In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries

Abstract Recently, all‐solid‐state sodium batteries (Na‐ASSBs) have received increased interest owing to their high safety and potential of high energy density. The potential of Na‐ASSBs based on sodium superionic conductor (NASICON)‐structured Na3V2(PO4)3(Na3VP) cathodes have been proven by their h...

Full description

Bibliographic Details
Main Authors: Fang‐Chun Shen, Qianli Ma, Frank Tietz, Jui‐Cheng Kao, Chi‐Ting Huang, Rahmandhika Firdauzha Hary Hernandha, Chun‐Wei Huang, Yu‐Chieh Lo, Jeng‐Kuei Chang, Wen‐Wei Wu
Format: Article
Language:English
Published: Wiley 2023-11-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202301490
_version_ 1797627743624495104
author Fang‐Chun Shen
Qianli Ma
Frank Tietz
Jui‐Cheng Kao
Chi‐Ting Huang
Rahmandhika Firdauzha Hary Hernandha
Chun‐Wei Huang
Yu‐Chieh Lo
Jeng‐Kuei Chang
Wen‐Wei Wu
author_facet Fang‐Chun Shen
Qianli Ma
Frank Tietz
Jui‐Cheng Kao
Chi‐Ting Huang
Rahmandhika Firdauzha Hary Hernandha
Chun‐Wei Huang
Yu‐Chieh Lo
Jeng‐Kuei Chang
Wen‐Wei Wu
author_sort Fang‐Chun Shen
collection DOAJ
description Abstract Recently, all‐solid‐state sodium batteries (Na‐ASSBs) have received increased interest owing to their high safety and potential of high energy density. The potential of Na‐ASSBs based on sodium superionic conductor (NASICON)‐structured Na3V2(PO4)3(Na3VP) cathodes have been proven by their high capacity and a long cycling stability closely related to the microstructural evolution. However, the detailed kinetics of the electrochemical processes in the cathodes is still unclear. In this work, the sodiation/desodiation process of Na3VP is first investigated using in situ high‐resolution transmission electron microscopy (HRTEM). The intermediate Na2V2(PO4)3 (Na2VP) phase with the P21/c space group, which would be inhibited by constant electron beam irradiation, is observed at the atomic scale. With the calculated volume change and the electrode–electrolyte interface after cycling, it can be concluded that the  Na2VP phase reduces the lattice mismatch between Na3VP and NaV2(PO4)3 (NaVP), preventing structural collapse. Based on the density functional theory calculation (DFT), the Na+ ion migrates more rapidly in the Na2VP structure, which facilitates the desodiation and sodiation processes. The formation of  Na2VP phase lowers the formation energy of NaVP. This study demonstrates the dynamic evolution of the Na3VP structure, paving the way for an in‐depth understanding of electrode materials for energy‐storage applications.
first_indexed 2024-03-11T10:28:40Z
format Article
id doaj.art-7f63d3cec13c4c88896dba6abeaa550b
institution Directory Open Access Journal
issn 2198-3844
language English
last_indexed 2024-03-11T10:28:40Z
publishDate 2023-11-01
publisher Wiley
record_format Article
series Advanced Science
spelling doaj.art-7f63d3cec13c4c88896dba6abeaa550b2023-11-15T05:46:35ZengWileyAdvanced Science2198-38442023-11-011032n/an/a10.1002/advs.202301490In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium BatteriesFang‐Chun Shen0Qianli Ma1Frank Tietz2Jui‐Cheng Kao3Chi‐Ting Huang4Rahmandhika Firdauzha Hary Hernandha5Chun‐Wei Huang6Yu‐Chieh Lo7Jeng‐Kuei Chang8Wen‐Wei Wu9Department of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanForschungszentrum Jülich GmbH Institute of Energy and Climate Research Materials Synthesis and Processing (IEK‐1) 52425 Jülich GermanyForschungszentrum Jülich GmbH Institute of Energy and Climate Research Materials Synthesis and Processing (IEK‐1) 52425 Jülich GermanyDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanDepartment of Materials Science and Engineering Feng Chia University No. 100, Wenhwa Rd., Seatwen Taichung 40724 TaiwanDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanDepartment of Materials Science and Engineering National Yang Ming Chiao Tung University Hsinchu 30010 TaiwanAbstract Recently, all‐solid‐state sodium batteries (Na‐ASSBs) have received increased interest owing to their high safety and potential of high energy density. The potential of Na‐ASSBs based on sodium superionic conductor (NASICON)‐structured Na3V2(PO4)3(Na3VP) cathodes have been proven by their high capacity and a long cycling stability closely related to the microstructural evolution. However, the detailed kinetics of the electrochemical processes in the cathodes is still unclear. In this work, the sodiation/desodiation process of Na3VP is first investigated using in situ high‐resolution transmission electron microscopy (HRTEM). The intermediate Na2V2(PO4)3 (Na2VP) phase with the P21/c space group, which would be inhibited by constant electron beam irradiation, is observed at the atomic scale. With the calculated volume change and the electrode–electrolyte interface after cycling, it can be concluded that the  Na2VP phase reduces the lattice mismatch between Na3VP and NaV2(PO4)3 (NaVP), preventing structural collapse. Based on the density functional theory calculation (DFT), the Na+ ion migrates more rapidly in the Na2VP structure, which facilitates the desodiation and sodiation processes. The formation of  Na2VP phase lowers the formation energy of NaVP. This study demonstrates the dynamic evolution of the Na3VP structure, paving the way for an in‐depth understanding of electrode materials for energy‐storage applications.https://doi.org/10.1002/advs.202301490all‐solid‐stateatomic‐scaledynamic evolutionin situ TEMNa2V2(PO4)3Na3V2(PO4)3
spellingShingle Fang‐Chun Shen
Qianli Ma
Frank Tietz
Jui‐Cheng Kao
Chi‐Ting Huang
Rahmandhika Firdauzha Hary Hernandha
Chun‐Wei Huang
Yu‐Chieh Lo
Jeng‐Kuei Chang
Wen‐Wei Wu
In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
Advanced Science
all‐solid‐state
atomic‐scale
dynamic evolution
in situ TEM
Na2V2(PO4)3
Na3V2(PO4)3
title In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
title_full In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
title_fullStr In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
title_full_unstemmed In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
title_short In Situ Atomic‐Scale Investigation of Structural Evolution During Sodiation/Desodiation Processes in Na3V2(PO4)3‐Based All‐Solid‐State Sodium Batteries
title_sort in situ atomic scale investigation of structural evolution during sodiation desodiation processes in na3v2 po4 3 based all solid state sodium batteries
topic all‐solid‐state
atomic‐scale
dynamic evolution
in situ TEM
Na2V2(PO4)3
Na3V2(PO4)3
url https://doi.org/10.1002/advs.202301490
work_keys_str_mv AT fangchunshen insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT qianlima insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT franktietz insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT juichengkao insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT chitinghuang insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT rahmandhikafirdauzhaharyhernandha insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT chunweihuang insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT yuchiehlo insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT jengkueichang insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries
AT wenweiwu insituatomicscaleinvestigationofstructuralevolutionduringsodiationdesodiationprocessesinna3v2po43basedallsolidstatesodiumbatteries