Transient Atom-Economy Utilization of Residual Binder for Upcycling the Spent LiFePO 4 Cathodes

Open AccessCCS ChemistryRESEARCH ARTICLES8 Sep 2025Transient Atom-Economy Utilization of Residual Binder for Upcycling the Spent LiFePO4 Cathodes Yuansheng Lin, Huijun Liu, Chenyu Wang, Hao Wang, Rui Liu, Enze Li, Yingbo Deng, Zhaowei Lin, Cihang Zhang, Honghao Wang, Haoyu Xue, Yixuan Liu, Zhe Pu, Guanwu Lian, Zhao-Hui Dong, Ke Yang, Zirui Lou, Zhongxin Chen, Baisheng Sa, Longlong Fan, Xiaoxu Zhao and Mingjian Zhang Yuansheng Lin , Huijun Liu , Chenyu Wang , Hao Wang , Rui Liu , Enze Li , Yingbo Deng , Zhaowei Lin , Cihang Zhang , Honghao Wang , Haoyu Xue , Yixuan Liu , Zhe Pu , Guanwu Lian , Zhao-Hui Dong , Ke Yang , Zirui Lou , Zhongxin Chen , Baisheng Sa , Longlong Fan , Xiaoxu Zhao and Mingjian Zhang https://doi.org/10.31635/ccschem.025.202506030 SectionsSupplemental MaterialAboutPDF ToolsAdd to favoritesDownload CitationsTrack Citations ShareFacebookTwitterLinked InEmail Direct repairing of spent cathodes represents a next-generation solution for establishing a closed-loop in the battery industry. Given the extreme complexity in compositional off-stoichiometry and structural degradation of spent cathodes, the direct repairing process remains challenging. Here, a transient upcycling strategy assisted by atom-economy utilization of residual binder polyvinylidene fluoride (PVDF) is first proposed to realize a target upgrading of spent LiFePO4 (LFP). Comprehensive multiscale characterizations combined with theoretical calculations reveal that the in-situ thermal decomposition of residual PVDF produces carbonaceous reductants (C and CH4) and fluorinated species (LixPFyOz and metal fluorides). The former assists ultrafast lithiation (~1 s) of degraded FePO4 phase, reconstructing Li-rich LFP with enhanced Li+ diffusion kinetics. Concurrently, the latter constitutes an F-rich cathode/electrolyte interphase layer on particle surface, providing effective bulk structural protection. Therefore, the upcycled LFP exhibits superior rate capability and cycling sustainability, outperforming the fresh commercial counterparts from different manufacturers. Techno-economic and carbon footprint analyses further confirm the significant industrial application potential of this strategy. Download figure Download PowerPoint Previous articleNext article FiguresReferencesRelatedDetails Issue AssignmentNot Yet AssignedSupporting Information Copyright & Permissions© 2025 Chinese Chemical Society Downloaded 100 times PDF downloadLoading ...