Title: Oriented porous LLZO 3D structures obtained by freeze casting for battery applications

Abstract

All solid-state lithium batteries are, potentially, higher energy density and safer alternatives to conventional lithium-ion batteries (LIBs). These are particularly attractive characteristics for large-scale applications such as electric vehicles and grid energy storage systems. However, the thin film deposition techniques used to make current devices are not readily scalable, and result in low areal capacities, which translate to low practical energy densities. To overcome these deficiencies, it is necessary to design thicker electrodes similar to what are used in LIBs (30–100 μm), in which the active material is composited with an ionic conductor and an electronically conducting additive, to overcome transport limitations. In this paper, we propose a method for making such an electrode, starting with a porous scaffold, i.e. Li₇La₃Zr₂O₁₂ (LLZO), made by freeze casting, which is then infiltrated with the active material LiNi_0.6Mn_0.2Co_0.2O₂ (NMC-622) and other components. The freeze casting technique results in the formation of oriented channels with low tortuosity, which run roughly parallel to the direction of the current. The scaffolds were characterized with synchrotron X-ray micro-tomography for structural analysis, as well as synchrotron X-ray fluorescence to map the elemental distribution in the infiltrated composite. A hybrid half-cell was constructed and cycled as proof of principle,more » and it showed good stability. In addition, a bilayer structure consisting of a porous layer combined with a dense LLZO film was successfully made as a prototype of an all solid-state battery. Finally, a mathematical model was established to propose optimized scaffold structures for battery performance.« less

Authors:

Shen, Hao ^[1]; Yi, Eongyu ^[2]; Amores, Marco  ^[2];

• Search DOE PAGES for author "Amores, Marco"
• Search DOE PAGES for ORCID "0000-0002-0856-7453"

Cheng, Lei ^[3]; Tamura, Nobumichi  ^[4];

• Search DOE PAGES for author "Tamura, Nobumichi"
• Search DOE PAGES for ORCID "0000-0002-3698-2611"

Parkinson, Dilworth Y.  ^[4];

• Search DOE PAGES for author "Parkinson, Dilworth Y."
• Search DOE PAGES for ORCID "0000-0002-1817-0716"

Chen, Guoying  ^[2];

• Search DOE PAGES for author "Chen, Guoying"
• Search DOE PAGES for ORCID "0000-0002-3218-2609"

Chen, Kai  ^[5];

• Search DOE PAGES for author "Chen, Kai"
• Search DOE PAGES for ORCID "0000-0002-4917-4445"

Doeff, Marca  ^[2]

• Search DOE PAGES for author "Doeff, Marca"
• Search DOE PAGES for ORCID "0000-0002-2148-8047"

---

+ Show Author Affiliations

1. Xi'an Jiaotong Univ., Shaanxi (China). Center for Advancing Materials Performance from the Nanoscale (CAMP-Nano), State Key Lab.for Mechanical Behavior of Materials; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division
3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Energy Storage and Distributed Resources Division; Robert Bosch LLC, Sunnyvale, CA (United States). Research and Technology Center
4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Advanced Light Source (ALS)
5. Xi'an Jiaotong Univ., Shaanxi (China). Center for Advancing Materials Performance from the Nanoscale (CAMP-Nano), State Key Lab.for Mechanical Behavior of Materials

Publication Date:

Tue Aug 20 00:00:00 EDT 2019

Research Org.:

Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:

USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V); National Natural Science Foundation of China (NSFC); USDOE Office of Energy Efficiency and Renewable Energy (EERE)

OSTI Identifier:

1571137

Alternate Identifier(s):

OSTI ID: 1560235

Grant/Contract Number:  

AC02-05CH11231; 51671154; 91860109; 2016YFB0700404

Resource Type:

Accepted Manuscript

Journal Name:

Journal of Materials Chemistry. A

Additional Journal Information:

Journal Volume: 7; Journal Issue: 36; Journal ID: ISSN 2050-7488

Publisher:

Royal Society of Chemistry

Country of Publication:

United States

Language:

English

Subject:

25 ENERGY STORAGE