Flexible, solid-state, ion-conducting membrane with 3D garnet nanofiber networks for lithium batteries

Fu, Kun (Kelvin); Gong, Yunhui; Dai, Jiaqi; Gong, Amy; Han, Xiaogang; Yao, Yonggang; Wang, Chengwei; Wang, Yibo; Chen, Yanan; Yan, Chaoyi; Li, Yiju; Wachsman, Eric D.; Hu, Liangbing

doi:10.1073/pnas.1600422113

Flexible, solid-state, ion-conducting membrane with 3D garnet nanofiber networks for lithium batteries

Journal Article · Wed Jun 15 00:00:00 EDT 2016 · Proceedings of the National Academy of Sciences of the United States of America

DOI:https://doi.org/10.1073/pnas.1600422113· OSTI ID:1608918

Fu, Kun (Kelvin) ^[1]; Gong, Yunhui ^[2]; Dai, Jiaqi ^[2]; Gong, Amy ^[2]; Han, Xiaogang ^[2]; Yao, Yonggang ^[2]; Wang, Chengwei ^[2]; Wang, Yibo ^[2]; Chen, Yanan ^[2]; Yan, Chaoyi ^[2]; Li, Yiju ^[2]; Wachsman, Eric D. ^[2]; Hu, Liangbing ^[2]

Univ. of Maryland, College Park, MD (United States); University of Maryland, College Park
Univ. of Maryland, College Park, MD (United States)

Beyond state-of-the-art lithium-ion battery (LIB) technology with metallic lithium anodes to replace conventional ion intercalation anode materials is highly desirable because of lithium’s highest specific capacity (3,860 mA/g) and lowest negative electrochemical potential (~3.040 V vs. the standard hydrogen electrode). In this work, we report for the first time, to our knowledge, a 3D lithium-ion–conducting ceramic network based on garnet-type Li_6.4La₃Zr₂Al_0.2O₁₂(LLZO) lithium-ion conductor to provide continuous Li⁺transfer channels in a polyethylene oxide (PEO)-based composite. This composite structure further provides structural reinforcement to enhance the mechanical properties of the polymer matrix. The flexible solid-state electrolyte composite membrane exhibited an ionic conductivity of 2.5 × 10^-4 S/cm at room temperature. The membrane can effectively block dendrites in a symmetric Li | electrolyte | Li cell during repeated lithium stripping/plating at room temperature, with a current density of 0.2 mA/cm² for around 500 h and a current density of 0.5 mA/cm² for over 300 h. Finally, these results provide an all solid ion-conducting membrane that can be applied to flexible LIBs and other electrochemical energy storage systems, such as lithium–sulfur batteries.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Maryland, College Park, MD (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE)

Grant/Contract Number:: EE0007807

OSTI ID:: 1608918

Journal Information:: Proceedings of the National Academy of Sciences of the United States of America, Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Issue: 26 Vol. 113; ISSN 0027-8424

Publisher:: National Academy of SciencesCopyright Statement

Country of Publication:: United States

Language:: English

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A flexible NASICON-type composite electrolyte for lithium-oxygen/air battery Zhang, Kaifang; Mu, Shijia; Liu, Wei Ionics, Vol. 25, Issue 1 https://doi.org/10.1007/s11581-018-2580-9	journal	May 2018
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Recent Advancements in Polymer-Based Composite Electrolytes for Rechargeable Lithium Batteries Tan, Shuang-Jie; Zeng, Xian-Xiang; Ma, Qiang Electrochemical Energy Reviews, Vol. 1, Issue 2 https://doi.org/10.1007/s41918-018-0011-2	journal	May 2018
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Self-smoothing anode for achieving high-energy lithium metal batteries under realistic conditions Niu, Chaojiang; Pan, Huilin; Xu, Wu Nature Nanotechnology, Vol. 14, Issue 6 https://doi.org/10.1038/s41565-019-0427-9	journal	April 2019
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High-voltage and free-standing poly(propylene carbonate)/Li _6.75 La ₃ Zr _1.75 Ta _0.25 O ₁₂ composite solid electrolyte for wide temperature range and flexible solid lithium ion battery Zhang, Jianjun; Zang, Xiao; Wen, Huijie Journal of Materials Chemistry A, Vol. 5, Issue 10 https://doi.org/10.1039/c6ta10066j	journal	January 2017
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Flexible/shape-versatile, bipolar all-solid-state lithium-ion batteries prepared by multistage printing Kim, Se-Hee; Choi, Keun-Ho; Cho, Sung-Ju Energy & Environmental Science, Vol. 11, Issue 2 https://doi.org/10.1039/c7ee01630a	journal	January 2018
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Hybrid electrolytes with 3D bicontinuous ordered ceramic and polymer microchannels for all-solid-state batteries Zekoll, Stefanie; Marriner-Edwards, Cassian; Hekselman, A. K. Ola Energy & Environmental Science, Vol. 11, Issue 1 https://doi.org/10.1039/c7ee02723k	journal	January 2018
Polyethylene oxide film coating enhances lithium cycling efficiency of an anode-free lithium-metal battery Assegie, Addisu Alemayehu; Cheng, Ju-Hsiang; Kuo, Li-Ming Nanoscale, Vol. 10, Issue 13 https://doi.org/10.1039/c7nr09058g	journal	January 2018
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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
A Si-doped flexible self-supporting comb-like polyethylene glycol copolymer (Si-PEG) film as a polymer electrolyte for an all solid-state lithium-ion battery Ji, Xiaoxiao; Zeng, Huihui; Gong, Xianjing Journal of Materials Chemistry A, Vol. 5, Issue 46 https://doi.org/10.1039/c7ta07741f	journal	January 2017
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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
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A facile and scalable process to synthesize flexible lithium ion conductive glass-ceramic fibers He, Kun; Xie, Pu; Zu, Chengkui RSC Advances, Vol. 9, Issue 8 https://doi.org/10.1039/c8ra08401g	journal	January 2019
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Engineering the conductive carbon/PEO interface to stabilize solid polymer electrolytes for all-solid-state high voltage LiCoO ₂ batteries Liang, Jianneng; Sun, Yipeng; Zhao, Yang Journal of Materials Chemistry A, Vol. 8, Issue 5 https://doi.org/10.1039/c9ta08607b	journal	January 2020
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High cathode utilization efficiency through interface engineering in all-solid-state lithium-metal batteries Guo, Xianwei; Hao, Liangwei; Yang, Yubo Journal of Materials Chemistry A, Vol. 7, Issue 45 https://doi.org/10.1039/c9ta09935b	journal	January 2019
Realization of the Li ⁺ domain diffusion effect via constructing molecular brushes on the LLZTO surface and its application in all-solid-state lithium batteries Li, Wenwen; Sun, Changzhi; Jin, Jun Journal of Materials Chemistry A, Vol. 7, Issue 48 https://doi.org/10.1039/c9ta10400c	journal	January 2019
An anion-immobilized composite electrolyte for dendrite-free lithium metal anodes Zhao, Chen-Zi; Zhang, Xue-Qiang; Cheng, Xin-Bing Proceedings of the National Academy of Sciences, Vol. 114, Issue 42 https://doi.org/10.1073/pnas.1708489114	journal	October 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
Nano MnO ₂ immobilized covalently cross-linked chitosan and PVA based highly flexible membranes Yar, Muhammad; Masood, Aneeqa; Batool, Razia Materials Research Express, Vol. 6, Issue 8 https://doi.org/10.1088/2053-1591/ab1dcb	journal	May 2019
Dense freeze-cast Li ₇ La ₃ Zr ₂ O ₁₂ solid electrolytes with oriented open porosity and contiguous ceramic scaffold Buannic, Lucienne; Naviroj, Maninpat; Miller, Sarah M. Journal of the American Ceramic Society, Vol. 102, Issue 3 https://doi.org/10.1111/jace.15938	journal	August 2018
Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface Fu, Kun (Kelvin); Gong, Yunhui; Liu, Boyang Science Advances, Vol. 3, Issue 4 https://doi.org/10.1126/sciadv.1601659	journal	April 2017
Energy storage: The future enabled by nanomaterials Pomerantseva, Ekaterina; Bonaccorso, Francesco; Feng, Xinliang Science, Vol. 366, Issue 6468 https://doi.org/10.1126/science.aan8285	journal	November 2019
Review—Solid Electrolytes for Safe and High Energy Density Lithium-Sulfur Batteries: Promises and Challenges Judez, Xabier; Zhang, Heng; Li, Chunmei Journal of The Electrochemical Society, Vol. 165, Issue 1 https://doi.org/10.1149/2.0041801jes	journal	June 2017
Review—Li Metal Anode in Working Lithium-Sulfur Batteries Cheng, Xin-Bing; Huang, Jia-Qi; Zhang, Qiang Journal of The Electrochemical Society, Vol. 165, Issue 1 https://doi.org/10.1149/2.0111801jes	journal	June 2017
Impedance Spectroscopy Analysis of the Lithium Ion Transport through the Li ₇ La ₃ Zr ₂ O ₁₂ /P(EO) ₂₀ Li Interface Langer, Frederieke; Palagonia, Maria Sofia; Bardenhagen, Ingo Journal of The Electrochemical Society, Vol. 164, Issue 12 https://doi.org/10.1149/2.0381712jes	journal	January 2017
Combinatorial Methods for Improving Lithium Metal Cycling Efficiency Genovese, Matthew; Louli, A. J.; Weber, Rochelle Journal of The Electrochemical Society, Vol. 165, Issue 13 https://doi.org/10.1149/2.0401813jes	journal	January 2018
Free-Standing PEO/LiTFSI/LAGP Composite Electrolyte Membranes for Applications to Flexible Solid-State Lithium-Based Batteries Lee, Jeremy; Howell, Thomas; Rottmayer, Michael Journal of The Electrochemical Society, Vol. 166, Issue 2 https://doi.org/10.1149/2.1321902jes	journal	January 2019
Review : Solid Electrolytes for Safe and High Energy Density Lithium-Sulfur Batteries : Promises and Challenges Judez, Xabier; Zhang, Heng; Li, Chunmei RWTH Aachen University https://doi.org/10.18154/rwth-2021-07455	text	January 2018
Research Progress of the Solid State Lithium-Sulfur Batteries Wang, HangChao; Cao, Xin; Liu, Wen Frontiers in Energy Research, Vol. 7 https://doi.org/10.3389/fenrg.2019.00112	journal	October 2019
A versatile and membrane-less electrochemical reactor for the electrolysis of water and brine Hashemi, S. Mohammad H.; Karnakov, Petr; Hadikhani, Pooria ETH Zurich https://doi.org/10.3929/ethz-b-000344975	text	January 2019

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