Accelerated Workflow for Antiperovskite-based Solid State Electrolytes

Benjamin H. Sjølin; Peter B. Jørgensen; Andrea Fedrigucci; Tejs Vegge; Arghya Bhowmik; Ivano E. Castelli

doi:10.1002/batt.202300041

Accelerated Workflow for Antiperovskite-based Solid State Electrolytes

Benjamin H. Sjølin
, Peter B. Jørgensen
, Andrea Fedrigucci
, Tejs Vegge
, Arghya Bhowmik^*
, Ivano E. Castelli^*

^*Corresponding author for this work

Research output: Contribution to journal › Journal article › Research › peer-review

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Abstract

We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials with general formula X₃BA (X=Li, Na, Mg) and Pm-3m space group, searching for stable high-performance solid state electrolytes for all-solid state batteries. The workflow is based on the calculation of thermodynamic and kinetic properties, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. To accelerate calculation of the kinetic properties, we use a surrogate model to predict the transition state structure during ionic diffusion. This reduces the calculation cost by more than one order of magnitude while keeping the mean error within 73 meV of the more accurate nudged elastic band method. This method identifies 14 materials that agree with the experimentally reported results as some of the best solid state electrolytes. Moreover, this approach is general and chemistry neutral, so can be applied to other battery chemistries and crystal prototypes.

Original language	English
Article number	e202300041
Journal	Batteries and Supercaps
Volume	6
Issue number	6
Number of pages	10
ISSN	2566-6223
DOIs	https://doi.org/10.1002/batt.202300041
Publication status	Published - 2023

Bibliographical note

The authors acknowledge support from the EU’s Horizon 2020 research and innovation program under grants agreement No 957189 (BIG-MAP) and No 957213 (BATTERY 2030PLUS). BHS and IEC acknowledge support from the Independent Research Fund Denmark (Research Project 1, project “Rational Design of High-Entropy Oxides for Protonic Ceramic Fuel Cells”, grant number No 1032-00269B). PBJ and AB acknowledges financial support from VILLUM FONDEN (DeepDFT project, research grant No 00023105).

Keywords

Antiperovskites
Density functional calculations
High-throughput screening
Solid state electrolytes
Surrogate model

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@article{8056d92acde4484089989f6d19dce0d3,

title = "Accelerated Workflow for Antiperovskite-based Solid State Electrolytes",

abstract = "We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials with general formula X3BA (X=Li, Na, Mg) and Pm-3m space group, searching for stable high-performance solid state electrolytes for all-solid state batteries. The workflow is based on the calculation of thermodynamic and kinetic properties, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. To accelerate calculation of the kinetic properties, we use a surrogate model to predict the transition state structure during ionic diffusion. This reduces the calculation cost by more than one order of magnitude while keeping the mean error within 73 meV of the more accurate nudged elastic band method. This method identifies 14 materials that agree with the experimentally reported results as some of the best solid state electrolytes. Moreover, this approach is general and chemistry neutral, so can be applied to other battery chemistries and crystal prototypes.",

keywords = "Antiperovskites, Density functional calculations, High-throughput screening, Solid state electrolytes, Surrogate model",

author = "Sj{\o}lin, \{Benjamin H.\} and J{\o}rgensen, \{Peter B.\} and Andrea Fedrigucci and Tejs Vegge and Arghya Bhowmik and Castelli, \{Ivano E.\}",

note = "The authors acknowledge support from the EU{\textquoteright}s Horizon 2020 research and innovation program under grants agreement No 957189 (BIG-MAP) and No 957213 (BATTERY 2030PLUS). BHS and IEC acknowledge support from the Independent Research Fund Denmark (Research Project 1, project {\textquotedblleft}Rational Design of High-Entropy Oxides for Protonic Ceramic Fuel Cells{\textquotedblright}, grant number No 1032-00269B). PBJ and AB acknowledges financial support from VILLUM FONDEN (DeepDFT project, research grant No 00023105).",

year = "2023",

doi = "10.1002/batt.202300041",

language = "English",

volume = "6",

journal = "Batteries and Supercaps",

issn = "2566-6223",

publisher = "Wiley-VCH",

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AU - Sjølin, Benjamin H.

AU - Jørgensen, Peter B.

AU - Fedrigucci, Andrea

AU - Vegge, Tejs

AU - Bhowmik, Arghya

AU - Castelli, Ivano E.

N1 - The authors acknowledge support from the EU’s Horizon 2020 research and innovation program under grants agreement No 957189 (BIG-MAP) and No 957213 (BATTERY 2030PLUS). BHS and IEC acknowledge support from the Independent Research Fund Denmark (Research Project 1, project “Rational Design of High-Entropy Oxides for Protonic Ceramic Fuel Cells”, grant number No 1032-00269B). PBJ and AB acknowledges financial support from VILLUM FONDEN (DeepDFT project, research grant No 00023105).

PY - 2023

Y1 - 2023

N2 - We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials with general formula X3BA (X=Li, Na, Mg) and Pm-3m space group, searching for stable high-performance solid state electrolytes for all-solid state batteries. The workflow is based on the calculation of thermodynamic and kinetic properties, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. To accelerate calculation of the kinetic properties, we use a surrogate model to predict the transition state structure during ionic diffusion. This reduces the calculation cost by more than one order of magnitude while keeping the mean error within 73 meV of the more accurate nudged elastic band method. This method identifies 14 materials that agree with the experimentally reported results as some of the best solid state electrolytes. Moreover, this approach is general and chemistry neutral, so can be applied to other battery chemistries and crystal prototypes.

AB - We developed and implemented a multi-target multi-fidelity workflow to explore the chemical space of antiperovskite materials with general formula X3BA (X=Li, Na, Mg) and Pm-3m space group, searching for stable high-performance solid state electrolytes for all-solid state batteries. The workflow is based on the calculation of thermodynamic and kinetic properties, including phase and electrochemical stability, semiconducting behavior, and ionic diffusivity. To accelerate calculation of the kinetic properties, we use a surrogate model to predict the transition state structure during ionic diffusion. This reduces the calculation cost by more than one order of magnitude while keeping the mean error within 73 meV of the more accurate nudged elastic band method. This method identifies 14 materials that agree with the experimentally reported results as some of the best solid state electrolytes. Moreover, this approach is general and chemistry neutral, so can be applied to other battery chemistries and crystal prototypes.

KW - Antiperovskites

KW - Density functional calculations

KW - High-throughput screening

KW - Solid state electrolytes

KW - Surrogate model

U2 - 10.1002/batt.202300041

DO - 10.1002/batt.202300041

M3 - Journal article

SN - 2566-6223

VL - 6

JO - Batteries and Supercaps

JF - Batteries and Supercaps

IS - 6

M1 - e202300041

ER -

Accelerated Workflow for Antiperovskite-based Solid State Electrolytes

Abstract

Bibliographical note

Keywords

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