Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12

Abstract Solid-state sodium metal batteries have attracted great interest because of their improved safety and abundant Na resources. However, the interfacial resistances and instabilities induced by parasitic reactions, together with Na dendrite issues, result in reduced rate capability and poor cy...

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Main Authors: Taiguang Li, Butian Chen, Tenghui Wang, Chong Liu, Wen Yin, Qianjiang Mao, Dongxu Zhou, Yongmei Hao, Xiangfeng Liu
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-60842-x
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author Taiguang Li
Butian Chen
Tenghui Wang
Chong Liu
Wen Yin
Qianjiang Mao
Dongxu Zhou
Yongmei Hao
Xiangfeng Liu
author_facet Taiguang Li
Butian Chen
Tenghui Wang
Chong Liu
Wen Yin
Qianjiang Mao
Dongxu Zhou
Yongmei Hao
Xiangfeng Liu
author_sort Taiguang Li
collection DOAJ
description Abstract Solid-state sodium metal batteries have attracted great interest because of their improved safety and abundant Na resources. However, the interfacial resistances and instabilities induced by parasitic reactions, together with Na dendrite issues, result in reduced rate capability and poor cycling stability. Here, we address these challenges by intrinsically inhibiting parasitic interfacial redox reactions through enhanced P-O covalency in Na3Zr2Si2PO12 (NZSP) with Na2SiF6 incorporation, wherein the high electronegativity of F strengthens P-O covalency. Additionally, SnF2 coating provides a sodiophilic surface and stabilizes the NZSP interface, which is essential for effective electrochemical cycling. This integrated approach significantly reduces interfacial impedance to 2.0 Ω cm2, enabling stable Na plating/stripping for 3600 hours at 0.5 mA cm-2/0.25 mAh cm-2. The full cell with Na3V2(PO4)3 positive electrode demonstrates stable cycling with high-rate capability (87.5% capacity retention after 2500 cycles at 1 C and 96.1% capacity retention after 1200 cycles at 5 C). This study sheds light on the development of high-performance quasi-solid-state sodium batteries.
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institution Kabale University
issn 2041-1723
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publishDate 2025-07-01
publisher Nature Portfolio
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spelling doaj-art-a5fd359a87e94ecfaaee2df6c261b13b2025-08-20T03:37:38ZengNature PortfolioNature Communications2041-17232025-07-0116111810.1038/s41467-025-60842-xAchieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12Taiguang Li0Butian Chen1Tenghui Wang2Chong Liu3Wen Yin4Qianjiang Mao5Dongxu Zhou6Yongmei Hao7Xiangfeng Liu8Center of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesSpallation Neutron Source Science CenterCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesSchool of Chemical Sciences, University of Chinese Academy of SciencesCenter of Materials Science and Optoelectronics Engineering, College of Materials Science and Optoelectronic Technology, University of Chinese Academy of SciencesAbstract Solid-state sodium metal batteries have attracted great interest because of their improved safety and abundant Na resources. However, the interfacial resistances and instabilities induced by parasitic reactions, together with Na dendrite issues, result in reduced rate capability and poor cycling stability. Here, we address these challenges by intrinsically inhibiting parasitic interfacial redox reactions through enhanced P-O covalency in Na3Zr2Si2PO12 (NZSP) with Na2SiF6 incorporation, wherein the high electronegativity of F strengthens P-O covalency. Additionally, SnF2 coating provides a sodiophilic surface and stabilizes the NZSP interface, which is essential for effective electrochemical cycling. This integrated approach significantly reduces interfacial impedance to 2.0 Ω cm2, enabling stable Na plating/stripping for 3600 hours at 0.5 mA cm-2/0.25 mAh cm-2. The full cell with Na3V2(PO4)3 positive electrode demonstrates stable cycling with high-rate capability (87.5% capacity retention after 2500 cycles at 1 C and 96.1% capacity retention after 1200 cycles at 5 C). This study sheds light on the development of high-performance quasi-solid-state sodium batteries.https://doi.org/10.1038/s41467-025-60842-x
spellingShingle Taiguang Li
Butian Chen
Tenghui Wang
Chong Liu
Wen Yin
Qianjiang Mao
Dongxu Zhou
Yongmei Hao
Xiangfeng Liu
Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
Nature Communications
title Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
title_full Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
title_fullStr Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
title_full_unstemmed Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
title_short Achieving stable and high-rate quasi-solid-state sodium batteries through strengthened P-O covalency and interface modification in Na3Zr2Si2PO12
title_sort achieving stable and high rate quasi solid state sodium batteries through strengthened p o covalency and interface modification in na3zr2si2po12
url https://doi.org/10.1038/s41467-025-60842-x
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