# First‐Principles Study on the Interfacial Cathode‐Contact Stability and Li Diffusivity of N‐Doped Li                    <sub>6</sub>                    Zr                    <sub>2</sub>                    O                    <sub>7</sub>                    for All‐Solid‐State Li‐Ion Batteries

https://mdr.nims.go.jp/datasets/088bb5db-8e53-4537-8190-55ac9a82ebb4

## File

- [manuscript_LZON_rev1_clean.pdf](https://mdr.nims.go.jp/filesets/9bfd2a86-04ab-418c-8dc0-c7fde19317d6/download) ([Detail](https://mdr.nims.go.jp/filesets/9bfd2a86-04ab-418c-8dc0-c7fde19317d6.md))

## Id

088bb5db-8e53-4537-8190-55ac9a82ebb4

## Local identifier



## Visibility

open_to_public

## State

published

## Created at

2025-12-16T09:03:46.923920Z

## Updated at

2025-12-18T23:30:58.888934Z

## Published at

2025-12-18T10:08:19.617580Z

## Doi

https://doi.org/10.48505/nims.6027

## First published url

https://doi.org/10.1002/smtd.202501289

## Date published

2025-10-01

## Recorded date published

2025-11

## Resource type

journal_article

## Manuscript type

accepted_manuscript

## Collection



## Title

- title: First‐Principles Study on the Interfacial Cathode‐Contact Stability and Li
    Diffusivity of N‐Doped Li                    <sub>6</sub>                    Zr                    <sub>2</sub>                    O                    <sub>7</sub>                    for
    All‐Solid‐State Li‐Ion Batteries
  title_type: original
  lang: en

## Description

- description: Here, N-doped Li6Zr2O7 (LZON) is investigated using first-principles
    density functional theory (DFT) methods to evaluate its (electro)chemical stability
    and Li-ion transport properties for its novel design as a practical dual-use Li
    ionic conductor, both as a cathode-coating layer (CCL) and solid electrolyte (SE)
    in all-solid-state Li-ion batteries (ASSBs). Thermodynamic free energy calculations
    showed that LZO, as CCL and SE, is chemically stable versus most known cathode
    materials. Focusing on LiCoO2 (LCO) cathode, explicit hetero-interface modeling
    analysis of the low-energy LCO(104)|LZO(001) interface revealed that LZO can form
    a strongly adhered and a low-strain contact with LCO. The electronic structure
    of this interface has LCO-side states (Co-3d, O-2p) occupying the highest occupied
    states, thereby facilitating a stable cell charging. Climbing-image nudged elastic
    band calculations results suggested that the LCO(104)|LZO(001) interface also
    has interface-normal diffusion pathways with low Li ion migration energy. Meanwhile,
    ab-initio- and machine-learning-based molecular dynamics simulation results confirmed
    that Li diffusivity in bulk LZO can be greatly enhanced by several orders of magnitude
    via aliovalent N-doping with Li interstitial addition. For the LCO(104)|LZON(001)
    interface, the N dopant is determined to energetically prefer the LZON bulk region,
    the corresponding interface electronic structure that can also facilitate a stable
    ASSB cell charging.
  description_type: abstract
  lang: und

## Creator

- name: Randy Jalem
  role: author
  orcid: https://orcid.org/0000-0001-9505-771X
- name: Yoshitaka Tateyama
  role: author
  orcid: https://orcid.org/0000-0002-5532-6134
- name: Kazunori Takada
  role: author
  orcid: https://orcid.org/0000-0001-7568-1806
- name: Tetsuya Yamada
  role: author
- name: Katsuya Teshima
  role: author

## Contact agent



## Publisher

organization: Wiley

## Managing organization



## Keyword

- subject: all solid state batteries
  schema: not_defined
- subject: lithium ion conductors
  schema: not_defined
- subject: solid electrolytes
  schema: not_defined
- subject: cathode coatings
  schema: not_defined
- subject: first-principles calculations
  schema: not_defined
- subject: molecular dynamics simulations
  schema: not_defined
- subject: machine learning interatomic potentials
  schema: not_defined
- subject: solid hetero-interface modeling
  schema: not_defined

## Rights

- identifier: https://creativecommons.org/licenses/by-nc/4.0/

## Other identifier(s)



## Data origin

- data_origin_type: other

## Embargo



## Journal

- title: Small Methods
  issn: '23669608'
  volume: '9'
  issue: '11'
  article_number: e01289

## Conference



## Related item



## Funding

- identifier: JPMXP1020230325
  funder_name: Ministry of Education, Culture, Sports, Science and Technology
- identifier: JP21K14729
  funder_name: Japan Society for the Promotion of Science
- identifier: JPMJGX23S2
  funder_name: Japan Science and Technology Agency
- identifier: JPMXP0219207397
  funder_name: Ministry of Education, Culture, Sports, Science and Technology

## Instrument



## Instrument operator



## Instrument managing organization



## Measurement method



## Specimen



## Chemical composition



## Structure for specimen



## Structural feature for specimen



## Specific property for specimen



## Process for specimen treatment



## Computational method



## Energy level/transition state



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## Fileset

- id: 9bfd2a86-04ab-418c-8dc0-c7fde19317d6
  filename: manuscript_LZON_rev1_clean.pdf
  content_type: application/pdf
  size: 1691060
  md5: 650bdc80ae5ac8d31611d9b9942ec3d5

## Thumbnail

fileset_id: 9bfd2a86-04ab-418c-8dc0-c7fde19317d6
filename: manuscript_LZON_rev1_clean.pdf