Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries

Fu, Kun (Kelvin); Gong, Yunhui; Hitz, Gregory T.; McOwen, Dennis W.; Li, Yiju; Xu, Shaomao; Wen, Yang; Zhang, Lei; Wang, Chengwei; Pastel, Glenn; Dai, Jiaqi; Liu, Boyang; Xie, Hua; Yao, Yonggang; Wachsman, Eric D.; Hu, Liangbing

doi:10.1039/c7ee01004d

Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries

Journal Article · Wed May 10 00:00:00 EDT 2017 · Energy & Environmental Science

DOI:https://doi.org/10.1039/c7ee01004d· OSTI ID:1433806

Fu, Kun (Kelvin) ^[1]; Gong, Yunhui ^[2]; Hitz, Gregory T. ^[2]; McOwen, Dennis W. ^[2]; Li, Yiju ^[3]; Xu, Shaomao ^[2]; Wen, Yang ^[2]; Zhang, Lei ^[2]; Wang, Chengwei ^[2]; Pastel, Glenn ^[3]; Dai, Jiaqi ^[3]; Liu, Boyang ^[3]; Xie, Hua ^[3]; Yao, Yonggang ^[3]; ^[2]; ^[2]

Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering; University of Maryland
Univ. of Maryland, College Park, MD (United States). Energy Research Center. Dept. of Materials Science and Engineering
Univ. of Maryland, College Park, MD (United States). Dept. of Materials Science and Engineering

To simultaneously address the challenges of chemical/physical short circuits and electrode volume variation, we demonstrate in this paper a three-dimensional (3D) bilayer garnet solid-state electrolyte framework for advanced Li metal batteries. The dense layer is reduced in thickness to a few microns and still retains good mechanical stability, thereby enabling the safe use of Li metal anodes. The thick porous layer acts as a mechanical support for the thin dense layer which serves as a host for high loading of cathode materials and provides pathways for continuous ion transport. Results show that the integrated sulfur cathode loading can reach >7 mg cm^-2 while the proposed hybrid Li–S battery exhibits a high initial coulombic efficiency (>99.8%) and high average coulombic efficiency (>99%) during the subsequent cycles. Finally, this electrolyte framework represents a promising strategy to revolutionize Li-metal batteries by transitioning to all-solid-state batteries and can be extended to other cathode materials.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: National Aeronautics and Space Administration (NASA) (United States); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: EE0006860

OSTI ID:: 1433806

Journal Information:: Energy & Environmental Science, Journal Name: Energy & Environmental Science Journal Issue: 7 Vol. 10; ISSN 1754-5692

Publisher:: Royal Society of ChemistryCopyright Statement

Country of Publication:: United States

Language:: English

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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
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
Vanadium-based nanowires for sodium-ion batteries Cheng, Yu; Xia, Yangyang; Chen, Yiming Nanotechnology, Vol. 30, Issue 19 https://doi.org/10.1088/1361-6528/aaff82	journal	February 2019
Integrated solid electrolyte with porous cathode by facilely one-step sintering for an all-solid-state Li–O ₂ battery Li, Chao; Liu, Yijie; Li, Bojie Nanotechnology, Vol. 30, Issue 36 https://doi.org/10.1088/1361-6528/ab226f	journal	June 2019
Carbon-Metal Oxide Nanocomposites as Lithium-Sulfur Battery Cathodes Zhu, Sheng; Li, Yan Functional Materials for Next-Generation Rechargeable Batteries https://doi.org/10.1142/9789811230677_0002	book	February 2021
Carbon-metal oxide nanocomposites as lithium-sulfur battery cathodes Zhu, Sheng; Li, Yan Functional Materials Letters, Vol. 11, Issue 06 https://doi.org/10.1142/s1793604718300074	journal	December 2018
Perspective—Lithium-Sulfur Batteries Bonnick, Patrick; Nagai, Erika; Muldoon, John Journal of The Electrochemical Society, Vol. 165, Issue 1 https://doi.org/10.1149/2.0031801jes	journal	June 2017
Electrochemical Stability of Garnet-Type Li ₇ La _2.75 Ca _0.25 Zr _1.75 Nb _0.25 O ₁₂ with and without Atomic Layer Deposited-Al ₂ O ₃ under CO ₂ and Humidity Hofstetter, Kyle; Samson, Alfred Junio; Dai, Jiaqi Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0201910jes	journal	January 2019
Ab Initio Study of the Interface of the Solid-State Electrolyte Li ₉ N ₂ Cl ₃ with a Li-Metal Electrode Galvez-Aranda, Diego E.; Seminario, Jorge M. Journal of The Electrochemical Society, Vol. 166, Issue 10 https://doi.org/10.1149/2.0211910jes	journal	January 2019
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
All-Solid-State Lithium Battery Fitted with Polymer Electrolyte Enhanced by Solid Plasticizer and Conductive Ceramic Filler Chen, Fei; Zha, Wenping; Yang, Dunjie Journal of The Electrochemical Society, Vol. 165, Issue 14 https://doi.org/10.1149/2.1371814jes	journal	January 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
Methods to Improve Lithium Metal Anode for Li-S Batteries Xiong, Xiaosong; Yan, Wenqi; You, Chaolin Frontiers in Chemistry, Vol. 7 https://doi.org/10.3389/fchem.2019.00827	journal	December 2019
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
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

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