Probing lithium mobility at a solid electrolyte surface

Woodahl, Clarisse; Jamnuch, Sasawat; Amado, Angelique; Uzundal, Can B.; Berger, Emma; Manset, Paul; Zhu, Yisi; Li, Yan; Fong, Dillon D.; Connell, Justin G.; Hirata, Yasuyuki; Kubota, Yuya; Owada, Shigeki; Tono, Kensuke; Yabashi, Makina; te Velthuis, Suzanne G. E.; Tepavcevic, Sanja; Matsuda, Iwao; Drisdell, Walter S.; Schwartz, Craig P.; Freeland, John W.; Pascal, Tod A.; Zong, Alfred; Zuerch, Michael

doi:10.1038/s41563-023-01535-y

Title: Probing lithium mobility at a solid electrolyte surface

Journal Article · 27 April 2023 · Nature Materials

DOI: https://doi.org/10.1038/s41563-023-01535-y · OSTI ID:1971702

Woodahl, Clarisse; Jamnuch, Sasawat; Amado, Angelique; Uzundal, Can B.; Berger, Emma; Manset, Paul; Zhu, Yisi;

;

; Hirata, Yasuyuki; Kubota, Yuya; Owada, Shigeki;

;

Abstract Solid-state electrolytes overcome many challenges of present-day lithium ion batteries, such as safety hazards and dendrite formation ^1,2 . However, detailed understanding of the involved lithium dynamics is missing due to a lack of in operando measurements with chemical and interfacial specificity. Here we investigate a prototypical solid-state electrolyte using linear and nonlinear extreme-ultraviolet spectroscopies. Leveraging the surface sensitivity of extreme-ultraviolet-second-harmonic-generation spectroscopy, we obtained a direct spectral signature of surface lithium ions, showing a distinct blueshift relative to bulk absorption spectra. First-principles simulations attributed the shift to transitions from the lithium 1 s state to hybridized Li- s /Ti- d orbitals at the surface. Our calculations further suggest a reduction in lithium interfacial mobility due to suppressed low-frequency rattling modes, which is the fundamental origin of the large interfacial resistance in this material. Our findings pave the way for new optimization strategies to develop these electrochemical devices via interfacial engineering of lithium ions.

View Journal Article

Cite

Export

Save

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: Federal Ministry of Education and Research (BMBF); Japan Synchrotron Radiation Research Institute (JASRI); National Science Foundation (NSF); USDOE; USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357; SC0004993; SC0012375; SC0023355; SC0023503

OSTI ID:: 1971702

Journal Information:: Nature Materials, Journal Name: Nature Materials Journal Issue: 7 Vol. 22; ISSN 1476-1122

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United Kingdom

Language:: English

References (28)

Promises, Challenges, and Recent Progress of Inorganic Solid-State Electrolytes for All-Solid-State Lithium Batteries Gao, Zhonghui; Sun, Huabin; Fu, Lin Advanced Materials, Vol. 30, Issue 17 https://doi.org/10.1002/adma.201705702	journal	February 2018
Anode‐Free Solid‐State Lithium Batteries: A Review Huang, Wen‐Ze; Zhao, Chen‐Zi; Wu, Peng Advanced Energy Materials, Vol. 12, Issue 26 https://doi.org/10.1002/aenm.202201044	journal	May 2022
Valence and core excitons in solids from velocity-gauge real-time TDDFT with range-separated hybrid functionals: An LCAO approach Pemmaraju, C. D. Computational Condensed Matter, Vol. 18 https://doi.org/10.1016/j.cocom.2018.e00348	journal	March 2019
LiNbO3-coated LiCoO2 as cathode material for all solid-state lithium secondary batteries Ohta, Narumi; Takada, Kazunori; Sakaguchi, Isao Electrochemistry Communications, Vol. 9, Issue 7 https://doi.org/10.1016/j.elecom.2007.02.008	journal	July 2007
Cryogenic Electron Microscopy for Characterizing and Diagnosing Batteries Wang, Xuefeng; Li, Yejing; Meng, Ying Shirley Joule, Vol. 2, Issue 11 https://doi.org/10.1016/j.joule.2018.10.005	journal	November 2018
High rate capabilities of all-solid-state lithium secondary batteries using Li4Ti5O12-coated LiNi0.8Co0.15Al0.05O2 and a sulfide-based solid electrolyte Seino, Yoshikatsu; Ota, Tsuyoshi; Takada, Kazunori Journal of Power Sources, Vol. 196, Issue 15 https://doi.org/10.1016/j.jpowsour.2011.03.090	journal	August 2011
Inorganic solid Li ion conductors: An overview Knauth, Philippe Solid State Ionics, Vol. 180, Issue 14-16, p. 911-916 https://doi.org/10.1016/j.ssi.2009.03.022	journal	June 2009
Interfacial phenomena in solid-state lithium battery with sulfide solid electrolyte Takada, Kazunori; Ohta, Narumi; Zhang, Lianqi Solid State Ionics, Vol. 225 https://doi.org/10.1016/j.ssi.2012.01.009	journal	October 2012
Extreme Ultraviolet Second Harmonic Generation Spectroscopy in a Polar Metal Berger, Emma; Jamnuch, Sasawat; Uzundal, Can B. Nano Letters, Vol. 21, Issue 14 https://doi.org/10.1021/acs.nanolett.1c01502	journal	July 2021
Lithium Lanthanum Titanium Oxides: A Fast Ionic Conductive Coating for Lithium-Ion Battery Cathodes Qian, Danna; Xu, Bo; Cho, Hyung-Man Chemistry of Materials, Vol. 24, Issue 14 https://doi.org/10.1021/cm300929r	journal	July 2012
Vibrational Analysis of Brucite Surfaces and the Development of an Improved Force Field for Molecular Simulation of Interfaces Zeitler, Todd R.; Greathouse, Jeffery A.; Gale, Julian D. The Journal of Physical Chemistry C, Vol. 118, Issue 15 https://doi.org/10.1021/jp411092b	journal	April 2014
Issues and challenges facing rechargeable lithium batteries Tarascon, J.-M.; Armand, M. Nature, Vol. 414, Issue 6861, p. 359-367 https://doi.org/10.1038/35104644	journal	November 2001
A reflection on lithium-ion battery cathode chemistry Manthiram, Arumugam Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15355-0	journal	March 2020
Processing thin but robust electrolytes for solid-state batteries Balaish, Moran; Gonzalez-Rosillo, Juan Carlos; Kim, Kun Joong Nature Energy, Vol. 6, Issue 3 https://doi.org/10.1038/s41560-020-00759-5	journal	February 2021
Understanding interface stability in solid-state batteries Xiao, Yihan; Wang, Yan; Bo, Shou-Hang Nature Reviews Materials, Vol. 5, Issue 2 https://doi.org/10.1038/s41578-019-0157-5	journal	December 2019
Emerging ultrafast techniques for studying quantum materials Zong, Alfred; Nebgen, Bailey R.; Lin, Sheng-Chih Nature Reviews Materials, Vol. 8, Issue 4 https://doi.org/10.1038/s41578-022-00530-0	journal	February 2023
Electrolytes for solid-state lithium rechargeable batteries: recent advances and perspectives Quartarone, Eliana; Mustarelli, Piercarlo Chemical Society Reviews, Vol. 40, Issue 5 https://doi.org/10.1039/c0cs00081g	journal	January 2011
Effect of average and local structures on lithium ion conductivity in La2/3−xLi3xTiO3 Okumura, Toyoki; Ina, Toshiaki; Orikasa, Yuki Journal of Materials Chemistry, Vol. 21, Issue 27 https://doi.org/10.1039/c0jm04372a	journal	January 2011
Atomic-scale origin of the large grain-boundary resistance in perovskite Li-ion-conducting solid electrolytes Ma, Cheng; Chen, Kai; Liang, Chengdu Energy & Environmental Science, Vol. 7, Issue 5 https://doi.org/10.1039/c4ee00382a	journal	January 2014
Soft X-Ray Second Harmonic Generation as an Interfacial Probe Lam, R. K.; Raj, S. L.; Pascal, T. A. Physical Review Letters, Vol. 120, Issue 2 https://doi.org/10.1103/PhysRevLett.120.023901	journal	January 2018
Element Selectivity in Second-Harmonic Generation of GaFeO 3 by a Soft-X-Ray Free-Electron Laser Yamamoto, Sh.; Omi, T.; Akai, H. Physical Review Letters, Vol. 120, Issue 22 https://doi.org/10.1103/PhysRevLett.120.223902	journal	June 2018
Angstrom-Resolved Interfacial Structure in Buried Organic-Inorganic Junctions Schwartz, Craig P.; Raj, Sumana L.; Jamnuch, Sasawat Physical Review Letters, Vol. 127, Issue 9 https://doi.org/10.1103/PhysRevLett.127.096801	journal	August 2021
Comparison of ultracapacitor electric circuit models Shi, Lisheng; Crow, M. L. 2008 IEEE Power and Energy Society General Meeting - Conversion and Delivery of Electrical Energy in the 21st Century https://doi.org/10.1109/PES.2008.4596576	conference	July 2008
Table-top extreme ultraviolet second harmonic generation Helk, Tobias; Berger, Emma; Jamnuch, Sasawat Science Advances, Vol. 7, Issue 21 https://doi.org/10.1126/sciadv.abe2265	journal	May 2021
Surface Second Harmonic Generation: A New Technique for Surface Studies Shen, Y. R. Annual Review of Materials Science, Vol. 16, Issue 1 https://doi.org/10.1146/annurev.ms.16.080186.000441	journal	August 1986
The Nature of the Passive Film on Iron Cahan, Boris D. Journal of The Electrochemical Society, Vol. 129, Issue 3 https://doi.org/10.1149/1.2123883	journal	January 1982
Fundamental Relationship of Microstructure and Ionic Conductivity of Amorphous LLTO as Solid Electrolyte Material Zhang, Yubin; Zheng, Zhangfeng; Liu, Xiaoming Journal of The Electrochemical Society, Vol. 166, Issue 4 https://doi.org/10.1149/2.0161904jes	journal	January 2019
Reduced Energy Barrier for Li+ Transport Across Grain Boundaries with Amorphous Domains in LLZO Thin Films Zhu, Yanlin; Wu, Shuai; Pan, Yilan Nanoscale Research Letters, Vol. 15, Issue 1 https://doi.org/10.1186/s11671-020-03378-x	journal	July 2020

Similar Records

A Perovskite Electrolyte That Is Stable in Moist Air for Lithium‐Ion Batteries

Journal Article · 2018 · Angewandte Chemie · OSTI ID:1441038

Li, Yutao; Xu, Henghui; Chien, Po‐Hsiu; +6 more

A Perovskite Electrolyte That Is Stable in Moist Air for Lithium‐Ion Batteries

Journal Article · 2018 · Angewandte Chemie (International Edition) · OSTI ID:1441039

Li, Yutao; Xu, Henghui; Chien, Po‐Hsiu; +6 more

Incombustible Polymer Electrolyte Boosting Safety of Solid–State Lithium Batteries: A Review

Journal Article · 2023 · Advanced Functional Materials · OSTI ID:2368844

Han, Longfei; Wang, Li; Chen, Zonghai; +4 more

Related Subjects

25 ENERGY STORAGE
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Batteries
Characterization and analytical techniques
Chemical physics
Density functional theory

Title: Probing lithium mobility at a solid electrolyte surface

Citation Formats

References (28)

Similar Records

Related Subjects