# Multiobjective Solid Electrolyte Design of Tetragonal and Cubic Inverse-Perovskites for All-Solid-State Lithium-Ion Batteries by High-Throughput Density Functional Theory Calculations and AI-Driven Methods https://mdr.nims.go.jp/datasets/31cd0c96-f1ea-400a-af53-1e35cf5cdf7b ## File - [jp3c02801_clean.pdf](https://mdr.nims.go.jp/filesets/ad9dd318-0e86-4b0b-86b0-f7a933362060/download) ([Detail](https://mdr.nims.go.jp/filesets/ad9dd318-0e86-4b0b-86b0-f7a933362060.md)) - [esi_clean.pdf](https://mdr.nims.go.jp/filesets/65bfece5-10fe-4c0b-8ff3-cd6c0b8c94bb/download) ([Detail](https://mdr.nims.go.jp/filesets/65bfece5-10fe-4c0b-8ff3-cd6c0b8c94bb.md)) ## Id 31cd0c96-f1ea-400a-af53-1e35cf5cdf7b ## Local identifier ## Visibility open_to_public ## State published ## Created at 2023-12-06T03:26:05.105279Z ## Updated at 2024-08-27T23:30:15.635368Z ## Published at 2024-08-27T23:30:16.327944Z ## Doi https://doi.org/10.48505/nims.4305 ## First published url https://doi.org/10.1021/acs.jpcc.3c02801 ## Date published 2023-09-07 ## Recorded date published 2023-9-7 ## Resource type journal_article ## Manuscript type accepted_manuscript ## Collection ## Title - title: Multiobjective Solid Electrolyte Design of Tetragonal and Cubic Inverse-Perovskites for All-Solid-State Lithium-Ion Batteries by High-Throughput Density Functional Theory Calculations and AI-Driven Methods title_type: original lang: en ## Description - description: 'Solid electrolytes (SEs) are crucial materials to realize highly safe and practical all-solid-state Li+-ion batteries. Here, we performed a large-scale computational SE screening on a chemical space of >10 000 Li-rich inverse-perovskite (ip) compounds with tetragonal and cubic structures by high-throughput density functional theory (DFT) and AI-driven methods. A total of 1413 novel candidate compounds were predicted to be synthesizable based on thermodynamic decomposition energy (Ed) and machine-learned experimental synthesis likelihood (Ls). These compounds were further screened using a Pareto-front approximation set of a multiobjective Bayesian optimization tasks for k = 3 DFT-calculated SE properties (fk, with k = 1, 2, and 3): (i) electrochemical window from electronic band gap energy (f1: Eg), (ii) chemical stability by reaction with moisture (f2: Eh), and (iii) 400 K bulk Li+-ion conductivity (f3: Λ). As a result, the compound list was reduced down to 24 candidate ip SEs, and examples include Cm Li8O2Cl3Br (Ed = 0, Ls > 0.5, Eg = 4.74 eV, Eh = −33.22 kJ/mol, and Λ = 9.0 × 10–4 S/cm), Amm2 Li8OSCl4 (Ed = 0.070 eV/atom, Ls > 0.5, Eg = 4.14 eV, Eh = −40.70 kJ/mol, and Λ = 9.2 × 10–2 S/cm), and Cmcm Li12O3SeClBr3 (Ed = 0.097 eV/atom, Ls > 0.5, Eg = 3.36 eV, Eh = −86.88 kJ/mol, and Λ = 7.8 × 10–1 S/cm). Possible solid-state synthesis routes for the screened SE candidates were also explored using thermodynamic phase competition analysis and classical nucleation theory reaction barrier. Aside from providing a well-informed list of potentially novel ip-type SEs, our work also reports on an effective calculation methodology for tiered large-scale material screening which, at the same time, incorporates “small data” learning on target property datasets that are computationally expensive to obtain. The generated datasets are expected as well to be of great utility for future data-driven material design efforts.' description_type: abstract lang: eng ## Creator - name: JALEM Randy role: author orcid: https://orcid.org/0000-0001-9505-771X organization: National Institute for Materials Science department: Research Center for Energy and Environmental Materials (GREEN)/Battery and Cell Materials Field/Interface Electrochemistry Group ror: https://ror.org/026v1ze26 - name: TATEYAMA Yoshitaka role: author orcid: https://orcid.org/0000-0002-5532-6134 organization: National Institute for Materials Science department: Research Center for Energy and Environmental Materials (GREEN)/Battery and Cell Materials Field/Interface Electrochemistry Group ror: https://ror.org/026v1ze26 - name: TAKADA Kazunori role: author orcid: https://orcid.org/0000-0001-7568-1806 organization: National Institute for Materials Science department: Research Center for Energy and Environmental Materials (GREEN)/Battery and Cell Materials Field/Solid-State Battery Group ror: https://ror.org/026v1ze26 - name: JANG Seonghoon role: author organization: National Institute for Materials Science department: Research Center for Energy and Environmental Materials (GREEN)/Battery and Cell Materials Field/Interface Electrochemistry Group ror: https://ror.org/026v1ze26 ## Contact agent ## Publisher organization: ACS Publications ## Managing organization ## Keyword - subject: all solid state batteries schema: not_defined - subject: solid electrolytes schema: not_defined - subject: density functional theory schema: not_defined - subject: materials informatics schema: not_defined - subject: machine learning schema: not_defined - subject: novel materials search schema: not_defined ## Rights - description: This document is the Accepted Manuscript version of a Published Work that appeared in final form in The Journal of Physical Chemistry C, copyright © 2023 American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpcc.3c02801 identifier: http://rightsstatements.org/vocab/InC/1.0/ ## Other identifier(s) ## Data origin - data_origin_type: other ## Embargo start_date: 2023-08-28 end_date: 2024-08-28 ## Journal - title: Journal of Physical Chemistry C issn: '19327455' volume: '127' issue: '35' start_page: 17307 end_page: 17323 ## Conference ## Related item ## Funding - identifier: JPMJAL1301 funder_name: JST ALCA-SPRING description: JST, Japan Science and Technology Agency - identifier: JPMJPF2016 funder_name: JST COI-NEXT description: JST, Japan Science and Technology Agency - identifier: JP19H05815 funder_name: JSPS KAKENHI description: JSPS, Japan Society for the Promotion of Science - identifier: JP21K14729 funder_name: JSPS KAKENHI description: JSPS, Japan Society for the Promotion of Science - identifier: JPMXP0219207397 funder_name: Materials Processing Science project (Materealize) description: MEXT - identifier: JPMXP1020200301 funder_name: Program for Promoting Researchon the Supercomputer Fugaku description: MEXT ## 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 ## Software ## Custom property ## Fileset - id: ad9dd318-0e86-4b0b-86b0-f7a933362060 filename: jp3c02801_clean.pdf content_type: application/pdf size: 2593031 md5: 500afca30ec6d82a309d89af28342ae5 - id: 65bfece5-10fe-4c0b-8ff3-cd6c0b8c94bb filename: esi_clean.pdf content_type: application/pdf size: 1467437 md5: 1d7a2f905bb7e80bc03e652e84860183 ## Thumbnail fileset_id: 65bfece5-10fe-4c0b-8ff3-cd6c0b8c94bb filename: esi_clean.pdf