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Separator membranes based on poly(vinylidene fluoride), PVDF, poly(vinylidene fluoride-co-trifluoroethylene), PVDF-TrFE, poly(vinylidene fluoride-co-hexafluropropylene), PVDF-HFP and poly(vinylidene fluoride-co-chlorotrifluoroethylene), PVDF-CTFE were prepared by solvent casting method using N,N-dimethylformamide (DMF) as solvent. In all cases, the same polymer/solvent ratio and solvent evaporation temperature were used. For all membranes, porous microstructure is achieved with a degree of porosity larger than 50%. The β-phase content as well as degree of crystallinity were different for each membrane, which were lower for the co-polymer membranes when compared with PVDF. On the other hand, the observed ionic conductivity values, electrolyte uptake, tortuosity and MacMullin number were similar for all membranes. The electrochemical performance of the separator membranes was evaluated in Li/C–LiFePO4 half-cell configuration showing good cyclability and rate capability for all membranes. Among the all separator membranes, PVDF-TrFE demonstrate the best electrochemical performance, with a discharge capacity value of 87 mAh.g-1 after 50 cycles with a capacity retention of 78 % at 2C.Finally, the correlation between the β-phase content in the membranes and the cycling performance was demonstrated (which was significant at high-C rates): larger β-phase contents, leading higher polarity, facilitates faster lithium ion migration within the separator for similar microstructures.This work was supported by the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Funding UID/FIS/04650/2013. The authors thank FEDER funds through the COMPETE 2020 Programme and National Funds through FCT under the projects PTDC/CTM-ENE/5387/2014 and UID/CTM/50025/2013 and grants SFRH/BD/90215/2012 (J.C.D.) and SFRH/BPD/112547/2015 (C.M.C.). The authors acknowledge funding by the Spanish Ministry of Economy and Competitiveness (MINECO) through the project MAT2016-76039-C4-3-R (AEI/FEDER, UE) (including the FEDER financial support) and from the Basque Government Industry Department under the ELKARTEK Program. Authors are grateful to the Government of the Basque Country for financial support (Grupos de Investigación, IT718-13). The authors thank Solvay, Timcal and Phostech for kindly supplying the high quality materials.info:eu-repo/semantics/publishedVersio

On the Relevance of the Polar β-Phase of Poly(vinylidene fluoride) for High Performance Lithium-Ion Battery Separators