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

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.

doi:10.1002/ange.201914478

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

Journal Article · 22 January 2020 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.201914478 · OSTI ID:1593496

^[1]; Chien, Po‐Hsiu ^[2]; Qian, Yumin ^[3];

^[3];

^[3]; Grundish, Nicholas S. ^[3];

^[3]; Jin, Haibo ^[4]; Hu, Yan‐Yan ^[5]; Yu, Guihua ^[3];

^[3]

Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science &, Engineering Beijing Institute of Technology Beijing 100081 P. R. China, Materials Science and Engineering Program and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA
Center of Interdisciplinary Magnetic Resonance National High Magnetic Field Laboratory 1800 East Paul Dirac Drive Tallahassee FL 32310 USA
Materials Science and Engineering Program and Texas Materials Institute The University of Texas at Austin Austin TX 78712 USA
Beijing Key Laboratory of Construction Tailorable Advanced Functional Materials and Green Applications School of Materials Science &, Engineering Beijing Institute of Technology Beijing 100081 P. R. China
Center of Interdisciplinary Magnetic Resonance National High Magnetic Field Laboratory 1800 East Paul Dirac Drive Tallahassee FL 32310 USA, Department of Chemistry and Biochemistry Florida State University Tallahassee FL 32306 USA

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 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.

View Accepted Manuscript (Publisher)

Cite

Export

Save

Sponsoring Organization:: USDOE

Grant/Contract Number:: EE0007762

OSTI ID:: 1593496

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie Journal Issue: 10 Vol. 132; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (46)

Li6PS5X: A Class of Crystalline Li-Rich Solids With an Unusually High Li+ Mobility Deiseroth, Hans-Jörg; Kong, Shiao-Tong; Eckert, Hellmut Angewandte Chemie, Vol. 120, Issue 4 https://doi.org/10.1002/ange.200703900	journal	January 2008
Study on ionic transport mechanism and interactions between salt and polymer chain in PAN based solid polymer electrolytes containing LiCF3SO3 Yoon, Hae-Kwon; Chung, Won-Sub; Jo, Nam-Ju Electrochimica Acta, Vol. 50, Issue 2-3 https://doi.org/10.1016/j.electacta.2004.01.095	journal	November 2004
Dendrite-Free Li-Metal Battery Enabled by a Thin Asymmetric Solid Electrolyte with Engineered Layers Duan, Hui; Yin, Ya-Xia; Shi, Yang Journal of the American Chemical Society, Vol. 140, Issue 1 https://doi.org/10.1021/jacs.7b10864	journal	December 2017
High-performance all-solid-state batteries enabled by salt bonding to perovskite in poly(ethylene oxide) Xu, Henghui; Chien, Po-Hsiu; Shi, Jianjian Proceedings of the National Academy of Sciences, Vol. 116, Issue 38 https://doi.org/10.1073/pnas.1907507116	journal	August 2019
The Li-Ion Rechargeable Battery: A Perspective Goodenough, John B.; Park, Kyu-Sung Journal of the American Chemical Society, Vol. 135, Issue 4 https://doi.org/10.1021/ja3091438	journal	January 2013
Fast Lithium Ion Conduction in Garnet-Type Li₇La₃Zr₂O₁₂ Murugan, Ramaswamy; Thangadurai, Venkataraman; Weppner, Werner Angewandte Chemie International Edition, Vol. 46, Issue 41, p. 7778-7781 https://doi.org/10.1002/anie.200701144	journal	October 2007
A High-Energy-Density Potassium Battery with a Polymer-Gel Electrolyte and a Polyaniline Cathode Gao, Hongcai; Xue, Leigang; Xin, Sen Angewandte Chemie, Vol. 130, Issue 19 https://doi.org/10.1002/ange.201802248	journal	April 2018
Synthesis of and densification of oxygen-conducting La0.8Sr0.2Ga0.8Mg0.2O2.8 nano powder prepared from a low temperature hydrothermal urea precipitation process Chen, Te-Yuan; Fung, Kuan-Zong Journal of the European Ceramic Society, Vol. 28, Issue 4 https://doi.org/10.1016/j.jeurceramsoc.2007.08.006	journal	January 2008
Structural, morphological and electrical properties of Gd0.1Ce0.9O1.95 prepared by a citrate complexation method Fuentes, Rodolfo O.; Baker, Richard T. Journal of Power Sources, Vol. 186, Issue 2 https://doi.org/10.1016/j.jpowsour.2008.09.119	journal	January 2009
Crystalline phases, morphology and conductivity of PEO:LiTFSI electrolytes in the eutectic region Marzantowicz, M.; Dygas, J. R.; Krok, F. Journal of Power Sources, Vol. 159, Issue 1 https://doi.org/10.1016/j.jpowsour.2006.02.044	journal	September 2006
Li _0.33 La _0.557 TiO ₃ ceramic nanofiber-enhanced polyethylene oxide-based composite polymer electrolytes for all-solid-state lithium batteries Zhu, Pei; Yan, Chaoyi; Dirican, Mahmut Journal of Materials Chemistry A, Vol. 6, Issue 10 https://doi.org/10.1039/C7TA10517G	journal	January 2018
Poly(ethylene oxide)-based electrolytes for lithium-ion batteries Xue, Zhigang; He, Dan; Xie, Xiaolin Journal of Materials Chemistry A, Vol. 3, Issue 38 https://doi.org/10.1039/C5TA03471J	journal	January 2015
Garnet Electrolyte with an Ultralow Interfacial Resistance for Li-Metal Batteries Li, Yutao; Chen, Xi; Dolocan, Andrei Journal of the American Chemical Society, Vol. 140, Issue 20 https://doi.org/10.1021/jacs.8b03106	journal	April 2018
Solid polymer electrolytes incorporating cubic Li7La3Zr2O12 for all-solid-state lithium rechargeable batteries Chen, Fei; Yang, Dunjie; Zha, Wenping Electrochimica Acta, Vol. 258 https://doi.org/10.1016/j.electacta.2017.11.164	journal	December 2017
Flexible, solid-state, ion-conducting membrane with 3D garnet nanofiber networks for lithium batteries Fu, Kun (Kelvin); Gong, Yunhui; Dai, Jiaqi Proceedings of the National Academy of Sciences, Vol. 113, Issue 26 https://doi.org/10.1073/pnas.1600422113	journal	June 2016
IONIC CONDUCTIVITY AND LITHIUM TRANSFERENCE NUMBER OF POLY(ETHYLENE OXIDE):LiTFSI SYSTEM Pożyczka, K.; Marzantowicz, M.; Dygas, J. R. Electrochimica Acta, Vol. 227 https://doi.org/10.1016/j.electacta.2016.12.172	journal	February 2017
Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li ₇ La ₃ Zr ₂ O ₁₂ –polyethylene oxide–tetraethylene glycol dimethyl ether Zheng, Jin; Dang, Heather; Feng, Xuyong Journal of Materials Chemistry A, Vol. 5, Issue 35 https://doi.org/10.1039/C7TA05832B	journal	January 2017
PEO/garnet composite electrolytes for solid-state lithium batteries: From “ceramic-in-polymer” to “polymer-in-ceramic” Chen, Long; Li, Yutao; Li, Shuai-Peng Nano Energy, Vol. 46 https://doi.org/10.1016/j.nanoen.2017.12.037	journal	April 2018
Solid Halide Electrolytes with High Lithium-Ion Conductivity for Application in 4 V Class Bulk-Type All-Solid-State Batteries Asano, Tetsuya; Sakai, Akihiro; Ouchi, Satoru Advanced Materials, Vol. 30, Issue 44 https://doi.org/10.1002/adma.201803075	journal	September 2018
Boosting Solid-State Diffusivity and Conductivity in Lithium Superionic Argyrodites by Halide Substitution Adeli, Parvin; Bazak, J. David; Park, Kern Ho Angewandte Chemie International Edition, Vol. 58, Issue 26 https://doi.org/10.1002/anie.201814222	journal	May 2019
Mixed phase solid electrolytes Skaarup, S. Solid State Ionics, Vol. 28-30 https://doi.org/10.1016/0167-2738(88)90314-1	journal	September 1988
Lithium Ion Pathway within Li 7 La 3 Zr 2 O 12 -Polyethylene Oxide Composite Electrolytes Zheng, Jin; Tang, Mingxue; Hu, Yan-Yan Angewandte Chemie, Vol. 128, Issue 40 https://doi.org/10.1002/ange.201607539	journal	September 2016
Li6PS5X: A Class of Crystalline Li-Rich Solids With an Unusually High Li+ Mobility Deiseroth, Hans-Jörg; Kong, Shiao-Tong; Eckert, Hellmut Angewandte Chemie International Edition, Vol. 47, Issue 4 https://doi.org/10.1002/anie.200703900	journal	January 2008
Recent advances in all-solid-state rechargeable lithium batteries Sun, Chunwen; Liu, Jin; Gong, Yudong Nano Energy, Vol. 33 https://doi.org/10.1016/j.nanoen.2017.01.028	journal	March 2017
Polymer Electrolytes Armand, Michel B. Annual Review of Materials Science, Vol. 16, Issue 1 https://doi.org/10.1146/annurev.ms.16.080186.001333	journal	August 1986
Lithium coordination and mobility in gel electrolytes based on an acrylate polymer with ethylene oxide side chains Adebahr, J.; Forsyth, M.; MacFarlane, D. R. Journal of Materials Chemistry, Vol. 13, Issue 4 https://doi.org/10.1039/b208354j	journal	February 2003
A High-Energy-Density Potassium Battery with a Polymer-Gel Electrolyte and a Polyaniline Cathode Gao, Hongcai; Xue, Leigang; Xin, Sen Angewandte Chemie International Edition, Vol. 57, Issue 19 https://doi.org/10.1002/anie.201802248	journal	April 2018
Pathways for practical high-energy long-cycling lithium metal batteries Liu, Jun; Bao, Zhenan; Cui, Yi Nature Energy, Vol. 4, Issue 3 https://doi.org/10.1038/s41560-019-0338-x	journal	February 2019
Nanotechnology for environmentally sustainable electromobility Ellingsen, Linda Ager-Wick; Hung, Christine Roxanne; Majeau-Bettez, Guillaume Nature Nanotechnology, Vol. 11, Issue 12 https://doi.org/10.1038/nnano.2016.237	journal	December 2016
Schnelle Lithiumionenleitung in granatartigem Li7La3Zr2O12 Murugan, Ramaswamy; Thangadurai, Venkataraman; Weppner, Werner Angewandte Chemie, Vol. 119, Issue 41 https://doi.org/10.1002/ange.200701144	journal	October 2007
Optimizing Li+ conductivity in a garnet framework Li, Yutao; Han, Jian- Tao; Wang, Chang- An Journal of Materials Chemistry, Vol. 22, Issue 30 https://doi.org/10.1039/c2jm31413d	journal	January 2012
Ultrathin, flexible, solid polymer composite electrolyte enabled with aligned nanoporous host for lithium batteries Wan, Jiayu; Xie, Jin; Kong, Xian Nature Nanotechnology, Vol. 14, Issue 7 https://doi.org/10.1038/s41565-019-0465-3	journal	May 2019
Lithium-7 NMR studies of concentrated LiI/PEO-based solid electrolytes Dai, Y.; Greenbaum, S.; Golodnitsky, D. Solid State Ionics, Vol. 106, Issue 1-2 https://doi.org/10.1016/S0167-2738(97)00488-8	journal	February 1998
Ionic Conductivity Enhancement of Polymer Electrolytes with Ceramic Nanowire Fillers Liu, Wei; Liu, Nian; Sun, Jie Nano Letters, Vol. 15, Issue 4, p. 2740-2745 https://doi.org/10.1021/acs.nanolett.5b00600	journal	March 2015
New Insights into the Compositional Dependence of Li-Ion Transport in Polymer–Ceramic Composite Electrolytes Zheng, Jin; Hu, Yan-Yan ACS Applied Materials & Interfaces, Vol. 10, Issue 4 https://doi.org/10.1021/acsami.7b17301	journal	January 2018
Contact ion pair formation and ether oxygen coordination in the polymer electrolytes M[N(CF3SO2)2]2PEOn for M = Mg, Ca, Sr and Ba Bakker, A. Polymer, Vol. 36, Issue 23 https://doi.org/10.1016/0032-3861(95)96841-U	journal	January 1995
Enhancing ionic conductivity in composite polymer electrolytes with well-aligned ceramic nanowires Liu, Wei; Lee, Seok Woo; Lin, Dingchang Nature Energy, Vol. 2, Issue 5 https://doi.org/10.1038/nenergy.2017.35	journal	April 2017
Polymer Electrolytes for Lithium-Ion Batteries Meyer, Wolfgang H. Advanced Materials, Vol. 10, Issue 6, p. 439-448 https://doi.org/10.1002/(SICI)1521-4095(199804)10:6<439::AID-ADMA439>3.0.CO;2-I	journal	April 1998
All solid-state polymer electrolytes for high-performance lithium ion batteries Yue, Liping; Ma, Jun; Zhang, Jianjun Energy Storage Materials, Vol. 5 https://doi.org/10.1016/j.ensm.2016.07.003	journal	October 2016
Vertically Aligned and Continuous Nanoscale Ceramic–Polymer Interfaces in Composite Solid Polymer Electrolytes for Enhanced Ionic Conductivity Zhang, Xiaokun; Xie, Jin; Shi, Feifei Nano Letters, Vol. 18, Issue 6 https://doi.org/10.1021/acs.nanolett.8b01111	journal	May 2018
The influence of phase segregation on properties of semicrystalline PEO:LiTFSI electrolytes Marzantowicz, M.; Krok, F.; Dygas, J. R. Solid State Ionics, Vol. 179, Issue 27-32 https://doi.org/10.1016/j.ssi.2007.11.035	journal	September 2008
Nanocomposite polymer electrolytes for lithium batteries Croce, F.; Appetecchi, G. B.; Persi, L. Nature, Vol. 394, Issue 6692 https://doi.org/10.1038/28818	journal	July 1998
Boosting Solid‐State Diffusivity and Conductivity in Lithium Superionic Argyrodites by Halide Substitution Adeli, Parvin; Bazak, J. David; Park, Kern Ho Angewandte Chemie, Vol. 131, Issue 26 https://doi.org/10.1002/ange.201814222	journal	May 2019
Mastering the interface for advanced all-solid-state lithium rechargeable batteries Li, Yutao; Zhou, Weidong; Chen, Xi Proceedings of the National Academy of Sciences, Vol. 113, Issue 47 https://doi.org/10.1073/pnas.1615912113	journal	November 2016
Lithium battery chemistries enabled by solid-state electrolytes Manthiram, Arumugam; Yu, Xingwen; Wang, Shaofei Nature Reviews Materials, Vol. 2, Issue 4 https://doi.org/10.1038/natrevmats.2016.103	journal	February 2017
Lithium Ion Pathway within Li ₇ La ₃ Zr ₂ O ₁₂ -Polyethylene Oxide Composite Electrolytes Zheng, Jin; Tang, Mingxue; Hu, Yan-Yan Angewandte Chemie International Edition, Vol. 55, Issue 40 https://doi.org/10.1002/anie.201607539	journal	September 2016

Similar Records

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

Journal Article · 2019 · Angewandte Chemie (International Edition) · OSTI ID:1799353

Wu, Nan; Chien, Po‐Hsiu; Qian, Yumin; +8 more

Li ₂ S ₆ ‐Integrated PEO‐Based Polymer Electrolytes for All‐Solid‐State Lithium‐Metal Batteries

Journal Article · 2021 · Angewandte Chemie · OSTI ID:1804902

Fang, Ruyi; Xu, Biyi; Grundish, Nicholas S.; +6 more

Effects of Plasticizer Content and Ceramic Addition on Electrochemical Properties of Cross-Linked Polymer Electrolyte

Journal Article · 2021 · Journal of the Electrochemical Society · OSTI ID:1807302

Du, Zhijia; Chen, Xi; Sahore, Ritu; +3 more

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

Citation Formats

References (46)

Similar Records

Related Subjects

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