All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating

Ren, Yaoyu; Wachsman, Eric D.

doi:10.1149/1945-7111/ac644f

Title: All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating

Journal Article · 01 April 2022 · Journal of the Electrochemical Society

DOI:https://doi.org/10.1149/1945-7111/ac644f· OSTI ID:1980879

;

Li₇La₃Zr₂O₁₂(LLZO) garnet-type lithium-ion conductors are being investigated as a promising solid electrolyte for solid-state lithium batteries. To enable a functional all-solid-state configuration intensive investigations are needed to reduce the cathode/electrolyte interfacial resistance which contributes the most to cell performance loss. Among the commercial cathode materials investigated so far, LiCoO₂(LCO) is one of the most stable with garnet electrolytes as only a superficial reaction has been detected between the two materials. However, even this minor reaction would block the Li-ion transport through the interface, resulting in deteriorated cell performance. In this work, we demonstrate that a thin aluminum oxide layer (5 nm) can be an effective interlayer to impede the formation of a harmful interphase and enable facile Li-ion transfer between LCO and the LLZO garnet. Room-temperature-sputtered LCO thin films were employed to form an interface with the garnet electrolyte and annealed at 800 °C to reveal the effect of the interfacial reaction on the Li-ion transfer across the interface. An aluminum oxide layer was then introduced between LCO and the garnet electrolyte by sputtering a metallic aluminum layer which is then annealed together with the upper LCO layer in oxygen, or by direct atomic layer deposition of the oxide. Compared to the LCO/LLZO/Li cells without an aluminum oxide interlayer, those with the interlayer exhibited improved performance, i.e., a stable discharge capacity of up to 90 mAh/(g LCO) at a C/10 rate, a rate capability up to 1.68C and a stable galvanostatic cycling at 0.1C for over 100 cycles with a discharge capacity fade rate of 0.15% per cycle. It was determined that aluminum diffused into the LCO layer after preventing the initial detrimental reaction between LCO and the LLZO garnet from happening during high temperature annealing, suggesting that the coating does not have to remain a physically blocking layer during cycling to function.

Cite

Export

Save

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

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

DOE Contract Number:: EE0008858

OSTI ID:: 1980879

Journal Information:: Journal of the Electrochemical Society, Vol. 169, Issue 4; ISSN 0013-4651

Publisher:: IOP Publishing

Country of Publication:: United States

Language:: English

References (45)

Oxide Electrolytes for Lithium Batteries Ren, Yaoyu; Chen, Kai; Chen, Rujun Journal of the American Ceramic Society, Vol. 98, Issue 12 https://doi.org/10.1111/jace.13844	journal	September 2015
Achieving high capacity in bulk-type solid-state lithium ion battery based on Li 6.75 La 3 Zr 1.75 Ta 0.25 O 12 electrolyte: Interfacial resistance Liu, Ting; Ren, Yaoyu; Shen, Yang Journal of Power Sources, Vol. 324 https://doi.org/10.1016/j.jpowsour.2016.05.111	journal	August 2016
Chemical compatibility between garnet-like solid state electrolyte Li6.75La3Zr1.75Ta0.25O12 and major commercial lithium battery cathode materials Ren, Yaoyu; Liu, Ting; Shen, Yang Journal of Materiomics, Vol. 2, Issue 3 https://doi.org/10.1016/j.jmat.2016.04.003	journal	September 2016
Structure, Chemistry, and Charge Transfer Resistance of the Interface between Li ₇ La ₃ Zr ₂ O ₁₂ Electrolyte and LiCoO ₂ Cathode Vardar, Gulin; Bowman, William J.; Lu, Qiyang Chemistry of Materials, Vol. 30, Issue 18 https://doi.org/10.1021/acs.chemmater.8b01713	journal	July 2018
Characterization of the interface between LiCoO2 and Li7La3Zr2O12 in an all-solid-state rechargeable lithium battery Kim, Ki Hyun; Iriyama, Yasutoshi; Yamamoto, Kazuo Journal of Power Sources, Vol. 196, Issue 2 https://doi.org/10.1016/j.jpowsour.2010.07.073	journal	January 2011
In-situ Li7La3Zr2O12/LiCoO2 interface modification for advanced all-solid-state battery Kato, Takehisa; Hamanaka, Tadashi; Yamamoto, Kazuo Journal of Power Sources, Vol. 260 https://doi.org/10.1016/j.jpowsour.2014.02.102	journal	August 2014
Fast Charge Transfer across the Li ₇ La ₃ Zr ₂ O ₁₂ Solid Electrolyte/LiCoO ₂ Cathode Interface Enabled by an Interphase-Engineered All-Thin-Film Architecture Sastre, Jordi; Chen, Xubin; Aribia, Abdessalem ACS Applied Materials & Interfaces, Vol. 12, Issue 32 https://doi.org/10.1021/acsami.0c09777	journal	July 2020
Garnet-type oxide electrolyte with novel porous-dense bilayer configuration for rechargeable all-solid-state lithium batteries Ren, Yaoyu; Liu, Ting; Shen, Yang Ionics, Vol. 23, Issue 9 https://doi.org/10.1007/s11581-017-2224-5	journal	July 2017
All-solid-state lithium ion battery using garnet-type oxide and Li3BO3 solid electrolytes fabricated by screen-printing Ohta, Shingo; Komagata, Shogo; Seki, Juntaro Journal of Power Sources, Vol. 238 https://doi.org/10.1016/j.jpowsour.2013.02.073	journal	September 2013
Electrochemical Nature of the Cathode Interface for a Solid-State Lithium-Ion Battery: Interface between LiCoO ₂ and Garnet-Li ₇ La ₃ Zr ₂ O ₁₂ Park, Kyusung; Yu, Byeong-Chul; Jung, Ji-Won Chemistry of Materials, Vol. 28, Issue 21 https://doi.org/10.1021/acs.chemmater.6b03870	journal	October 2016
Interphase Engineering Enabled All-Ceramic Lithium Battery Han, Fudong; Yue, Jie; Chen, Cheng Joule, Vol. 2, Issue 3 https://doi.org/10.1016/j.joule.2018.02.007	journal	March 2018
Mixed Anion Effect in Conductivity of Rapidly Quenched Li₄SiO₄-Li₃BO₃ Glasses Tatsumisago, Masahiro; Machida, Nobuya; Minami, Tsutomu Journal of the Ceramic Association, Japan, Vol. 95, Issue 1098 https://doi.org/10.2109/jcersj1950.95.1098_197	journal	January 1987
Novel LiCoO₂ Cathode Material with Al₂O₃ Coating for a Li Ion Cell Cho, Jaephil; Kim, Yong Jeong; Park, Byungwoo Chemistry of Materials, Vol. 12, Issue 12, p. 3788-3791 https://doi.org/10.1021/cm000511k	journal	December 2000
Cathode materials modified by surface coating for lithium ion batteries Li, C.; Zhang, H. P.; Fu, L. J. Electrochimica Acta, Vol. 51, Issue 19 https://doi.org/10.1016/j.electacta.2005.11.015	journal	May 2006
Role of surface coating on cathode materials for lithium-ion batteries Chen, Zonghai; Qin, Yan; Amine, Khalil Journal of Materials Chemistry, Vol. 20, Issue 36, p. 7606-7612 https://doi.org/10.1039/c0jm00154f	journal	January 2010
Fabrication of All-Solid-State Lithium Polymer Secondary Batteries Using Al ₂ O ₃ -Coated LiCoO ₂ Miyashiro, Hajime; Kobayashi, Yo; Seki, Shiro Chemistry of Materials, Vol. 17, Issue 23 https://doi.org/10.1021/cm0517115	journal	November 2005
Nanoscale Interface Modification of LiCoO ₂ by Al ₂ O ₃ Atomic Layer Deposition for Solid-State Li Batteries Woo, Jae Ha; Trevey, James E.; Cavanagh, Andrew S. Journal of The Electrochemical Society, Vol. 159, Issue 7 https://doi.org/10.1149/2.085207jes	journal	January 2012
Negating interfacial impedance in garnet-based solid-state Li metal batteries Han, Xiaogang; Gong, Yunhui; Fu, Kun (Kelvin) Nature Materials, Vol. 16, Issue 5 https://doi.org/10.1038/nmat4821	journal	December 2016
How Do Li Atoms Pass through the Al ₂ O ₃ Coating Layer during Lithiation in Li-ion Batteries? Jung, Sung Chul; Han, Young-Kyu The Journal of Physical Chemistry Letters, Vol. 4, Issue 16 https://doi.org/10.1021/jz401231e	journal	July 2013
Li⁺ Diffusion in Amorphous and Crystalline Al₂O₃ for Battery Electrode Coatings Nolan, Adelaide M.; Wickramaratne, Darshana; Bernstein, Noam Chemistry of Materials, Vol. 33, Issue 19 https://doi.org/10.1021/acs.chemmater.1c02239	journal	September 2021
Effects of Li source on microstructure and ionic conductivity of Al-contained Li6.75La3Zr1.75Ta0.25O12 ceramics Ren, Yaoyu; Deng, Hui; Chen, Rujun Journal of the European Ceramic Society, Vol. 35, Issue 2 https://doi.org/10.1016/j.jeurceramsoc.2014.09.007	journal	February 2015
LiCoO2/Li6.75La3Zr1.75Nb0.25O12 interface modification enables all-solid-state battery Guo, Hong; Shen, Fei; Guo, Weichang Materials Letters, Vol. 301 https://doi.org/10.1016/j.matlet.2021.130302	journal	October 2021
High-rate lithium cycling in a scalable trilayer Li-garnet-electrolyte architecture Hitz, Gregory T.; McOwen, Dennis W.; Zhang, Lei Materials Today, Vol. 22 https://doi.org/10.1016/j.mattod.2018.04.004	journal	January 2019
Computation-guided discovery of coating materials to stabilize the interface between lithium garnet solid electrolyte and high-energy cathodes for all-solid-state lithium batteries Nolan, Adelaide M.; Wachsman, Eric D.; Mo, Yifei Energy Storage Materials, Vol. 41 https://doi.org/10.1016/j.ensm.2021.06.027	journal	October 2021
LiCoO[sub 2] and LiMn[sub 2]O[sub 4] Thin-Film Electrodes for Rechargeable Lithium Batteries Rho, Young Ho; Kanamura, Kiyoshi; Umegaki, Takao Journal of The Electrochemical Society, Vol. 150, Issue 1 https://doi.org/10.1149/1.1526514	journal	January 2003
A garnet structure-based all-solid-state Li battery without interface modification: resolving incompatibility issues on positive electrodes Tsai, Chih-Long; Ma, Qianli; Dellen, Christian Sustainable Energy & Fuels, Vol. 3, Issue 1 https://doi.org/10.1039/C8SE00436F	journal	January 2019
Avoiding CO ₂ Improves Thermal Stability at the Interface of Li ₇ La ₃ Zr ₂ O ₁₂ Electrolyte with Layered Oxide Cathodes Kim, Younggyu; Waluyo, Iradwikanari; Hunt, Adrian Advanced Energy Materials, Vol. 12, Issue 13 https://doi.org/10.1002/aenm.202102741	journal	February 2022
The origin of conductivity variations in Al-stabilized Li7La3Zr2O12 ceramics Wachter-Welzl, A.; Kirowitz, J.; Wagner, R. Solid State Ionics, Vol. 319 https://doi.org/10.1016/j.ssi.2018.01.036	journal	June 2018
The grain boundary impedance of random microstructures: numerical simulations and implications for the analysis of experimental data Fleig, J. Solid State Ionics, Vol. 150, Issue 1-2 https://doi.org/10.1016/S0167-2738(02)00274-6	journal	September 2002
Fabrication of LiCoO2 thin-film cathodes for rechargeable lithium microbatteries Julien, C.; Camacho-Lopez, M. A.; Escobar-Alarcon, L. Materials Chemistry and Physics, Vol. 68, Issue 1-3 https://doi.org/10.1016/S0254-0584(00)00372-2	journal	February 2001
High performance sputtered LiCoO2 thin films obtained at a moderate annealing treatment combined to a bias effect Tintignac, Sophie; Baddour-Hadjean, Rita; Pereira-Ramos, Jean-Pierre Electrochimica Acta, Vol. 60 https://doi.org/10.1016/j.electacta.2011.11.033	journal	January 2012
Epitaxial LiCoO ₂ Films as a Model System for Fundamental Electrochemical Studies of Positive Electrodes Takeuchi, Saya; Tan, Haiyan; Bharathi, K. Kamala ACS Applied Materials & Interfaces, Vol. 7, Issue 15 https://doi.org/10.1021/am508512q	journal	April 2015
Impact of the Crystal Orientation of Positive Electrodes on the Interface Resistance across a Solid Electrolyte and Electrode Nishio, Kazunori; Nakamura, Naoto; Horiba, Koji ACS Applied Energy Materials, Vol. 3, Issue 7 https://doi.org/10.1021/acsaem.0c00644	journal	June 2020
Raman spectroscopic determination of phase evolutions in LiAl_xCo_1−xO₂ battery materials Dobal, P. S.; Katiyar, R. S.; Tomar, M. S. Journal of Materials Research, Vol. 16, Issue 1 https://doi.org/10.1557/JMR.2001.0001	journal	January 2001
Understanding the Role of Temperature and Cathode Composition on Interface and Bulk: Optimizing Aluminum Oxide Coatings for Li-Ion Cathodes Han, Binghong; Paulauskas, Tadas; Key, Baris ACS Applied Materials & Interfaces, Vol. 9, Issue 17 https://doi.org/10.1021/acsami.7b00595	journal	April 2017
Effects of Al doping on the microstructure of LiCoO2 cathode materials Myung, S. Solid State Ionics, Vol. 139, Issue 1-2 https://doi.org/10.1016/S0167-2738(00)00828-6	journal	January 2001
Effect of Al2O3 coating on electrochemical performance of LiCoO2 as cathode materials for secondary lithium batteries Oh, Seungsuk; Lee, Joong Kee; Byun, Dongim Journal of Power Sources, Vol. 132, Issue 1-2 https://doi.org/10.1016/j.jpowsour.2004.01.049	journal	May 2004
Garnet-type solid-state fast Li ion conductors for Li batteries: critical review Thangadurai, Venkataraman; Narayanan, Sumaletha; Pinzaru, Dana Chemical Society Reviews, Vol. 43, Issue 13 https://doi.org/10.1039/c4cs00020j	journal	January 2014
Theoretical study of cubic-Li7La3Zr2O12(001)/LiCoO2(10–14) interface Panahian Jand, Sara; Kaghazchi, Payam MRS Communications, Vol. 8, Issue 02 https://doi.org/10.1557/mrc.2018.33	journal	March 2018
First principles study on electrochemical and chemical stability of solid electrolyte–electrode interfaces in all-solid-state Li-ion batteries Zhu, Yizhou; He, Xingfeng; Mo, Yifei Journal of Materials Chemistry A, Vol. 4, Issue 9 https://doi.org/10.1039/C5TA08574H	journal	January 2016
First-Principles Studies on Cation Dopants and Electrolyte\|Cathode Interphases for Lithium Garnets Miara, Lincoln J.; Richards, William Davidson; Wang, Yan E. Chemistry of Materials, Vol. 27, Issue 11 https://doi.org/10.1021/acs.chemmater.5b01023	journal	May 2015
Mechanism Study on the Interfacial Stability of a Lithium Garnet-Type Oxide Electrolyte against Cathode Materials Zhang, Nian; Long, Xinghui; Wang, Zhi ACS Applied Energy Materials, Vol. 1, Issue 11 https://doi.org/10.1021/acsaem.8b01035	journal	October 2018
Reactive-sputter-deposited TiN films on glass substrates Pelleg, Joshua; Zevin, L. Z.; Lungo, S. Thin Solid Films, Vol. 197, Issue 1-2 https://doi.org/10.1016/0040-6090(91)90225-M	journal	March 1991
Preferred Orientation of Polycrystalline LiCoO[sub 2] Films Bates, J. B.; Dudney, N. J.; Neudecker, B. J. Journal of The Electrochemical Society, Vol. 147, Issue 1 https://doi.org/10.1149/1.1393157	journal	January 2000
Lattice model calculation of the strain energy density and other properties of crystalline LiCoO2 Hart, F. X.; Bates, J. B. Journal of Applied Physics, Vol. 83, Issue 12 https://doi.org/10.1063/1.367521	journal	June 1998

Similar Records

Cathode Interface Compatibility of Amorphous LiMn₂O₄ (LMO) and Li₇La₃Zr₂O₁₂ (LLZO) Characterized with Thin-Film Solid-State Electrochemical Cells

Journal Article · 2020 · ACS Applied Materials and Interfaces · OSTI ID:1980879

Delluva, Alexander A.; Dudoff, Jessica; Teeter, Glenn; +1 more

Computation-guided discovery of coating materials to stabilize the interface between lithium garnet solid electrolyte and high-energy cathodes for all-solid-state lithium batteries

Journal Article · 2021 · Energy Storage Materials · OSTI ID:1980879

Nolan, Adelaide M.; Wachsman, Eric D.; Mo, Yifei

The Riddle of Dark LLZO: Cobalt Diffusion in Garnet Separators of Solid-State Lithium Batteries

Journal Article · 2023 · Advanced Functional Materials · OSTI ID:1980879

Scheld, Walter Sebastian; Kim, Kwangnam; Schwab, Christian; +17 more

Related Subjects

Electrochemistry
Materials Science

Title: All Solid-State Li/LLZO/LCO Battery Enabled by Alumina Interfacial Coating

Citation Formats

References (45)

Similar Records

Related Subjects