Dynamic Monkey Bar Mechanism of Superionic Li‐ion Transport in LiTaCl 6

Lei, Ming; Li, Bo; Liu, Hongjun; Jiang, De‐en

doi:10.1002/ange.202315628

Title: Dynamic Monkey Bar Mechanism of Superionic Li‐ion Transport in LiTaCl ₆

Journal Article · 21 December 2023 · Angewandte Chemie

DOI: https://doi.org/10.1002/ange.202315628 · OSTI ID:2251523

^[1];

^[1]; Liu, Hongjun ^[1];

^[2]

Department of Chemical and Biomolecular Engineering Vanderbilt University Nashville TN-37235 USA
Department of Chemical and Biomolecular Engineering Vanderbilt University Nashville TN-37235 USA, Department of Chemistry Vanderbilt University Nashville TN-37235 USA

Abstract The LiTaCl ₆ solid electrolyte has the lowest activation energy of ionic conduction at ambient conditions (0.165 eV), with a record high ionic conductivity for a ternary compound (11 mS cm ⁻¹ ). However, the mechanism has been unclear. We train machine‐learning force fields (MLFF) on ab initio molecular dynamics (AIMD) data on‐the‐fly and perform MLFF MD simulations of AIMD quality up to the nanosecond scale at the experimental temperatures, which allows us to predict accurate activation energy for Li‐ion diffusion (at 0.164 eV). Detailed analyses of trajectories and vibrational density of states show that the large‐amplitude vibrations of Cl ⁻ ions in TaCl ₆ ⁻ enable the fast Li‐ion transport by allowing dynamic breaking and reforming of Li−Cl bonds across the space in between the TaCl ₆ ⁻ octahedra. We term this process the dynamic‐monkey‐bar mechanism of superionic Li ⁺ transport which could aid the development of new solid electrolytes for all‐solid‐state lithium batteries.

View Accepted Manuscript (Publisher)

Cite

Export

Save

Sponsoring Organization:: USDOE

Grant/Contract Number:: NONE; SC0023408

OSTI ID:: 2251523

Journal Information:: Angewandte Chemie, Journal Name: Angewandte Chemie; ISSN 0044-8249

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

References (40)

Fast Lithium Ion Conduction in Garnet-Type Li₇La₃Zr₂O₁₂ Murugan, Ramaswamy; Thangadurai, Venkataraman; Weppner, Werner Angewandte Chemie International Edition, Vol. 46, Issue 41, p. 7778-7781 https://doi.org/10.1002/anie.200701144	journal	October 2007
Spin-Torque Switching with the Giant Spin Hall Effect of Tantalum Liu, L.; Pai, C. -F.; Li, Y. Science, Vol. 336, Issue 6081 https://doi.org/10.1126/science.1218197	journal	May 2012
Designing solid-state electrolytes for safe, energy-dense batteries Zhao, Qing; Stalin, Sanjuna; Zhao, Chen-Zi Nature Reviews Materials, Vol. 5, Issue 3 https://doi.org/10.1038/s41578-019-0165-5	journal	February 2020
Enhanced ionic conductivity and lack of paddle-wheel effect in pseudohalogen-substituted Li argyrodites Sun, Yingzhi; Ouyang, Bin; Wang, Yan Matter, Vol. 5, Issue 12 https://doi.org/10.1016/j.matt.2022.08.029	journal	December 2022
Ordering of hidden multipoles in spin-orbit entangled 5 d 1 Ta chlorides Ishikawa, H.; Takayama, T.; Kremer, R. K. Physical Review B, Vol. 100, Issue 4 https://doi.org/10.1103/PhysRevB.100.045142	journal	July 2019
A lithium superionic conductor for millimeter-thick battery electrode Li, Yuxiang; Song, Subin; Kim, Hanseul Science, Vol. 381, Issue 6653 https://doi.org/10.1126/science.add7138	journal	July 2023
Exploiting the paddle-wheel mechanism for the design of fast ion conductors Zhang, Zhizhen; Nazar, Linda F. Nature Reviews Materials, Vol. 7, Issue 5 https://doi.org/10.1038/s41578-021-00401-0	journal	January 2022
Universal ion-transport descriptors and classes of inorganic solid-state electrolytes López, Cibrán; Emperador, Agustí; Saucedo, Edgardo Materials Horizons, Vol. 10, Issue 5 https://doi.org/10.1039/D2MH01516A	journal	January 2023
Prospects of halide-based all-solid-state batteries: From material design to practical application Wang, Changhong; Liang, Jianwen; Kim, Jung Tae Science Advances, Vol. 8, Issue 36 https://doi.org/10.1126/sciadv.adc9516	journal	September 2022
Solid Halide Electrolytes with High Lithium-Ion Conductivity for Application in 4 V Class Bulk-Type All-Solid-State Batteries Asano, Tetsuya; Sakai, Akihiro; Ouchi, Satoru Advanced Materials, Vol. 30, Issue 44 https://doi.org/10.1002/adma.201803075	journal	September 2018
Anharmonic Cation–Anion Coupling Dynamics Assisted Lithium‐Ion Diffusion in Sulfide Solid Electrolytes Xu, Zhenming; Chen, Xi; Zhu, Hong Advanced Materials, Vol. 34, Issue 49 https://doi.org/10.1002/adma.202207411	journal	October 2022
Lithium superionic conductors with corner-sharing frameworks Jun, KyuJung; Sun, Yingzhi; Xiao, Yihan Nature Materials, Vol. 21, Issue 8 https://doi.org/10.1038/s41563-022-01222-4	journal	March 2022
Origin of fast ion diffusion in super-ionic conductors He, Xingfeng; Zhu, Yizhou; Mo, Yifei Nature Communications, Vol. 8, Issue 1 https://doi.org/10.1038/ncomms15893	journal	June 2017
Boosting Solid-State Diffusivity and Conductivity in Lithium Superionic Argyrodites by Halide Substitution Adeli, Parvin; Bazak, J. David; Park, Kern Ho Angewandte Chemie International Edition, Vol. 58, Issue 26 https://doi.org/10.1002/anie.201814222	journal	May 2019
Argyrodite-type advanced lithium conductors and transport mechanisms beyond paddle-wheel effect Fang, Hong; Jena, Puru Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-29769-5	journal	April 2022
From nanoscale interface characterization to sustainable energy storage using all-solid-state batteries Tan, Darren H. S.; Banerjee, Abhik; Chen, Zheng Nature Nanotechnology, Vol. 15, Issue 3 https://doi.org/10.1038/s41565-020-0657-x	journal	March 2020
Low-temperature paddlewheel effect in glassy solid electrolytes Smith, Jeffrey G.; Siegel, Donald J. Nature Communications, Vol. 11, Issue 1 https://doi.org/10.1038/s41467-020-15245-5	journal	March 2020
Inorganic Solid-State Electrolytes for Lithium Batteries: Mechanisms and Properties Governing Ion Conduction Bachman, John Christopher; Muy, Sokseiha; Grimaud, Alexis Chemical Reviews, Vol. 116, Issue 1 https://doi.org/10.1021/acs.chemrev.5b00563	journal	December 2015
Emerging Halide Superionic Conductors for All-Solid-State Batteries: Design, Synthesis, and Practical Applications Kwak, Hiram; Wang, Shuo; Park, Juhyoun ACS Energy Letters, Vol. 7, Issue 5 https://doi.org/10.1021/acsenergylett.2c00438	journal	April 2022
Phase Transitions of Hybrid Perovskites Simulated by Machine-Learning Force Fields Trained on the Fly with Bayesian Inference Jinnouchi, Ryosuke; Lahnsteiner, Jonathan; Karsai, Ferenc Physical Review Letters, Vol. 122, Issue 22 https://doi.org/10.1103/PhysRevLett.122.225701	journal	June 2019
Coupled Cation–Anion Dynamics Enhances Cation Mobility in Room-Temperature Superionic Solid-State Electrolytes Zhang, Zhizhen; Roy, Pierre-Nicholas; Li, Hui Journal of the American Chemical Society, Vol. 141, Issue 49 https://doi.org/10.1021/jacs.9b09343	journal	November 2019
Extreme phonon anharmonicity underpins superionic diffusion and ultralow thermal conductivity in argyrodite Ag8SnSe6 Ren, Qingyong; Gupta, Mayanak K.; Jin, Min Nature Materials, Vol. 22, Issue 8 https://doi.org/10.1038/s41563-023-01560-x	journal	May 2023
Rotational Cluster Anion Enabling Superionic Conductivity in Sodium-Rich Antiperovskite Na ₃ OBH ₄ Sun, Yulong; Wang, Yuechao; Liang, Xinmiao Journal of the American Chemical Society, Vol. 141, Issue 14 https://doi.org/10.1021/jacs.9b01746	journal	March 2019
Effect of Spin–Orbit Coupling on Phonon-Mediated Magnetic Relaxation in a Series of Zero-Valent Vanadium, Niobium, and Tantalum Isocyanide Complexes Chakarawet, Khetpakorn; Atanasov, Mihail; Ellis, John E. Inorganic Chemistry, Vol. 60, Issue 23 https://doi.org/10.1021/acs.inorgchem.1c03173	journal	November 2021
Fast Na diffusion and anharmonic phonon dynamics in superionic Na ₃ PS ₄ Gupta, Mayanak K.; Ding, Jingxuan; Osti, Naresh C. Energy & Environmental Science, Vol. 14, Issue 12 https://doi.org/10.1039/D1EE01509E	journal	January 2021
Anharmonic lattice dynamics and superionic transition in AgCrSe ₂ Ding, Jingxuan; Niedziela, Jennifer L.; Bansal, Dipanshu Proceedings of the National Academy of Sciences, Vol. 117, Issue 8 https://doi.org/10.1073/pnas.1913916117	journal	February 2020
Superionic Diffusion through Frustrated Energy Landscape Di Stefano, Davide; Miglio, Anna; Robeyns, Koen Chem, Vol. 5, Issue 9 https://doi.org/10.1016/j.chempr.2019.07.001	journal	September 2019
Targeting Superionic Conductivity by Turning on Anion Rotation at Room Temperature in Fast Ion Conductors Zhang, Zhizhen; Li, Hui; Kaup, Kavish Matter, Vol. 2, Issue 6 https://doi.org/10.1016/j.matt.2020.04.027	journal	June 2020
Descriptors representing two- and three-body atomic distributions and their effects on the accuracy of machine-learned inter-atomic potentials Jinnouchi, Ryosuke; Karsai, Ferenc; Verdi, Carla The Journal of Chemical Physics, Vol. 152, Issue 23 https://doi.org/10.1063/5.0009491	journal	June 2020
Tuning mobility and stability of lithium ion conductors based on lattice dynamics Muy, Sokseiha; Bachman, John C.; Giordano, Livia Energy & Environmental Science, Vol. 11, Issue 4 https://doi.org/10.1039/C7EE03364H	journal	January 2018
A lithium superionic conductor Kamaya, Noriaki; Homma, Kenji; Yamakawa, Yuichiro Nature Materials, Vol. 10, Issue 9, p. 682-686 https://doi.org/10.1038/nmat3066	journal	July 2011
Phonon–Ion Interactions: Designing Ion Mobility Based on Lattice Dynamics Muy, Sokseiha; Schlem, Roman; Shao‐Horn, Yang Advanced Energy Materials, Vol. 11, Issue 15 https://doi.org/10.1002/aenm.202002787	journal	December 2020
A LaCl3-based lithium superionic conductor compatible with lithium metal Yin, Yi-Chen; Yang, Jing-Tian; Luo, Jin-Da Nature, Vol. 616, Issue 7955 https://doi.org/10.1038/s41586-023-05899-8	journal	April 2023
New horizons for inorganic solid state ion conductors Zhang, Zhizhen; Shao, Yuanjun; Lotsch, Bettina Energy & Environmental Science, Vol. 11, Issue 8 https://doi.org/10.1039/C8EE01053F	journal	January 2018
All-solid-state lithium batteries enabled by sulfide electrolytes: from fundamental research to practical engineering design Wang, Changhong; Liang, Jianwen; Zhao, Yang Energy & Environmental Science, Vol. 14, Issue 5 https://doi.org/10.1039/D1EE00551K	journal	January 2021
High-power all-solid-state batteries using sulfide superionic conductors Kato, Yuki; Hori, Satoshi; Saito, Toshiya Nature Energy, Vol. 1, Issue 4 https://doi.org/10.1038/nenergy.2016.30	journal	March 2016
TaCl₅-glassified Ultrafast Lithium Ion-conductive Halide Electrolytes for High-performance All-solid-state Lithium Batteries Ishiguro, Yoshitaka; Ueno, Kenji; Nishimura, Sayaka Chemistry Letters, Vol. 52, Issue 4 https://doi.org/10.1246/cl.220540	journal	April 2023
Bottleneck of Diffusion and Inductive Effects in Li ₁₀ Ge _{1– x} Sn _x P ₂ S ₁₂ Krauskopf, Thorben; Culver, Sean P.; Zeier, Wolfgang G. Chemistry of Materials, Vol. 30, Issue 5 https://doi.org/10.1021/acs.chemmater.8b00266	journal	February 2018
New Oxyhalide Solid Electrolytes with High Lithium Ionic Conductivity >10 mS cm⁻¹for All‐Solid‐State Batteries Tanaka, Yoshiaki; Ueno, Koki; Mizuno, Keita Angewandte Chemie, Vol. 135, Issue 13 https://doi.org/10.1002/ange.202217581	journal	February 2023
Metal Halide Superionic Conductors for All-Solid-State Batteries Liang, Jianwen; Li, Xiaona; Adair, Keegan R. Accounts of Chemical Research, Vol. 54, Issue 4 https://doi.org/10.1021/acs.accounts.0c00762	journal	January 2021

Similar Records

Dynamic Monkey Bar Mechanism of Superionic Li–ion Transport in LiTaCl₆

Journal Article · 2023 · Angewandte Chemie (International Edition) · OSTI ID:2340922

Lei, Ming; Li, Bo; Liu, Hongjun; +1 more

A Dual Anion Chemistry-Based Superionic Glass Enabling Long-Cycling All-Solid-State Sodium-Ion Batteries

Journal Article · 2023 · Angewandte Chemie (International Edition) · OSTI ID:2344964

Lin, Xiaoting; Zhao, Yang; Wang, Changhong; +14 more

Exploring Li-Ion Transport Properties of Li ₃ TiCl ₆ : A Machine Learning Molecular Dynamics Study

Journal Article · 2024 · Journal of the Electrochemical Society · OSTI ID:2352792

Selvaraj, Selva Chandrasekaran; Koverga, Volodymyr; Ngo, Anh T.

Title: Dynamic Monkey Bar Mechanism of Superionic Li‐ion Transport in LiTaCl 6

Citation Formats

References (40)

Similar Records

Related Subjects

Title: Dynamic Monkey Bar Mechanism of Superionic Li‐ion Transport in LiTaCl ₆