Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries
Abstract Anode-free lithium batteries represent a promising avenue for high-energy-density storage, yet their practical application is hindered by lithium inventory loss from parasitic interfacial reactions, cathode degradation, and limited Li+ reversibility. Herein, we propose a polyolefin separato...
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Nature Portfolio
2025-05-01
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| Series: | Nature Communications |
| Online Access: | https://doi.org/10.1038/s41467-025-59521-8 |
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| author | Ahu Shao Helin Wang Min Zhang Jiacheng Liu Lu Cheng Yunsong Li Yuxiang Guo Zhiqiao Wang Qiurong Jia Xin Wang Xiaoyu Tang Xiaodong Zhao Yue Ma |
| author_facet | Ahu Shao Helin Wang Min Zhang Jiacheng Liu Lu Cheng Yunsong Li Yuxiang Guo Zhiqiao Wang Qiurong Jia Xin Wang Xiaoyu Tang Xiaodong Zhao Yue Ma |
| author_sort | Ahu Shao |
| collection | DOAJ |
| description | Abstract Anode-free lithium batteries represent a promising avenue for high-energy-density storage, yet their practical application is hindered by lithium inventory loss from parasitic interfacial reactions, cathode degradation, and limited Li+ reversibility. Herein, we propose a polyolefin separator integrated with a Li2S@C sacrificial layer, achieving multiscale interfacial stabilization in Ah-class anode-free pouch cells. This approach simultaneously replenishes the customized Li+ inventory during the formation cycle and establishes the lithium polysulfide-containing cathode interface with high-voltage tolerance (till 4.5 V). Real-time tracking via in-situ electrochemical impedance spectroscopy and transmission-mode operando X-ray diffraction reveals accelerated Li+ diffusion kinetics and stabilized phase evolution in LiNi0.8Co0.1Mn0.1O2 cathode interfaced with Li2S@C|PE prelithiation separator. Consequently, a 1.22 Ah pouch cell with an Ag-modified Cu foil and LiNi0.8Co0.1Mn0.1O2 cathode is assembled with Li2S@C|PE separator and exhibits gravimetric and volumetric energy densities of 450 Wh kg-1 and 1355 Wh L-1, respectively. This prelithiation protocol demonstrates upscaling potential and generic applicability to secure the interfacial chemistries for anode free/less lithium metal batteries. |
| format | Article |
| id | doaj-art-070b3564c23a44a2ba8e1df3e536c15e |
| institution | OA Journals |
| issn | 2041-1723 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Nature Communications |
| spelling | doaj-art-070b3564c23a44a2ba8e1df3e536c15e2025-08-20T02:11:22ZengNature PortfolioNature Communications2041-17232025-05-0116111210.1038/s41467-025-59521-8Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteriesAhu Shao0Helin Wang1Min Zhang2Jiacheng Liu3Lu Cheng4Yunsong Li5Yuxiang Guo6Zhiqiao Wang7Qiurong Jia8Xin Wang9Xiaoyu Tang10Xiaodong Zhao11Yue Ma12State Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityShaanxi Raisight Energy Tech Co. LtdState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityFujian Blue Ocean & Black Stone Technology Co. LtdState Key Laboratory of Solidification Processing, Center for Nano Energy Materials, School of Materials Science and Engineering, Northwestern Polytechnical UniversityAbstract Anode-free lithium batteries represent a promising avenue for high-energy-density storage, yet their practical application is hindered by lithium inventory loss from parasitic interfacial reactions, cathode degradation, and limited Li+ reversibility. Herein, we propose a polyolefin separator integrated with a Li2S@C sacrificial layer, achieving multiscale interfacial stabilization in Ah-class anode-free pouch cells. This approach simultaneously replenishes the customized Li+ inventory during the formation cycle and establishes the lithium polysulfide-containing cathode interface with high-voltage tolerance (till 4.5 V). Real-time tracking via in-situ electrochemical impedance spectroscopy and transmission-mode operando X-ray diffraction reveals accelerated Li+ diffusion kinetics and stabilized phase evolution in LiNi0.8Co0.1Mn0.1O2 cathode interfaced with Li2S@C|PE prelithiation separator. Consequently, a 1.22 Ah pouch cell with an Ag-modified Cu foil and LiNi0.8Co0.1Mn0.1O2 cathode is assembled with Li2S@C|PE separator and exhibits gravimetric and volumetric energy densities of 450 Wh kg-1 and 1355 Wh L-1, respectively. This prelithiation protocol demonstrates upscaling potential and generic applicability to secure the interfacial chemistries for anode free/less lithium metal batteries.https://doi.org/10.1038/s41467-025-59521-8 |
| spellingShingle | Ahu Shao Helin Wang Min Zhang Jiacheng Liu Lu Cheng Yunsong Li Yuxiang Guo Zhiqiao Wang Qiurong Jia Xin Wang Xiaoyu Tang Xiaodong Zhao Yue Ma Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries Nature Communications |
| title | Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries |
| title_full | Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries |
| title_fullStr | Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries |
| title_full_unstemmed | Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries |
| title_short | Multiscale interfacial stabilization via prelithiation separator engineering for Ah-level anode-free lithium batteries |
| title_sort | multiscale interfacial stabilization via prelithiation separator engineering for ah level anode free lithium batteries |
| url | https://doi.org/10.1038/s41467-025-59521-8 |
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