Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries
Polymer-based composite solid electrolytes (PCSEs) are increasingly studied in all-solid-state lithium-metal batteries (ASSLMBs) due to the combined advantages of better flexibility of polymer and higher ion conductivity of ceramic electrolytes. However, most reported PCSEs are overly thick, increas...
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IOP Publishing
2025-01-01
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| Series: | Materials Futures |
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| Online Access: | https://doi.org/10.1088/2752-5724/ada0cc |
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| author | Fenghua Yu Yongbiao Mu Meisheng Han Jie Liu Kunxiong Zheng Zhiyu Zou Hengyuan Hu Quanyan Man Wenjia Li Lei Wei Lin Zeng Tianshou Zhao |
| author_facet | Fenghua Yu Yongbiao Mu Meisheng Han Jie Liu Kunxiong Zheng Zhiyu Zou Hengyuan Hu Quanyan Man Wenjia Li Lei Wei Lin Zeng Tianshou Zhao |
| author_sort | Fenghua Yu |
| collection | DOAJ |
| description | Polymer-based composite solid electrolytes (PCSEs) are increasingly studied in all-solid-state lithium-metal batteries (ASSLMBs) due to the combined advantages of better flexibility of polymer and higher ion conductivity of ceramic electrolytes. However, most reported PCSEs are overly thick, increasing internal resistances. Besides, the poor stability at the Li metal–electrolyte interfaces often leads to severe lithium dendrite formation and reduced cycling stability. Here, we fabricate an ultrathin PCSE with a thickness of 12.4 μ m, incorporating polyacrylonitrile (PAN) nanofibers as the structural matrix, and a filler with polyethylene oxide and Li _6.5 La _3 Zr _1.5 Ta _0.5 O _12 (LLZTO). Due to the formation of the LiCN layer on the surface of the lithium metal and the Li-ion transport pathways induced by the dehydrocyanation reaction at the LLZTO/PAN interfaces, the PCSE exhibits a high critical current density of 1.8 mA cm ^−2 and a low energy barrier of 0.278 eV for Li-ion transfer, accommodating the fast Li-ion migration to avoid Li-dendrite growth. In addition, the stable nitrile groups and the dehydrocyanation reaction ensure the electrochemical stability of the PCSE with a high oxidation voltage of 5.5 V and an exceptional cycling stability (2100 h) in Li||PCSE||Li symmetric cells. Additionally, the Li||PCSE||LiFePO _4 full cells demonstrate a high volumetric energy density of 338.3 Wh L ^−1 at 0.1 C and a robust stability over 100 cycles at 0.5 C. The study offers a new approach for fabricating ultrathin PCSEs and provides insights into the mechanisms of dendrite-free formation, guiding the development of high-performance PCSEs for ASSLMBs. |
| format | Article |
| id | doaj-art-00c578fdf2834f34ae7c2e6e1728ed3f |
| institution | Kabale University |
| issn | 2752-5724 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | IOP Publishing |
| record_format | Article |
| series | Materials Futures |
| spelling | doaj-art-00c578fdf2834f34ae7c2e6e1728ed3f2025-01-16T11:47:32ZengIOP PublishingMaterials Futures2752-57242025-01-014101510110.1088/2752-5724/ada0ccElectrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteriesFenghua Yu0Yongbiao Mu1Meisheng Han2https://orcid.org/0000-0001-9462-3572Jie Liu3Kunxiong Zheng4Zhiyu Zou5Hengyuan Hu6Quanyan Man7Wenjia Li8Lei Wei9Lin Zeng10Tianshou Zhao11https://orcid.org/0000-0003-4825-2381Shenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaShenzhen Key Laboratory of Advanced Energy Storage, Department of Mechanical and Energy Engineering, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of China; SUSTech Energy Institute for Carbon Neutrality, Southern University of Science and Technology , Shenzhen 518055, People’s Republic of ChinaPolymer-based composite solid electrolytes (PCSEs) are increasingly studied in all-solid-state lithium-metal batteries (ASSLMBs) due to the combined advantages of better flexibility of polymer and higher ion conductivity of ceramic electrolytes. However, most reported PCSEs are overly thick, increasing internal resistances. Besides, the poor stability at the Li metal–electrolyte interfaces often leads to severe lithium dendrite formation and reduced cycling stability. Here, we fabricate an ultrathin PCSE with a thickness of 12.4 μ m, incorporating polyacrylonitrile (PAN) nanofibers as the structural matrix, and a filler with polyethylene oxide and Li _6.5 La _3 Zr _1.5 Ta _0.5 O _12 (LLZTO). Due to the formation of the LiCN layer on the surface of the lithium metal and the Li-ion transport pathways induced by the dehydrocyanation reaction at the LLZTO/PAN interfaces, the PCSE exhibits a high critical current density of 1.8 mA cm ^−2 and a low energy barrier of 0.278 eV for Li-ion transfer, accommodating the fast Li-ion migration to avoid Li-dendrite growth. In addition, the stable nitrile groups and the dehydrocyanation reaction ensure the electrochemical stability of the PCSE with a high oxidation voltage of 5.5 V and an exceptional cycling stability (2100 h) in Li||PCSE||Li symmetric cells. Additionally, the Li||PCSE||LiFePO _4 full cells demonstrate a high volumetric energy density of 338.3 Wh L ^−1 at 0.1 C and a robust stability over 100 cycles at 0.5 C. The study offers a new approach for fabricating ultrathin PCSEs and provides insights into the mechanisms of dendrite-free formation, guiding the development of high-performance PCSEs for ASSLMBs.https://doi.org/10.1088/2752-5724/ada0ccpolymer-based composite solid electrolytesall-solid-state lithium-metal batteriesinterfacial stabilityultrathin thicknessdendrite-free growth |
| spellingShingle | Fenghua Yu Yongbiao Mu Meisheng Han Jie Liu Kunxiong Zheng Zhiyu Zou Hengyuan Hu Quanyan Man Wenjia Li Lei Wei Lin Zeng Tianshou Zhao Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries Materials Futures polymer-based composite solid electrolytes all-solid-state lithium-metal batteries interfacial stability ultrathin thickness dendrite-free growth |
| title | Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries |
| title_full | Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries |
| title_fullStr | Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries |
| title_full_unstemmed | Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries |
| title_short | Electrochemically stable and ultrathin polymer-based solid electrolytes for dendrite-free all-solid-state lithium-metal batteries |
| title_sort | electrochemically stable and ultrathin polymer based solid electrolytes for dendrite free all solid state lithium metal batteries |
| topic | polymer-based composite solid electrolytes all-solid-state lithium-metal batteries interfacial stability ultrathin thickness dendrite-free growth |
| url | https://doi.org/10.1088/2752-5724/ada0cc |
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