Enhanced Surface Interactions Enable Fast Li+ Conduction in Oxide/Polymer Composite Electrolyte

Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+‐insulating oxides...

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Vydané v:	Angewandte Chemie (International ed.) Ročník 59; číslo 10; s. 4131 - 4137
Hlavní autori:	Wu, Nan, Chien, Po‐Hsiu, Qian, Yumin, Li, Yutao, Xu, Henghui, Grundish, Nicholas S., Xu, Biyi, Jin, Haibo, Hu, Yan‐Yan, Yu, Guihua, Goodenough, John B.
Médium:	Journal Article
Jazyk:	English
Vydavateľské údaje:	Germany Wiley Subscription Services, Inc 02.03.2020 Wiley Blackwell (John Wiley & Sons)
Vydanie:	International ed. in English
Predmet:	all-solid-state battery composite electrolyte Composite materials Conduction Conductivity Electrolytes Electrolytic cells Ethylene oxide Fillers Fluorite Li-ion conductivity Li-ion transfer mechanism Lithium ions NMR Nuclear magnetic resonance Occupancy Oxides Oxygen Perovskites Polyethylene oxide Polymer matrix composites Polymers solid-state NMR Strong interactions (field theory) Vacancies Li-ion conductivity composite electrolyte solid-state NMR all-solid-state battery Li-ion transfer mechanism
ISSN:	1433-7851, 1521-3773, 1521-3773
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Abstract	Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+‐insulating oxides (fluorite Gd0.1Ce0.9O1.95 and perovskite La0.8Sr0.2Ga0.8Mg0.2O2.55) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li+ conductivity above 10−4 S cm−1 at 30 °C. Li solid‐state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O2− of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. The strong interaction between the surface oxygen vacancies of GDC/LSGM and the TFSI− anions in the composite polymer electrolyte changes Li+ distribution in two local environments, and the population increase of mobile Li+ ions in A2 significantly enhances the Li+ conductivity of the composite electrolyte.
AbstractList	Li -conducting oxides are considered better ceramic fillers than Li -insulating oxides for improving Li conductivity in composite polymer electrolytes owing to their ability to conduct Li through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li -insulating oxides (fluorite Gd Ce O and perovskite La Sr Ga Mg O ) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)-based polymer composite electrolytes, each with a Li conductivity above 10 S cm at 30 °C. Li solid-state NMR results show an increase in Li ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2-site occupancy originates from the strong interaction between the O of Li-salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li transport. All-solid-state Li-metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+‐insulating oxides (fluorite Gd0.1Ce0.9O1.95 and perovskite La0.8Sr0.2Ga0.8Mg0.2O2.55) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li+ conductivity above 10−4 S cm−1 at 30 °C. Li solid‐state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O2− of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. The strong interaction between the surface oxygen vacancies of GDC/LSGM and the TFSI− anions in the composite polymer electrolyte changes Li+ distribution in two local environments, and the population increase of mobile Li+ ions in A2 significantly enhances the Li+ conductivity of the composite electrolyte. Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+‐insulating oxides (fluorite Gd0.1Ce0.9O1.95 and perovskite La0.8Sr0.2Ga0.8Mg0.2O2.55) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li+ conductivity above 10−4 S cm−1 at 30 °C. Li solid‐state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O2− of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. Li+ -conducting oxides are considered better ceramic fillers than Li+ -insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+ -insulating oxides (fluorite Gd0.1 Ce0.9 O1.95 and perovskite La0.8 Sr0.2 Ga0.8 Mg0.2 O2.55 ) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)-based polymer composite electrolytes, each with a Li+ conductivity above 10-4 S cm-1 at 30 °C. Li solid-state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2-site occupancy originates from the strong interaction between the O2- of Li-salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All-solid-state Li-metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C.Li+ -conducting oxides are considered better ceramic fillers than Li+ -insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing to their ability to conduct Li+ through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li+ -insulating oxides (fluorite Gd0.1 Ce0.9 O1.95 and perovskite La0.8 Sr0.2 Ga0.8 Mg0.2 O2.55 ) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)-based polymer composite electrolytes, each with a Li+ conductivity above 10-4 S cm-1 at 30 °C. Li solid-state NMR results show an increase in Li+ ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2-site occupancy originates from the strong interaction between the O2- of Li-salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li+ transport. All-solid-state Li-metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C. Li + ‐conducting oxides are considered better ceramic fillers than Li + ‐insulating oxides for improving Li + conductivity in composite polymer electrolytes owing to their ability to conduct Li + through the ceramic oxide as well as across the oxide/polymer interface. Here we use two Li + ‐insulating oxides (fluorite Gd 0.1 Ce 0.9 O 1.95 and perovskite La 0.8 Sr 0.2 Ga 0.8 Mg 0.2 O 2.55 ) with a high concentration of oxygen vacancies to demonstrate two oxide/poly(ethylene oxide) (PEO)‐based polymer composite electrolytes, each with a Li + conductivity above 10 −4 S cm −1 at 30 °C. Li solid‐state NMR results show an increase in Li + ions (>10 %) occupying the more mobile A2 environment in the composite electrolytes. This increase in A2‐site occupancy originates from the strong interaction between the O 2− of Li‐salt anion and the surface oxygen vacancies of each oxide and contributes to the more facile Li + transport. All‐solid‐state Li‐metal cells with these composite electrolytes demonstrate a small interfacial resistance with good cycling performance at 35 °C.
Author	Xu, Biyi Chien, Po‐Hsiu Grundish, Nicholas S. Li, Yutao Jin, Haibo Hu, Yan‐Yan Goodenough, John B. Qian, Yumin Wu, Nan Xu, Henghui Yu, Guihua
Author_xml	– sequence: 1 givenname: Nan orcidid: 0000-0003-3100-199X surname: Wu fullname: Wu, Nan organization: The University of Texas at Austin – sequence: 2 givenname: Po‐Hsiu surname: Chien fullname: Chien, Po‐Hsiu organization: National High Magnetic Field Laboratory – sequence: 3 givenname: Yumin surname: Qian fullname: Qian, Yumin organization: The University of Texas at Austin – sequence: 4 givenname: Yutao orcidid: 0000-0003-0798-6880 surname: Li fullname: Li, Yutao email: lytthu@utexas.edu organization: The University of Texas at Austin – sequence: 5 givenname: Henghui orcidid: 0000-0003-2790-3122 surname: Xu fullname: Xu, Henghui organization: The University of Texas at Austin – sequence: 6 givenname: Nicholas S. surname: Grundish fullname: Grundish, Nicholas S. organization: The University of Texas at Austin – sequence: 7 givenname: Biyi orcidid: 0000-0002-8608-5257 surname: Xu fullname: Xu, Biyi organization: The University of Texas at Austin – sequence: 8 givenname: Haibo surname: Jin fullname: Jin, Haibo organization: Beijing Institute of Technology – sequence: 9 givenname: Yan‐Yan surname: Hu fullname: Hu, Yan‐Yan organization: Florida State University – sequence: 10 givenname: Guihua surname: Yu fullname: Yu, Guihua organization: The University of Texas at Austin – sequence: 11 givenname: John B. orcidid: 0000-0001-9350-3034 surname: Goodenough fullname: Goodenough, John B. email: jgoodenough@mail.utexas.edu organization: The University of Texas at Austin
BackLink	https://www.ncbi.nlm.nih.gov/pubmed/31893468$$D View this record in MEDLINE/PubMed https://www.osti.gov/biblio/1593491$$D View this record in Osti.gov
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Snippet	Li+‐conducting oxides are considered better ceramic fillers than Li+‐insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing... Li + ‐conducting oxides are considered better ceramic fillers than Li + ‐insulating oxides for improving Li + conductivity in composite polymer electrolytes... Li -conducting oxides are considered better ceramic fillers than Li -insulating oxides for improving Li conductivity in composite polymer electrolytes owing to... Li+ -conducting oxides are considered better ceramic fillers than Li+ -insulating oxides for improving Li+ conductivity in composite polymer electrolytes owing...
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SubjectTerms	all-solid-state battery composite electrolyte Composite materials Conduction Conductivity Electrolytes Electrolytic cells Ethylene oxide Fillers Fluorite Li-ion conductivity Li-ion transfer mechanism Lithium ions NMR Nuclear magnetic resonance Occupancy Oxides Oxygen Perovskites Polyethylene oxide Polymer matrix composites Polymers solid-state NMR Strong interactions (field theory) Vacancies
Title	Enhanced Surface Interactions Enable Fast Li+ Conduction in Oxide/Polymer Composite Electrolyte
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