Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries
The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li-ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and g...
Gespeichert in:
Veröffentlicht in: | ACS applied materials & interfaces 2020-08, Vol.12 (31), p.34806-34814 |
---|---|
Hauptverfasser: | , , , , , , , |
Format: | Artikel |
Sprache: | eng |
Schlagworte: | |
Online-Zugang: | Volltext |
Tags: |
Tag hinzufügen
Keine Tags, Fügen Sie den ersten Tag hinzu!
|
container_end_page | 34814 |
---|---|
container_issue | 31 |
container_start_page | 34806 |
container_title | ACS applied materials & interfaces |
container_volume | 12 |
creator | Park, Dongsu Park, Haesun Lee, Yongheum Kim, Sang-Ok Jung, Hun-Gi Chung, Kyung Yoon Shim, Joon Hyung Yu, Seungho |
description | The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li-ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li3MCl6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li3MCl6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, Tl, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li3MCl6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M3+ with Zr4+. Zr-substituted phase (Li2.5M0.5Zr0.5Cl6, M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li3MCl6 SEs could lead to superionic Li3MCl6 SEs. |
doi_str_mv | 10.1021/acsami.0c07003 |
format | Article |
fullrecord | <record><control><sourceid>proquest_osti_</sourceid><recordid>TN_cdi_osti_scitechconnect_1661692</recordid><sourceformat>XML</sourceformat><sourcesystem>PC</sourcesystem><sourcerecordid>2422007956</sourcerecordid><originalsourceid>FETCH-LOGICAL-a440t-aae399b916404a04c43bb1746915b3bdce3adf60eb8ad888168280966fef98793</originalsourceid><addsrcrecordid>eNp1kT1PwzAQhiMEEqWwMltMCCnl7LhuPEL5lCoxFFgtx7k0rty42M7AvycowMZ0p9PzvtLpybJzCjMKjF5rE_XOzsDAAqA4yCZUcp6XbM4O_3bOj7OTGLcAomAwn2TxtUUfMFmjHbnDaDcd8Q1Z2dTafkeWrfPB1kjW_R6D9Z01ZOm7ujfJh0gaH8iNc_naO1vn66QTkie7afN375Le4G9P_uw7cqtTGjownmZHjXYRz37mNHt7uH9dPuWrl8fn5c0q15xDyrXGQspKUsGBa-CGF1VFF1xIOq-KqjZY6LoRgFWp67IsqShZCVKIBhtZLmQxzS7GXh-TVdHYhKY1vuvQJEWFoEKyAbocoX3wHz3GpHY2GnROd-j7qBhnDGAh52JAZyNqgo8xYKP2we50-FQU1LcCNSpQPwqGwNUYGO5q6_vQDe_-B38B5HmJDw</addsrcrecordid><sourcetype>Open Access Repository</sourcetype><iscdi>true</iscdi><recordtype>article</recordtype><pqid>2422007956</pqid></control><display><type>article</type><title>Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries</title><source>American Chemical Society Journals</source><creator>Park, Dongsu ; Park, Haesun ; Lee, Yongheum ; Kim, Sang-Ok ; Jung, Hun-Gi ; Chung, Kyung Yoon ; Shim, Joon Hyung ; Yu, Seungho</creator><creatorcontrib>Park, Dongsu ; Park, Haesun ; Lee, Yongheum ; Kim, Sang-Ok ; Jung, Hun-Gi ; Chung, Kyung Yoon ; Shim, Joon Hyung ; Yu, Seungho ; Argonne National Lab. (ANL), Argonne, IL (United States)</creatorcontrib><description>The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li-ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li3MCl6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li3MCl6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, Tl, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li3MCl6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M3+ with Zr4+. Zr-substituted phase (Li2.5M0.5Zr0.5Cl6, M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li3MCl6 SEs could lead to superionic Li3MCl6 SEs.</description><identifier>ISSN: 1944-8244</identifier><identifier>EISSN: 1944-8252</identifier><identifier>DOI: 10.1021/acsami.0c07003</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>all-solid-state batteries ; ENERGY STORAGE ; Energy, Environmental, and Catalysis Applications ; lithium chloride electrolytes ; materials design ; solid electrolytes</subject><ispartof>ACS applied materials & interfaces, 2020-08, Vol.12 (31), p.34806-34814</ispartof><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a440t-aae399b916404a04c43bb1746915b3bdce3adf60eb8ad888168280966fef98793</citedby><cites>FETCH-LOGICAL-a440t-aae399b916404a04c43bb1746915b3bdce3adf60eb8ad888168280966fef98793</cites><orcidid>0000-0002-1273-746X ; 0000-0001-5628-9331 ; 0000-0003-3912-6463 ; 0000-0002-3995-1968 ; 0000-0001-6266-8151 ; 0000-0002-2162-2680 ; 0000000221622680 ; 0000000239951968 ; 0000000156289331 ; 0000000162668151 ; 0000000339126463 ; 000000021273746X</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.0c07003$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acsami.0c07003$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,780,784,885,2765,27076,27924,27925,56738,56788</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1661692$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Park, Dongsu</creatorcontrib><creatorcontrib>Park, Haesun</creatorcontrib><creatorcontrib>Lee, Yongheum</creatorcontrib><creatorcontrib>Kim, Sang-Ok</creatorcontrib><creatorcontrib>Jung, Hun-Gi</creatorcontrib><creatorcontrib>Chung, Kyung Yoon</creatorcontrib><creatorcontrib>Shim, Joon Hyung</creatorcontrib><creatorcontrib>Yu, Seungho</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States)</creatorcontrib><title>Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries</title><title>ACS applied materials & interfaces</title><addtitle>ACS Appl. Mater. Interfaces</addtitle><description>The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li-ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li3MCl6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li3MCl6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, Tl, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li3MCl6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M3+ with Zr4+. Zr-substituted phase (Li2.5M0.5Zr0.5Cl6, M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li3MCl6 SEs could lead to superionic Li3MCl6 SEs.</description><subject>all-solid-state batteries</subject><subject>ENERGY STORAGE</subject><subject>Energy, Environmental, and Catalysis Applications</subject><subject>lithium chloride electrolytes</subject><subject>materials design</subject><subject>solid electrolytes</subject><issn>1944-8244</issn><issn>1944-8252</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNp1kT1PwzAQhiMEEqWwMltMCCnl7LhuPEL5lCoxFFgtx7k0rty42M7AvycowMZ0p9PzvtLpybJzCjMKjF5rE_XOzsDAAqA4yCZUcp6XbM4O_3bOj7OTGLcAomAwn2TxtUUfMFmjHbnDaDcd8Q1Z2dTafkeWrfPB1kjW_R6D9Z01ZOm7ujfJh0gaH8iNc_naO1vn66QTkie7afN375Le4G9P_uw7cqtTGjownmZHjXYRz37mNHt7uH9dPuWrl8fn5c0q15xDyrXGQspKUsGBa-CGF1VFF1xIOq-KqjZY6LoRgFWp67IsqShZCVKIBhtZLmQxzS7GXh-TVdHYhKY1vuvQJEWFoEKyAbocoX3wHz3GpHY2GnROd-j7qBhnDGAh52JAZyNqgo8xYKP2we50-FQU1LcCNSpQPwqGwNUYGO5q6_vQDe_-B38B5HmJDw</recordid><startdate>20200805</startdate><enddate>20200805</enddate><creator>Park, Dongsu</creator><creator>Park, Haesun</creator><creator>Lee, Yongheum</creator><creator>Kim, Sang-Ok</creator><creator>Jung, Hun-Gi</creator><creator>Chung, Kyung Yoon</creator><creator>Shim, Joon Hyung</creator><creator>Yu, Seungho</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7X8</scope><scope>OIOZB</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0002-1273-746X</orcidid><orcidid>https://orcid.org/0000-0001-5628-9331</orcidid><orcidid>https://orcid.org/0000-0003-3912-6463</orcidid><orcidid>https://orcid.org/0000-0002-3995-1968</orcidid><orcidid>https://orcid.org/0000-0001-6266-8151</orcidid><orcidid>https://orcid.org/0000-0002-2162-2680</orcidid><orcidid>https://orcid.org/0000000221622680</orcidid><orcidid>https://orcid.org/0000000239951968</orcidid><orcidid>https://orcid.org/0000000156289331</orcidid><orcidid>https://orcid.org/0000000162668151</orcidid><orcidid>https://orcid.org/0000000339126463</orcidid><orcidid>https://orcid.org/000000021273746X</orcidid></search><sort><creationdate>20200805</creationdate><title>Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries</title><author>Park, Dongsu ; Park, Haesun ; Lee, Yongheum ; Kim, Sang-Ok ; Jung, Hun-Gi ; Chung, Kyung Yoon ; Shim, Joon Hyung ; Yu, Seungho</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a440t-aae399b916404a04c43bb1746915b3bdce3adf60eb8ad888168280966fef98793</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>all-solid-state batteries</topic><topic>ENERGY STORAGE</topic><topic>Energy, Environmental, and Catalysis Applications</topic><topic>lithium chloride electrolytes</topic><topic>materials design</topic><topic>solid electrolytes</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Park, Dongsu</creatorcontrib><creatorcontrib>Park, Haesun</creatorcontrib><creatorcontrib>Lee, Yongheum</creatorcontrib><creatorcontrib>Kim, Sang-Ok</creatorcontrib><creatorcontrib>Jung, Hun-Gi</creatorcontrib><creatorcontrib>Chung, Kyung Yoon</creatorcontrib><creatorcontrib>Shim, Joon Hyung</creatorcontrib><creatorcontrib>Yu, Seungho</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States)</creatorcontrib><collection>CrossRef</collection><collection>MEDLINE - Academic</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>ACS applied materials & interfaces</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Park, Dongsu</au><au>Park, Haesun</au><au>Lee, Yongheum</au><au>Kim, Sang-Ok</au><au>Jung, Hun-Gi</au><au>Chung, Kyung Yoon</au><au>Shim, Joon Hyung</au><au>Yu, Seungho</au><aucorp>Argonne National Lab. (ANL), Argonne, IL (United States)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries</atitle><jtitle>ACS applied materials & interfaces</jtitle><addtitle>ACS Appl. Mater. Interfaces</addtitle><date>2020-08-05</date><risdate>2020</risdate><volume>12</volume><issue>31</issue><spage>34806</spage><epage>34814</epage><pages>34806-34814</pages><issn>1944-8244</issn><eissn>1944-8252</eissn><abstract>The development of solid electrolytes (SEs) is a promising pathway to improve the energy density and safety of conventional Li-ion batteries. Several lithium chloride SEs, Li3MCl6 (M = Y, Er, In, and Sc), have gained popularity due to their high ionic conductivity, wide electrochemical window, and good chemical stability. This study systematically investigated 17 Li3MCl6 SEs to identify novel and promising lithium chloride SEs. Calculation results revealed that 12 Li3MCl6 (M = Bi, Dy, Er, Ho, In, Lu, Sc, Sm, Tb, Tl, Tm, and Y) were stable phase with a wide electrochemical stability window and excellent chemical stability against cathode materials and moisture. Li-ion transport properties were examined using bond valence site energy (BVSE) and ab initio molecular dynamics (AIMD) calculation. Li3MCl6 showed the lower migration energy barrier in monoclinic structures, while orthorhombic and trigonal structures exhibited higher energy barriers due to the sluggish diffusion along the two-dimensional path based on the BVSE model. AIMD results confirmed the slower ion migration along the 2D path, exhibiting lower ionic diffusivity and higher activation energy in orthorhombic and trigonal structures. For the further increase of ionic conductivity in monoclinic structures, Li-ion vacancy was formed by the substitution of M3+ with Zr4+. Zr-substituted phase (Li2.5M0.5Zr0.5Cl6, M = In, Sc) exhibited up to a fourfold increase in ionic conductivity. This finding suggested that the optimization of Li vacancy in the Li3MCl6 SEs could lead to superionic Li3MCl6 SEs.</abstract><cop>United States</cop><pub>American Chemical Society</pub><doi>10.1021/acsami.0c07003</doi><tpages>9</tpages><orcidid>https://orcid.org/0000-0002-1273-746X</orcidid><orcidid>https://orcid.org/0000-0001-5628-9331</orcidid><orcidid>https://orcid.org/0000-0003-3912-6463</orcidid><orcidid>https://orcid.org/0000-0002-3995-1968</orcidid><orcidid>https://orcid.org/0000-0001-6266-8151</orcidid><orcidid>https://orcid.org/0000-0002-2162-2680</orcidid><orcidid>https://orcid.org/0000000221622680</orcidid><orcidid>https://orcid.org/0000000239951968</orcidid><orcidid>https://orcid.org/0000000156289331</orcidid><orcidid>https://orcid.org/0000000162668151</orcidid><orcidid>https://orcid.org/0000000339126463</orcidid><orcidid>https://orcid.org/000000021273746X</orcidid><oa>free_for_read</oa></addata></record> |
fulltext | fulltext |
identifier | ISSN: 1944-8244 |
ispartof | ACS applied materials & interfaces, 2020-08, Vol.12 (31), p.34806-34814 |
issn | 1944-8244 1944-8252 |
language | eng |
recordid | cdi_osti_scitechconnect_1661692 |
source | American Chemical Society Journals |
subjects | all-solid-state batteries ENERGY STORAGE Energy, Environmental, and Catalysis Applications lithium chloride electrolytes materials design solid electrolytes |
title | Theoretical Design of Lithium Chloride Superionic Conductors for All-Solid-State High-Voltage Lithium-Ion Batteries |
url | https://sfx.bib-bvb.de/sfx_tum?ctx_ver=Z39.88-2004&ctx_enc=info:ofi/enc:UTF-8&ctx_tim=2024-12-25T16%3A10%3A24IST&url_ver=Z39.88-2004&url_ctx_fmt=infofi/fmt:kev:mtx:ctx&rfr_id=info:sid/primo.exlibrisgroup.com:primo3-Article-proquest_osti_&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.genre=article&rft.atitle=Theoretical%20Design%20of%20Lithium%20Chloride%20Superionic%20Conductors%20for%20All-Solid-State%20High-Voltage%20Lithium-Ion%20Batteries&rft.jtitle=ACS%20applied%20materials%20&%20interfaces&rft.au=Park,%20Dongsu&rft.aucorp=Argonne%20National%20Lab.%20(ANL),%20Argonne,%20IL%20(United%20States)&rft.date=2020-08-05&rft.volume=12&rft.issue=31&rft.spage=34806&rft.epage=34814&rft.pages=34806-34814&rft.issn=1944-8244&rft.eissn=1944-8252&rft_id=info:doi/10.1021/acsami.0c07003&rft_dat=%3Cproquest_osti_%3E2422007956%3C/proquest_osti_%3E%3Curl%3E%3C/url%3E&disable_directlink=true&sfx.directlink=off&sfx.report_link=0&rft_id=info:oai/&rft_pqid=2422007956&rft_id=info:pmid/&rfr_iscdi=true |