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Title: Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes

Abstract

Abstract Solid‐state lithium batteries are promising for safety and energy density compared with traditional lithium‐ion batteries. However, the large interfacial resistance between the electrode and electrolyte is a bottleneck to achieving high‐performance solid‐state batteries. Engineered electrode structures with a porous scaffold of the solid electrolyte material are promising to lower the interfacial resistance and provide a mechanical support for a thin solid electrolyte layer. In this work, two ceramic processing techniques are used to fabricate porous/dense bilayer architectures based on a Li 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO) Li‐garnet material. Finger‐like vertically aligned pores are created by the phase inversion (PI) process. A water bath presaturated with Li salt prevents Li loss during the PI solvent exchange step. Pore size and porosity can be optimized by adjusting the bath temperature. The high shear compaction process was used to prepare LLZO tapes with 40, 60, and 80 vol% poreformer. The porosity of the tapes after sintering is 39.5%, 58.4%, and 75.4%, respectively. Microtomography exhibits the porosity, pore shape, and pore distribution of the tapes. A typical cathode material LiNi 0.33 Mn 0.33 Co 0.33 O 2  (NMC) is filled into the pores via vacuum infiltration, and a densemore » cathode layer is formed within the garnet scaffold.« less

Authors:
ORCiD logo [1];  [1];  [1];  [1]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Laboratory Directed Research and Development (LDRD) Program
OSTI Identifier:
1864178
Alternate Identifier(s):
OSTI ID: 1810887
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Ceramic Society
Additional Journal Information:
Journal Volume: 105; Journal Issue: 1; Journal ID: ISSN 0002-7820
Publisher:
American Ceramic Society
Country of Publication:
United States
Language:
English
Subject:
25 ENERGY STORAGE; garnet; infiltration; LLZO; porous scaffold; solid-state battery

Citation Formats

Shen, Fengyu, Jonson, Robert A., Parkinson, Dilworth Y., and Tucker, Michael C. Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes. United States: N. p., 2021. Web. doi:10.1111/jace.18037.
Shen, Fengyu, Jonson, Robert A., Parkinson, Dilworth Y., & Tucker, Michael C. Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes. United States. https://doi.org/10.1111/jace.18037
Shen, Fengyu, Jonson, Robert A., Parkinson, Dilworth Y., and Tucker, Michael C. Sat . "Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes". United States. https://doi.org/10.1111/jace.18037. https://www.osti.gov/servlets/purl/1864178.
@article{osti_1864178,
title = {Preparing Li-garnet electrodes with engineered structures by phase inversion and high shear compaction processes},
author = {Shen, Fengyu and Jonson, Robert A. and Parkinson, Dilworth Y. and Tucker, Michael C.},
abstractNote = {Abstract Solid‐state lithium batteries are promising for safety and energy density compared with traditional lithium‐ion batteries. However, the large interfacial resistance between the electrode and electrolyte is a bottleneck to achieving high‐performance solid‐state batteries. Engineered electrode structures with a porous scaffold of the solid electrolyte material are promising to lower the interfacial resistance and provide a mechanical support for a thin solid electrolyte layer. In this work, two ceramic processing techniques are used to fabricate porous/dense bilayer architectures based on a Li 6.25 Al 0.25 La 3 Zr 2 O 12 (LLZO) Li‐garnet material. Finger‐like vertically aligned pores are created by the phase inversion (PI) process. A water bath presaturated with Li salt prevents Li loss during the PI solvent exchange step. Pore size and porosity can be optimized by adjusting the bath temperature. The high shear compaction process was used to prepare LLZO tapes with 40, 60, and 80 vol% poreformer. The porosity of the tapes after sintering is 39.5%, 58.4%, and 75.4%, respectively. Microtomography exhibits the porosity, pore shape, and pore distribution of the tapes. A typical cathode material LiNi 0.33 Mn 0.33 Co 0.33 O 2  (NMC) is filled into the pores via vacuum infiltration, and a dense cathode layer is formed within the garnet scaffold.},
doi = {10.1111/jace.18037},
journal = {Journal of the American Ceramic Society},
number = 1,
volume = 105,
place = {United States},
year = {Sat Jul 17 00:00:00 EDT 2021},
month = {Sat Jul 17 00:00:00 EDT 2021}
}

Works referenced in this record:

Structural and Electrochemical Consequences of Al and Ga Cosubstitution in Li 7 La 3 Zr 2 O 12 Solid Electrolytes
journal, March 2016

  • Rettenwander, Daniel; Redhammer, Günther; Preishuber-Pflügl, Florian
  • Chemistry of Materials, Vol. 28, Issue 7
  • DOI: 10.1021/acs.chemmater.6b00579

Ionic Conductivity and Air Stability of Al-Doped Li 7 La 3 Zr 2 O 12 Sintered in Alumina and Pt Crucibles
journal, February 2016

  • Xia, Wenhao; Xu, Biyi; Duan, Huanan
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 8
  • DOI: 10.1021/acsami.5b12186

3D-Printing Electrolytes for Solid-State Batteries
journal, March 2018

  • McOwen, Dennis W.; Xu, Shaomao; Gong, Yunhui
  • Advanced Materials, Vol. 30, Issue 18
  • DOI: 10.1002/adma.201707132

Cost-Effective Single Step Cofiring Process for Manufacturing Solid Oxide Fuel Cells Using HSC™ Anode
journal, January 2010

  • Yoon, Kyung Joong; Ye, Guosheng; Gopalan, Srikanth
  • Journal of Fuel Cell Science and Technology, Vol. 7, Issue 2
  • DOI: 10.1115/1.3177449

Method Using Water-Based Solvent to Prepare Li 7 La 3 Zr 2 O 12 Solid Electrolytes
journal, April 2018

  • Huang, Xiao; Lu, Yang; Jin, Jun
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 20
  • DOI: 10.1021/acsami.8b01961

All-Solid-State Batteries Using Rationally Designed Garnet Electrolyte Frameworks
journal, December 2019

  • Yi, Eongyu; Shen, Hao; Heywood, Stephen
  • ACS Applied Energy Materials, Vol. 3, Issue 1
  • DOI: 10.1021/acsaem.9b02101

Benchmarking the performance of all-solid-state lithium batteries
journal, March 2020


Batteries Safety: Recent Progress and Current Challenges
journal, September 2019

  • Ould Ely, Teyeb; Kamzabek, Dana; Chakraborty, Dhritiman
  • Frontiers in Energy Research, Vol. 7
  • DOI: 10.3389/fenrg.2019.00071

Application and modification of polysulfone membranes
journal, August 2018

  • Kheirieh, Sareh; Asghari, Morteza; Afsari, Morteza
  • Reviews in Chemical Engineering, Vol. 34, Issue 5
  • DOI: 10.1515/revce-2017-0011

Cubic phases of garnet-type Li7La3Zr2O12: the role of hydration
journal, January 2013

  • Larraz, G.; Orera, A.; Sanjuán, M. L.
  • Journal of Materials Chemistry A, Vol. 1, Issue 37
  • DOI: 10.1039/c3ta11996c

Practical Challenges and Future Perspectives of All-Solid-State Lithium-Metal Batteries
journal, April 2019


Reduced Energy Barrier for Li+ Transport Across Grain Boundaries with Amorphous Domains in LLZO Thin Films
journal, July 2020


Scalable Freeze-Tape-Casting Fabrication and Pore Structure Analysis of 3D LLZO Solid-State Electrolytes
journal, December 2019

  • Shen, Hao; Yi, Eongyu; Heywood, Stephen
  • ACS Applied Materials & Interfaces, Vol. 12, Issue 3
  • DOI: 10.1021/acsami.9b11780

Steam electrolysis in a solid oxide electrolysis cell fabricated by the phase-inversion tape casting method
journal, December 2015


A perspective on low-temperature solid oxide fuel cells
journal, January 2016

  • Gao, Zhan; Mogni, Liliana V.; Miller, Elizabeth C.
  • Energy & Environmental Science, Vol. 9, Issue 5
  • DOI: 10.1039/C5EE03858H

Continuous plating/stripping behavior of solid-state lithium metal anode in a 3D ion-conductive framework
journal, March 2018

  • Yang, Chunpeng; Zhang, Lei; Liu, Boyang
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 15
  • DOI: 10.1073/pnas.1719758115

Composite Electrode Ink Formulation for All Solid-State Batteries
journal, January 2019

  • Shen, Fengyu; Dixit, Marm B.; Zaman, Wahid
  • Journal of The Electrochemical Society, Vol. 166, Issue 14
  • DOI: 10.1149/2.0141914jes

Oriented porous LLZO 3D structures obtained by freeze casting for battery applications
journal, January 2019

  • Shen, Hao; Yi, Eongyu; Amores, Marco
  • Journal of Materials Chemistry A, Vol. 7, Issue 36
  • DOI: 10.1039/C9TA06520B

Polymer Template Synthesis of Soft, Light, and Robust Oxide Ceramic Films
journal, May 2019


Research Progresses of Garnet-Type Solid Electrolytes for Developing All-Solid-State Li Batteries
journal, June 2020


Three-dimensional bilayer garnet solid electrolyte based high energy density lithium metal–sulfur batteries
journal, January 2017

  • Fu, Kun (Kelvin); Gong, Yunhui; Hitz, Gregory T.
  • Energy & Environmental Science, Vol. 10, Issue 7
  • DOI: 10.1039/C7EE01004D

Elevated-Temperature 3D Printing of Hybrid Solid-State Electrolyte for Li-Ion Batteries
journal, August 2018


Long term durability test and post mortem for metal-supported solid oxide electrolysis cells
journal, October 2020


Preparation and Characterization of Membranes Formed by Nonsolvent Induced Phase Separation: A Review
journal, April 2011

  • Guillen, Gregory R.; Pan, Yinjin; Li, Minghua
  • Industrial & Engineering Chemistry Research, Vol. 50, Issue 7
  • DOI: 10.1021/ie101928r

Correction: Li 7 La 3 Zr 2 O 12 ceramic nanofiber-incorporated composite polymer electrolytes for lithium metal batteries
journal, January 2019

  • Li, Yang; Zhang, Wei; Dou, Qianqian
  • Journal of Materials Chemistry A, Vol. 7, Issue 8
  • DOI: 10.1039/C9TA90038A

Low-temperature densification of Al-doped Li 7 La 3 Zr 2 O 12 : a reliable and controllable synthesis of fast-ion conducting garnets
journal, January 2017

  • El-Shinawi, Hany; Paterson, Gary W.; MacLaren, Donald A.
  • Journal of Materials Chemistry A, Vol. 5, Issue 1
  • DOI: 10.1039/C6TA06961D

Toward Safe Lithium Metal Anode in Rechargeable Batteries: A Review
journal, July 2017


Thick Electrode Batteries: Principles, Opportunities, and Challenges
journal, July 2019

  • Kuang, Yudi; Chen, Chaoji; Kirsch, Dylan
  • Advanced Energy Materials, Vol. 9, Issue 33
  • DOI: 10.1002/aenm.201901457

Morphology Control of Polysulfone Membranes in Filtration Processes: a Critical Review
journal, February 2015


Dense freeze-cast Li 7 La 3 Zr 2 O 12 solid electrolytes with oriented open porosity and contiguous ceramic scaffold
journal, August 2018

  • Buannic, Lucienne; Naviroj, Maninpat; Miller, Sarah M.
  • Journal of the American Ceramic Society, Vol. 102, Issue 3
  • DOI: 10.1111/jace.15938

Perovskite Membranes with Vertically Aligned Microchannels for All-Solid-State Lithium Batteries
journal, August 2018

  • Jiang, Zhouyang; Xie, Huiqi; Wang, Suqing
  • Advanced Energy Materials, Vol. 8, Issue 27
  • DOI: 10.1002/aenm.201801433

Optimization of Tape Casting for Fabrication of Li 6.25 Al 0.25 La 3 Zr 2 O 12 Sheets
journal, May 2021


Optimization of anode structure for intermediate temperature solid oxide fuel cell via phase-inversion cotape casting
journal, April 2017

  • Lin, Jie; Miao, Guoshuan; Xia, Changrong
  • Journal of the American Ceramic Society, Vol. 100, Issue 8
  • DOI: 10.1111/jace.14907

Effect of Pore Connectivity on Li Dendrite Propagation within LLZO Electrolytes Observed with Synchrotron X-ray Tomography
journal, March 2018


The Li-Ion Rechargeable Battery: A Perspective
journal, January 2013

  • Goodenough, John B.; Park, Kyu-Sung
  • Journal of the American Chemical Society, Vol. 135, Issue 4
  • DOI: 10.1021/ja3091438

High-rate lithium cycling in a scalable trilayer Li-garnet-electrolyte architecture
journal, January 2019


Status and challenges in enabling the lithium metal electrode for high-energy and low-cost rechargeable batteries
journal, December 2017


Three-Dimensional Garnet Framework-Reinforced Solid Composite Electrolytes with High Lithium-Ion Conductivity and Excellent Stability
journal, July 2019

  • Li, Zhuo; Sha, Wu-Xin; Guo, Xin
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 30
  • DOI: 10.1021/acsami.9b07830

Preparation of Nano- and Microstructured Garnet Li 7 La 3 Zr 2 O 12 Solid Electrolytes for Li-Ion Batteries via Cellulose Templating
journal, October 2016

  • Gordon, Zachary D.; Yang, Ting; Gomes Morgado, Guilherme Bruno
  • ACS Sustainable Chemistry & Engineering, Vol. 4, Issue 12
  • DOI: 10.1021/acssuschemeng.6b01032

Novel highly scalable carbon nanotube-strengthened ceramics by high shear compaction and spark plasma sintering
journal, September 2015