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; Xu, Shaomao; Yao, Yonggang; Luo, Wei; Wang, Chengwei; Lacey, Steven D.; Dai, Jiaqi; Chen, Yanan; Mo, Yifei; Wachsman, Eric; Hu, Liangbing

doi:10.1126/sciadv.1601659

Title: Toward garnet electrolyte–based Li metal batteries: An ultrathin, highly effective, artificial solid-state electrolyte/metallic Li interface

Journal Article · 07 April 2017 · Science Advances

DOI: https://doi.org/10.1126/sciadv.1601659 · OSTI ID:1425393

Fu, Kun (Kelvin) ^[1]; Gong, Yunhui ^[1]; Liu, Boyang ^[1]; Xu, Shaomao ^[1]; Yao, Yonggang ^[1];

^[1]; Wang, Chengwei ^[1]; Lacey, Steven D. ^[1]; Dai, Jiaqi ^[1]; Chen, Yanan ^[1];

^[1]; Wachsman, Eric ^[1]; Hu, Liangbing ^[1]

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

Solid-state batteries are a promising option toward high energy and power densities due to the use of lithium (Li) metal as an anode. Among all solid electrolyte materials ranging from sulfides to oxides and oxynitrides, cubic garnet–type Li₇La₃Zr₂O₁₂ (LLZO) ceramic electrolytes are superior candidates because of their high ionic conductivity (10^-3 to 10^-4 S/cm) and good stability against Li metal. However, garnet solid electrolytes generally have poor contact with Li metal, which causes high resistance and uneven current distribution at the interface. To address this challenge, we demonstrate a strategy to engineer the garnet solid electrolyte and the Li metal interface by forming an intermediary Li-metal alloy, which changes the wettability of the garnet surface (lithiophobic to lithiophilic) and reduces the interface resistance by more than an order of magnitude: 950 ohm·cm2 for the pristine garnet/Li and 75 ohm·cm² for the surface-engineered garnet/Li. Li₇La_2.75Ca_0.25Zr_1.75Nb_0.25O₁₂ (LLCZN) was selected as the solid-state electrolyte (SSE) in this work because of its low sintering temperature, stabilized cubic garnet phase, and high ionic conductivity. This low area-specific resistance enables a solid-state garnet SSE/Li metal configuration and promotes the development of a hybrid electrolyte system. The hybrid system uses the improved solid-state garnet SSE Li metal anode and a thin liquid electrolyte cathode interfacial layer. This work provides new ways to address the garnet SSE wetting issue against Li and get more stable cell performances based on the hybrid electrolyte system for Li-ion, Li-sulfur, and Li-oxygen batteries toward the next generation of Li metal batteries.

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

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

Grant/Contract Number:: EE0006860

OSTI ID:: 1425393

Journal Information:: Science Advances, Vol. 3, Issue 4; ISSN 2375-2548

Publisher:: AAASCopyright Statement

Country of Publication:: United States

Language:: English

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Synthesis and Properties of NaSICON‐type LATP and LAGP Solid Electrolytes DeWees, Rachel; Wang, Hui ChemSusChem, Vol. 12, Issue 16 https://doi.org/10.1002/cssc.201900725	journal	July 2019
Design Principles of the Anode–Electrolyte Interface for All Solid‐State Lithium Metal Batteries Shen, Zeyu; Zhang, Weidong; Zhu, Guannan Small Methods, Vol. 4, Issue 1 https://doi.org/10.1002/smtd.201900592	journal	October 2019
Using in operando diffraction to relate lattice strain with degradation mechanism in a NMC battery Jha, Shikhar Krishn; Charalambous, Harry; Okasinski, John S. Journal of Materials Science, Vol. 54, Issue 3 https://doi.org/10.1007/s10853-018-3007-8	journal	October 2018
Mechanistic understanding and strategies to design interfaces of solid electrolytes: insights gained from transmission electron microscopy Hood, Zachary D.; Chi, Miaofang Journal of Materials Science, Vol. 54, Issue 15 https://doi.org/10.1007/s10853-019-03633-2	journal	May 2019
Infiltrating lithium into carbon cloth decorated with zinc oxide arrays for dendrite-free lithium metal anode Wang, Xianshu; Pan, Zhenghui; Wu, Yang Nano Research, Vol. 12, Issue 3 https://doi.org/10.1007/s12274-018-2245-z	journal	November 2018
Rechargeable solid-state Li-air batteries: a status report Yang, Chu-Shu; Gao, Kang-Ning; Zhang, Xiao-Ping Rare Metals, Vol. 37, Issue 6 https://doi.org/10.1007/s12598-018-1036-8	journal	April 2018
Solid-State Electrolytes for Lithium-Ion Batteries: Fundamentals, Challenges and Perspectives Zhao, Wenjia; Yi, Jin; He, Ping Electrochemical Energy Reviews, Vol. 2, Issue 4 https://doi.org/10.1007/s41918-019-00048-0	journal	August 2019
Diatomite derived hierarchical hybrid anode for high performance all-solid-state lithium metal batteries Zhou, Fei; Li, Zheng; Lu, Yu-Yang Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10473-w	journal	June 2019
Tuning wettability of molten lithium via a chemical strategy for lithium metal anodes Wang, Shu-Hua; Yue, Junpei; Dong, Wei Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12938-4	journal	October 2019
A low ride on processing temperature for fast lithium conduction in garnet solid-state battery films Pfenninger, Reto; Struzik, Michal; Garbayo, Iñigo Nature Energy, Vol. 4, Issue 6 https://doi.org/10.1038/s41560-019-0384-4	journal	May 2019
Sur-/interfacial regulation in all-solid-state rechargeable Li-ion batteries based on inorganic solid-state electrolytes: advances and perspectives Liang, Longwei; Sun, Xuan; Zhang, Jinyang Materials Horizons, Vol. 6, Issue 5 https://doi.org/10.1039/c8mh01593g	journal	January 2019
Acid induced conversion towards a robust and lithiophilic interface for Li–Li ₇ La ₃ Zr ₂ O ₁₂ solid-state batteries Ruan, Yadong; Lu, Yang; Huang, Xiao Journal of Materials Chemistry A, Vol. 7, Issue 24 https://doi.org/10.1039/c9ta01911a	journal	January 2019
Single-ion conducting artificial solid electrolyte interphase layers for dendrite-free and highly stable lithium metal anodes Deng, Kuirong; Han, Dongmei; Ren, Shan Journal of Materials Chemistry A, Vol. 7, Issue 21 https://doi.org/10.1039/c9ta02407g	journal	January 2019
Oriented porous LLZO 3D structures obtained by freeze casting for battery applications Shen, Hao; Yi, Eongyu; Amores, Marco Journal of Materials Chemistry A, Vol. 7, Issue 36 https://doi.org/10.1039/c9ta06520b	journal	January 2019
Rationalizing the interphase stability of Li\|doped-Li ₇ La ₃ Zr ₂ O ₁₂ via automated reaction screening and machine learning Liu, Bo; Yang, Jiong; Yang, Hongliang Journal of Materials Chemistry A, Vol. 7, Issue 34 https://doi.org/10.1039/c9ta06748e	journal	January 2019
Continuous plating/stripping behavior of solid-state lithium metal anode in a 3D ion-conductive framework Yang, Chunpeng; Zhang, Lei; Liu, Boyang Proceedings of the National Academy of Sciences, Vol. 115, Issue 15 https://doi.org/10.1073/pnas.1719758115	journal	March 2018
Stitching h-BN by atomic layer deposition of LiF as a stable interface for lithium metal anode Xie, Jin; Liao, Lei; Gong, Yongji Science Advances, Vol. 3, Issue 11 https://doi.org/10.1126/sciadv.aao3170	journal	November 2017
Upgrading traditional liquid electrolyte via in situ gelation for future lithium metal batteries Liu, Feng-Quan; Wang, Wen-Peng; Yin, Ya-Xia Science Advances, Vol. 4, Issue 10 https://doi.org/10.1126/sciadv.aat5383	journal	October 2018
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Communication—Demonstration and Electrochemistry of a Self-Forming Solid State Rechargeable LiI(HPN) ₂ Based Li/I ₂ Battery Abraham, Alyson; Huang, Jianping; Smith, Paul F. Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.0371810jes	journal	January 2018
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
Towards Mixed Ionic and Electronic Conducting Li-Stuffed Garnets Samson, Alfred Junio; Hofstetter, Kyle; Wachsman, Eric Journal of The Electrochemical Society, Vol. 165, Issue 10 https://doi.org/10.1149/2.1001810jes	journal	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
Mixed Ionic and Electronic Conductor for Li-Metal Anode Protection Yan, Jianhua; Yu, Jianyong; Ding, Bin Advanced Materials, Vol. 30, Issue 7 https://doi.org/10.1002/adma.201705105	journal	January 2018
Borohydride-Scaffolded Li/Na/Mg Fast Ionic Conductors for Promising Solid-State Electrolytes Cuan, Jing; Zhou, You; Zhou, Tengfei Advanced Materials, Vol. 31, Issue 1 https://doi.org/10.1002/adma.201803533	journal	October 2018
Interphases, Interfaces, and Surfaces of Active Materials in Rechargeable Batteries and Perovskite Solar Cells Liu, Chaofeng; Yuan, Jifeng; Masse, Robert Advanced Materials https://doi.org/10.1002/adma.201905245	journal	January 2020
A Material Perspective of Rechargeable Metallic Lithium Anodes Li, Bin; Wang, Ying; Yang, Shubin Advanced Energy Materials, Vol. 8, Issue 13 https://doi.org/10.1002/aenm.201702296	journal	February 2018
Perovskite Membranes with Vertically Aligned Microchannels for All-Solid-State Lithium Batteries Jiang, Zhouyang; Xie, Huiqi; Wang, Suqing Advanced Energy Materials, Vol. 8, Issue 27 https://doi.org/10.1002/aenm.201801433	journal	August 2018
Constructing Multifunctional Interphase between Li _1.4 Al _0.4 Ti _1.6 (PO ₄ ) ₃ and Li Metal by Magnetron Sputtering for Highly Stable Solid‐State Lithium Metal Batteries Hao, Xiaoge; Zhao, Qiang; Su, Shiming Advanced Energy Materials, Vol. 9, Issue 34 https://doi.org/10.1002/aenm.201901604	journal	July 2019
Interfacial Incompatibility and Internal Stresses in All‐Solid‐State Lithium Ion Batteries He, Yanming; Lu, Chuanyang; Liu, Shan Advanced Energy Materials, Vol. 9, Issue 36 https://doi.org/10.1002/aenm.201901810	journal	August 2019
Diffusion Limitation of Lithium Metal and Li–Mg Alloy Anodes on LLZO Type Solid Electrolytes as a Function of Temperature and Pressure Krauskopf, Thorben; Mogwitz, Boris; Rosenbach, Carolin Advanced Energy Materials, Vol. 9, Issue 44 https://doi.org/10.1002/aenm.201902568	journal	October 2019
Solid‐State Lithium Batteries: Bipolar Design, Fabrication, and Electrochemistry Jung, Kyu‐Nam; Shin, Hyun‐Seop; Park, Min‐Sik ChemElectroChem, Vol. 6, Issue 15 https://doi.org/10.1002/celc.201900736	journal	May 2019
A review of solid electrolytes for safe lithium-sulfur batteries Sun, Ying-Zhi; Huang, Jia-Qi; Zhao, Chen-Zi Science China Chemistry, Vol. 60, Issue 12 https://doi.org/10.1007/s11426-017-9164-2	journal	November 2017
Stabilizing a high-voltage LiNi _0.5 Mn _1.5 O ₄ cathode towards all solid state batteries: a Li–Al–Ti–P–O solid electrolyte nano-shell with a host material Li, Li; Zhao, Rui; Xu, Tinghua Nanoscale, Vol. 11, Issue 18 https://doi.org/10.1039/c9nr01655d	journal	January 2019
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A borate decorated anion-immobilized solid polymer electrolyte for dendrite-free, long-life Li metal batteries Ma, Cheng; Feng, Yiming; Xing, Fangzhou Journal of Materials Chemistry A, Vol. 7, Issue 34 https://doi.org/10.1039/c9ta07551h	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
Building Better Batteries in the Solid State: A Review Mauger, Alain; Julien, Christian M.; Paolella, Andrea Materials, Vol. 12, Issue 23, p. 3892 https://doi.org/10.3390/ma12233892	journal	November 2019
Transient Behavior of the Metal Interface in Lithium Metal-Garnet Batteries Fu, Kun Kelvin; Gong, Yunhui; Fu, Zhezhen Angewandte Chemie, Vol. 129, Issue 47 https://doi.org/10.1002/ange.201708637	journal	October 2017
A Perovskite Electrolyte That Is Stable in Moist Air for Lithium-Ion Batteries Li, Yutao; Xu, Henghui; Chien, Po-Hsiu Angewandte Chemie International Edition, Vol. 57, Issue 28 https://doi.org/10.1002/anie.201804114	journal	June 2018
Graphitic Carbon Nitride (g‐C ₃ N ₄ ): An Interface Enabler for Solid‐State Lithium Metal Batteries Huang, Ying; Chen, Bo; Duan, Jian Angewandte Chemie International Edition, Vol. 59, Issue 9 https://doi.org/10.1002/anie.201914417	journal	January 2020
Nanostructured Metal–Organic Framework (MOF)‐Derived Solid Electrolytes Realizing Fast Lithium Ion Transportation Kinetics in Solid‐State Batteries Wu, Jian‐Fang; Guo, Xin Small, Vol. 15, Issue 27 https://doi.org/10.1002/smll.201902429	journal	April 2019
In situ X-ray photoelectron spectroscopy investigation of the solid electrolyte interphase in a Li/Li6.4Ga0.2La3Zr2O12/LiFePO4 all-solid-state battery Liu, Zhen; Li, Guozhu; Borodin, Andriy Journal of Solid State Electrochemistry, Vol. 23, Issue 7 https://doi.org/10.1007/s10008-019-04296-4	journal	June 2019
Recent Progress in All-Solid-State Lithium−Sulfur Batteries Using High Li-Ion Conductive Solid Electrolytes Umeshbabu, Ediga; Zheng, Bizhu; Yang, Yong Electrochemical Energy Reviews, Vol. 2, Issue 2 https://doi.org/10.1007/s41918-019-00029-3	journal	February 2019
High Li ⁺ transference gel interface between solid-oxide electrolyte and cathode for quasi-solid lithium-ion batteries Subramani, Ramesh; Tseng, Yu-Hsien; Lee, Yuh-Lang Journal of Materials Chemistry A, Vol. 7, Issue 19 https://doi.org/10.1039/c9ta02515d	journal	January 2019
Communication—Li/Li ₇ La ₃ Zr ₂ O ₁₂ Interfacial Modification by Constructing a Layer of Cu-Li Alloy Xiang, Xing; Cao, Shiyu; Chen, Fei Journal of The Electrochemical Society, Vol. 166, Issue 13 https://doi.org/10.1149/2.0651913jes	journal	January 2019
Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li7La3Zr2O12 Substituted with Iron Paulus, Anja; Kammler, Simon; Heuer, Sabrina RWTH Aachen University https://doi.org/10.18154/rwth-2019-01971	text	January 2019
Graphitic Carbon Nitride (g‐C ₃ N ₄ ): An Interface Enabler for Solid‐State Lithium Metal Batteries Huang, Ying; Chen, Bo; Duan, Jian Angewandte Chemie, Vol. 132, Issue 9 https://doi.org/10.1002/ange.201914417	journal	January 2020
Nanostructured Metal–Organic Framework (MOF)‐Derived Solid Electrolytes Realizing Fast Lithium Ion Transportation Kinetics in Solid‐State Batteries Wu, Jian‐Fang; Guo, Xin Small, Vol. 15, Issue 5 https://doi.org/10.1002/smll.201804413	journal	January 2019
Engineering stable interfaces for three-dimensional lithium metal anodes Xie, Jin; Wang, Jiangyan; Lee, Hye Ryoung Science Advances, Vol. 4, Issue 7 https://doi.org/10.1126/sciadv.aat5168	journal	July 2018
Review—Practical Challenges Hindering the Development of Solid State Li Ion Batteries Kerman, Kian; Luntz, Alan; Viswanathan, Venkatasubramanian Journal of The Electrochemical Society, Vol. 164, Issue 7 https://doi.org/10.1149/2.1571707jes	journal	January 2017
A Perovskite Electrolyte That Is Stable in Moist Air for Lithium‐Ion Batteries Li, Yutao; Xu, Henghui; Chien, Po‐Hsiu Angewandte Chemie, Vol. 130, Issue 28 https://doi.org/10.1002/ange.201804114	journal	June 2018
A 3D Lithium/Carbon Fiber Anode with Sustained Electrolyte Contact for Solid‐State Batteries Zhang, Ying; Shi, Yang; Hu, Xin‐Cheng Advanced Energy Materials, Vol. 10, Issue 3 https://doi.org/10.1002/aenm.201903325	journal	December 2019
Sol Gel vs Solid State Synthesis of the Fast Lithium-Ion Conducting Solid State Electrolyte Li ₇ La ₃ Zr ₂ O ₁₂ Substituted with Iron Paulus, Anja; Kammler, Simon; Heuer, Sabrina Journal of The Electrochemical Society, Vol. 166, Issue 3 https://doi.org/10.1149/2.0641903jes	journal	January 2019
Diatomite derived hierarchical hybrid anode for high performance all-solid-state lithium metal batteries Zhou, Fei; Li, Zheng; Lu, Yu-Yang Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-10473-w	journal	June 2019
Tuning wettability of molten lithium via a chemical strategy for lithium metal anodes Wang, Shu-Hua; Yue, Junpei; Dong, Wei Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-12938-4	journal	October 2019
Engineering stable interfaces for three-dimensional lithium metal anodes Xie, Jin; Wang, Jiangyan; Lee, Hye Ryoung Science Advances, Vol. 4, Issue 7 https://doi.org/10.1126/sciadv.aat5168	journal	July 2018
Making Sense of Complex Carbon and Metal/Carbon Systems by Secondary Electron Hyperspectral Imaging Abrams, Kerry J.; Dapor, Maurizio; Stehling, Nicola Weinheim : Wiley-VCH https://doi.org/10.34657/9127	text	January 2019

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