d2d294857ca8b114a8a2ce1d3ad0275d922ac9f5aa53</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>electrolyte water concentration</topic><topic>Energy, Environmental, and Catalysis Applications</topic><topic>fluorophosphates</topic><topic>hydrolysis of LiPF6</topic><topic>MATERIALS SCIENCE</topic><topic>silicon-electrolyte interphase (SiEI)</topic><topic>surface pitting</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Ha, Yeyoung</creatorcontrib><creatorcontrib>Stetson, Caleb</creatorcontrib><creatorcontrib>Harvey, Steven P</creatorcontrib><creatorcontrib>Teeter, Glenn</creatorcontrib><creatorcontrib>Tremolet de Villers, Bertrand J</creatorcontrib><creatorcontrib>Jiang, Chun-Sheng</creatorcontrib><creatorcontrib>Schnabel, Manuel</creatorcontrib><creatorcontrib>Stradins, Paul</creatorcontrib><creatorcontrib>Burrell, Anthony</creatorcontrib><creatorcontrib>Han, Sang-Don</creatorcontrib><creatorcontrib>National Renewable Energy Lab. 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Interfaces</addtitle><date>2020-11-04</date><risdate>2020</risdate><volume>12</volume><issue>44</issue><spage>49563</spage><epage>49573</epage><pages>49563-49573</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>A trace amount of water in an electrolyte is one of the factors detrimental to the electrochemical performance of silicon (Si)-based lithium-ion batteries that adversely affect the formation and evolution of the solid electrolyte interphase (SEI) on Si-based anodes and change its properties. Thus far, a lack of fundamental and mechanistic understanding of SEI formation, evolution, and properties in the presence of water has inhibited efforts to stabilize the SEI for improved electrochemical performance. Thus, we investigated the SEI formed in a Gen2 electrolyte (1.2 M LiPF6 in ethylene carbonate/ethyl methyl carbonate, 3:7 wt %, water content: <10 ppm) with and without additional water (50 ppm) at varying potentials (1.0, 0.5, 0.2, and 0.01 V vs Li/Li+). The impact of additional water on the morphological, (electro)chemical, and structural properties of SEI was studied using microscopic (atomic force microscopy and scanning spreading resistance microscopy) and spectroscopic (X-ray photoelectron spectroscopy, attenuated total reflection Fourier-transform infrared spectroscopy, and time-of-flight secondary ion mass spectrometry) techniques. The SEI exhibits both potential- and water concentration-dependent trends in its morphology and chemical composition. The presence of additional water in the electrolyte causes parasitic reactions, which onset at ∼1.0 V, resulting in a reduction of electrolyte components and result in the formation of an insulating, fluorophosphate-rich SEI. 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| subjects | electrolyte water concentration Energy, Environmental, and Catalysis Applications fluorophosphates hydrolysis of LiPF6 MATERIALS SCIENCE silicon-electrolyte interphase (SiEI) surface pitting |
| title | Effect of Water Concentration in LiPF6‑Based Electrolytes on the Formation, Evolution, and Properties of the Solid Electrolyte Interphase on Si Anodes |
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