Disorder-Driven Fast Na+ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaOxCl6−2x Oxychlorides

Justin Leifeld; Abigail C. Parsons; Alexandra Morscher; Xabier Martinez de Irujo-Labalde; Marvin A. Kraft; Oskar G. Soulas; Bibek Samanta; Wiebke Zielasko; Neelam Yadav; Kyra Strotmann; Niina Jalarvo; Bruno V.M. Rodrigues; Adam Slabon; Philipp Adelhelm; Michael Ryan Hansen; David O. Scanlon; Wolfgang G. Zeier; Alexander G. Squires

doi:10.1002/aenm.70977

Disorder-Driven Fast Na⁺ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaO_xCl₆₋₂_x Oxychlorides

Justin Leifeld
, Abigail C. Parsons
, Alexandra Morscher
, Xabier Martinez de Irujo-Labalde
, Marvin A. Kraft
, Oskar G. Soulas
, Bibek Samanta
, Wiebke Zielasko
, Neelam Yadav
, Kyra Strotmann
, Niina Jalarvo
, Bruno V.M. Rodrigues
, Adam Slabon
, Philipp Adelhelm
, Michael Ryan Hansen
, David O. Scanlon
, Wolfgang G. Zeier
, Alexander G. Squires

Chemical Spectroscopy

Research output: Contribution to journal › Article › peer-review

Abstract

Solid electrolytes are central to enabling safe, high-energy solid-state sodium batteries. While oxyhalide-type conductors have rapidly advanced lithium-based systems, their sodium analogues remain less understood and underdeveloped. This gap arises from their intrinsically amorphous nature, which obscures structure–transport relationships and limits rational design. Here, we elucidate the atomic-scale origins of sodium-ion conduction in the mixed-anion series NaTaO_xCl_6–2_x using a combination of experimental and computational approaches. We reveal that composition-dependent, disordered yet extended chain motifs emerge as key structural units governing ion mobility. By tuning chain connectivity, we achieve a high ionic conductivity of ∼4 mS cm⁻¹ and a corresponding self-diffusion coefficient of 6.6–8.2 × 10⁻¹¹ m² s⁻¹, ranking among to the fastest reported for sodium oxyhalides. These findings establish clear structure–property correlations in amorphous superionic conductors and provide a blueprint for the targeted design of next-generation solid electrolytes for sodium solid-state batteries.

Original language	English
Article number	e70977
Journal	Advanced Energy Materials
Volume	16
Issue number	24
DOIs	https://doi.org/10.1002/aenm.70977
State	Published - Jun 24 2026

Funding

D.O.S. gratefully acknowledges illuminating conversations with Professor Vladan Stevanovic on modelling amorphous materials. This work was funded by the Federal Ministry for Research, Technology, and Space (BMFTR) under the project HiPoBat: High Power Batteries (FKZ: 13XP0611A). This research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The beamtime was allocated to BASIS on proposal number IPTS‐35994. This study is funded by the European Union (ERC, DIONISOS, 101123802). Views and opinions expressed are, however, those of the author(s) only and do not necessarily reflect those of the European Union or the European Research Council Executive Agency. Neither the European Union nor the granting authority can be held responsible for them. Furthermore, would like to thank the University of Wuppertal for the research support and the DELTA synchrotron (Dortmund, Germany) for the beam time provided. University of Birmingham's BlueBEAR HPC service, the Baskerville Tier 2 HPC service ( https://www.baskerville.ac.uk/; funded by the EPSRC and UKRI through the World Class Labs scheme (EP/T022221/1) and the Digital Research Infrastructure programme (EP/W032244/1)), and the Sulis Tier 2 HPC platform hosted by the Scientific Computing Research Technology Platform at the University of Warwick (funded by EPSRC Grant EP/T022108/1 and the HPC Midlands+ consortium). Through our membership of the UK's HEC Materials Chemistry Consortium, which is funded by the UK Engineering and Physical Sciences Research Council (EPSRC; EP/L000202, EP/R029431, EP/T022213), this work also used ARCHER2 UK National Supercomputing Services. We are also grateful to the UK Materials and Molecular Modelling Hub for computational resources, which is partially funded by EPSRC (EP/T022213/1, EP/W032260/1 and EP/P020194/1). We would also like to thank M.R.H. and B.S. who carried out NMR measurements and are members of the International Graduate School for Battery Chemistry, Characterization, Analysis, Recycling and Application (BACCARA), which is funded by the Ministry of Culture and Science of the State of North Rhine‐Westphalia, Germany.

Access to Document

10.1002/aenm.70977

Cite this

Leifeld, J., Parsons, A. C., Morscher, A., de Irujo-Labalde, X. M., Kraft, M. A., Soulas, O. G., Samanta, B., Zielasko, W., Yadav, N., Strotmann, K., Jalarvo, N., Rodrigues, B. V. M., Slabon, A., Adelhelm, P., Hansen, M. R., Scanlon, D. O., Zeier, W. G., & Squires, A. G. (2026). Disorder-Driven Fast Na⁺ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaO_xCl₆₋₂_x Oxychlorides. Advanced Energy Materials, 16(24), Article e70977. https://doi.org/10.1002/aenm.70977

@article{6c69467b7c9f4032b002914dfa21d48c,

title = "Disorder-Driven Fast Na+ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaOxCl6−2x Oxychlorides",

abstract = "Solid electrolytes are central to enabling safe, high-energy solid-state sodium batteries. While oxyhalide-type conductors have rapidly advanced lithium-based systems, their sodium analogues remain less understood and underdeveloped. This gap arises from their intrinsically amorphous nature, which obscures structure–transport relationships and limits rational design. Here, we elucidate the atomic-scale origins of sodium-ion conduction in the mixed-anion series NaTaOxCl6–2x using a combination of experimental and computational approaches. We reveal that composition-dependent, disordered yet extended chain motifs emerge as key structural units governing ion mobility. By tuning chain connectivity, we achieve a high ionic conductivity of ∼4 mS cm−1 and a corresponding self-diffusion coefficient of 6.6–8.2 × 10−11 m2 s−1, ranking among to the fastest reported for sodium oxyhalides. These findings establish clear structure–property correlations in amorphous superionic conductors and provide a blueprint for the targeted design of next-generation solid electrolytes for sodium solid-state batteries.",

author = "Justin Leifeld and Parsons, \{Abigail C.\} and Alexandra Morscher and \{de Irujo-Labalde\}, \{Xabier Martinez\} and Kraft, \{Marvin A.\} and Soulas, \{Oskar G.\} and Bibek Samanta and Wiebke Zielasko and Neelam Yadav and Kyra Strotmann and Niina Jalarvo and Rodrigues, \{Bruno V.M.\} and Adam Slabon and Philipp Adelhelm and Hansen, \{Michael Ryan\} and Scanlon, \{David O.\} and Zeier, \{Wolfgang G.\} and Squires, \{Alexander G.\}",

note = "Publisher Copyright: {\textcopyright} 2026 The Author(s). Advanced Energy Materials published by Wiley-VCH GmbH.",

year = "2026",

month = jun,

day = "24",

doi = "10.1002/aenm.70977",

language = "English",

volume = "16",

journal = "Advanced Energy Materials",

issn = "1614-6832",

publisher = "wiley",

number = "24",

}

Leifeld, J, Parsons, AC, Morscher, A, de Irujo-Labalde, XM, Kraft, MA, Soulas, OG, Samanta, B, Zielasko, W, Yadav, N, Strotmann, K, Jalarvo, N, Rodrigues, BVM, Slabon, A, Adelhelm, P, Hansen, MR, Scanlon, DO, Zeier, WG & Squires, AG 2026, 'Disorder-Driven Fast Na⁺ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaO_xCl₆₋₂_x Oxychlorides', Advanced Energy Materials, vol. 16, no. 24, e70977. https://doi.org/10.1002/aenm.70977

TY - JOUR

T1 - Disorder-Driven Fast Na+ Transport

T2 - From Crystalline to Amorphous Networks in the Mixed-Anion NaTaOxCl6−2x Oxychlorides

AU - Leifeld, Justin

AU - Parsons, Abigail C.

AU - Morscher, Alexandra

AU - de Irujo-Labalde, Xabier Martinez

AU - Kraft, Marvin A.

AU - Soulas, Oskar G.

AU - Samanta, Bibek

AU - Zielasko, Wiebke

AU - Yadav, Neelam

AU - Strotmann, Kyra

AU - Jalarvo, Niina

AU - Rodrigues, Bruno V.M.

AU - Slabon, Adam

AU - Adelhelm, Philipp

AU - Hansen, Michael Ryan

AU - Scanlon, David O.

AU - Zeier, Wolfgang G.

AU - Squires, Alexander G.

PY - 2026/6/24

Y1 - 2026/6/24

N2 - Solid electrolytes are central to enabling safe, high-energy solid-state sodium batteries. While oxyhalide-type conductors have rapidly advanced lithium-based systems, their sodium analogues remain less understood and underdeveloped. This gap arises from their intrinsically amorphous nature, which obscures structure–transport relationships and limits rational design. Here, we elucidate the atomic-scale origins of sodium-ion conduction in the mixed-anion series NaTaOxCl6–2x using a combination of experimental and computational approaches. We reveal that composition-dependent, disordered yet extended chain motifs emerge as key structural units governing ion mobility. By tuning chain connectivity, we achieve a high ionic conductivity of ∼4 mS cm−1 and a corresponding self-diffusion coefficient of 6.6–8.2 × 10−11 m2 s−1, ranking among to the fastest reported for sodium oxyhalides. These findings establish clear structure–property correlations in amorphous superionic conductors and provide a blueprint for the targeted design of next-generation solid electrolytes for sodium solid-state batteries.

AB - Solid electrolytes are central to enabling safe, high-energy solid-state sodium batteries. While oxyhalide-type conductors have rapidly advanced lithium-based systems, their sodium analogues remain less understood and underdeveloped. This gap arises from their intrinsically amorphous nature, which obscures structure–transport relationships and limits rational design. Here, we elucidate the atomic-scale origins of sodium-ion conduction in the mixed-anion series NaTaOxCl6–2x using a combination of experimental and computational approaches. We reveal that composition-dependent, disordered yet extended chain motifs emerge as key structural units governing ion mobility. By tuning chain connectivity, we achieve a high ionic conductivity of ∼4 mS cm−1 and a corresponding self-diffusion coefficient of 6.6–8.2 × 10−11 m2 s−1, ranking among to the fastest reported for sodium oxyhalides. These findings establish clear structure–property correlations in amorphous superionic conductors and provide a blueprint for the targeted design of next-generation solid electrolytes for sodium solid-state batteries.

UR - https://www.scopus.com/pages/publications/105036492965

U2 - 10.1002/aenm.70977

DO - 10.1002/aenm.70977

M3 - Article

AN - SCOPUS:105036492965

SN - 1614-6832

VL - 16

JO - Advanced Energy Materials

JF - Advanced Energy Materials

IS - 24

M1 - e70977

ER -

Disorder-Driven Fast Na⁺ Transport: From Crystalline to Amorphous Networks in the Mixed-Anion NaTaO_xCl₆₋₂_x Oxychlorides

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this