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The separator membrane is an essential component of lithium-ion batteries, separating the anode and cathode, and controlling the number and mobility of the lithium ions. Among the polymer matrices most commonly investigated for battery separators are poly(vinylidene fluoride) (PVDF) and its copolymers poly(vinylidene fluoride-co-trifluoroethylene) (PVDF-TrFE), poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP), and poly(vinylidene fluoride-cochlorotrifluoroethylene) (PVDF-CTFE), due to their excellent properties such as high polarity and the possibility of controlling the porosity of the materials through binary and ternary polymer/solvent systems, among others. This review presents the recent advances on battery separators based on PVDF and its copolymers for lithium-ion batteries. It is divided into the following sections: single polymer and co-polymers, surface modification, composites, and polymer blends. Further, a critical comparison between those membranes and other separator membranes is presented, as well as the future trends on this area. ; Portuguese Foundation for Science and Technology (FCT): UID/FIS/04650/2013, PTDC/CTM-ENE/5387/2014, UID/CTM/50025/2013, project NO. 28157/02/SAICT/2017 and grants SFRH/BPD/112547/2015 (C.M.C.), including FEDER funds through the COMPETE 2020 programme and National Funds through FCT. Financial support from the Basque Government Industry Department under the ELKARTEK and HAZITEK programs is also acknowledged. ...

Low voltage actuators based on poly(vinylidene fluoride)(PVDF)with 10, 25 and 40 % 1-hexyl-3-methylimidazolium chloride ([C6mim][Cl])and 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([C6mim][NTf2]) are prepared by solvent casting in order to evaluate the effect of anion size in the bending properties. Independently of the ionic liquid type and content, its presence leads to the crystallization of PVDF in the -phase. The addition of ionic liquid into the polymer matrix decreases significantly its degree of crystallinity and the elastic modulus. It is also confirmed the good miscibility between PVDF and IL,determinedby the interaction of the CF2groups from the PVDF chains with the imidazolium ring in the ionic liquid (IL). The AC conductivity of the composites depends both on the amount of ionic liquid content and anion size. The bending movement of the IL/PVDF composites is correlated to theirdegree of crystallinity, mechanical properties and ionic conductivity value and the best value of bending response (0.53 %) being found for IL/PVDF composite with40 wt% of [C6mim][Cl] at an applied voltage of 10 volts square signal. ; The authors thank the FCT-Fundação para a Ciência e Tecnologia-for financial support in the framework of the Strategic Funding UID/FIS/04650/2013, projects PTDC/EEI-SII/5582/2014 and PTDC/CTM-ENE/5387/2014,and grants SFRH/BD/90215/2012 (J.C.D.), SFRH/BPD/112547/2015 (C.M.C.). The authors thank Solvay for kindly supplying the high quality materials. Financial support from the Basque Government Industry Department under the ELKARTEK Program is also acknowledged.The authorsexpress their gratitude to the Ministry of the Higher Education and Scientific Research of Tunisiafor a research ...

Actuators based on polymer blends of poly(vinylidene fluoride) (PVDF) with 40 % of different ionic liquids (IL) are prepared by solvent casting. [C2mim][Cl], [C6mim][Cl], [C10mim][Cl], [C2mim][NTf2], [C6mim][NTf2] and [C10mim][NTf2] were selected in order to evaluate the effect of anion and cation sizes in the bending properties. The microstructure, mechanical and electrical properties of the blend depend on the IL type, which in turn leads to a different bending response. In particular, the mechanical properties are independent on the IL type but the AC conductivity of the composites depend more on the anion type than on the size of the alkyl chain connected to the imidazolium based cation. Thus, the bending response of the IL/PVDF composites is correlated with the anion and cation sizes and a maximum bending response of 0.3 % is achieved for a 10 volts square signal in the IL/PVDF composite with 40 wt% content of [C2mim][NTf2]. ; The authors thank FEDER funds through the COMPETE 2020 Programme and National Funds through FCT - Portuguese Foundation for Science and Technology under Strategic Funding UID/FIS/04650/2013, UID/Multi/04551/2013, UID/QUI/50006/2013, project PTDC/EEI-SII/5582/2014, a contract under Investigador FCT 2012 program (J.M.S.S.E.), and grants SFRH/BD/90215/2012 (JCD) and SFRH/BPD/112547/2015 (CMC). Financial support from the Basque Government Industry Department under the ELKARTEK Program is also acknowledged. The authors (R. M. and S. B. H.) would like to thank the Tunisian Ministry of Higher Education and Research for its financial support. The authors thank the support of M. S. Martins (U. Minho) for supporting the electromechanical ...

[EN] The increasing use of electronic portable systems and the consequent energy demand, leads to the need to improve energy storage systems. According to that and due to safety issues, high-performance non-flammable electrolytes and solid polymer electrolytes (SPE) are needed. SPE containing different amounts of lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) into a poly(vinylidene fluoride-co-hexafluoropropylene), PVDF-HFP, polymer matrix have been prepared by solvent casting. The addition of LiTFSI into PVDF-HFP allows to tailor thermal, mechanical and electrical properties of the composite. In particular, the ionic conductivity of the composites increases with LiTFSI content, the best ionic conductivities of 0.0011 mS/cmat 25 degrees C and 0.23 mS/cmat 90 degrees C were obtained for the PVDF-HFP/LiTFSI composites with 80 wt % of LiTFSI. This solid electrolyte allows the fabrication of Li metallic/SPE/C-LiFePO4 half-cells with a discharge capacity of 51.2 mAh/ g at C/20. Further, theoretical simulations show that the discharge capacity value depends on the lithium concentration and percentage of free ions and is independent of the solid polymer electrolyte thickness. On the other hand, the voltage plateau depends on the SPE thickness. Thus, a solid electrolyte is presented for the next generation of safer solid-state batteries. ; The authors thank the FCT (Fundacao para a Ciencia e Tecnologia) for financial support under the framework of Strategic Funding grants UID/FIS/04650/2013, UID/EEA/04436/2013 and UID/QUI/0686/2016; and project no. PTDC/FIS-MAC/28157/2017. The authors also thank the FCT for financial support under grant SFRH/BPD/112547/2015 (C.M.C.). Financial support from the Basque Government Industry Department under the ELKARTEK and HAZITEK programs is also acknowledged. JMMD and JLGR acknowledge funding by the Spanish Ministry of Economy and Competitiveness (MINECO) through the project MAT2016-76039-C4-1 and 3-R (including the FEDER financial support) CIBER-BBN is an initiative funded by the ...

The increasing use of electronic portable systems and the consequent energy demand, leads to the need to improve energy storage systems. According to that and due to safety issues, high-performance non-flammable electrolytes and solid polymer electrolytes (SPE) are needed.SPE containing different amounts of lithium bis(trifluoromethanesulfonyl) imide (LiTFSI) into a poly(vinylidene fluoride-co-hexafluoropropylene), PVDF-HFP, polymer matrix have been prepared by solvent casting. The addition of LiTFSI into PVDF-HFP allows to tailor thermal, mechanical and electrical properties of the composite.In particular, the ionic conductivity of the composites increases with LiTFSI content, the best ionic conductivities of 0.0011 mS/cmat 25 degrees C and 0.23 mS/cmat 90 degrees C were obtained for the PVDF-HFP/LiTFSI composites with 80 wt % of LiTFSI.This solid electrolyte allows the fabrication of Li metallic/SPE/C-LiFePO4 half-cells with a discharge capacity of 51.2 mAh/ g at C/20. Further, theoretical simulations show that the discharge capacity value depends on the lithium concentration and percentage of free ions and is independent of the solid polymer electrolyte thickness. On the other hand, the voltage plateau depends on the SPE thickness. Thus, a solid electrolyte is presented for the next generation of safer solid-state batteries. ; The authors thank the FCT (Fundação para a Ciência e Tecnologia) for financial support under the framework of Strategic Funding grants UID/FIS/04650/2013, UID/EEA/04436/2013 and UID/QUI/0686/2016; and project no. PTDC/FIS-MAC/28157/2017. The authors also thank the FCT for financial support under grant SFRH/BPD/112547/2015 (C.M.C.). Financial support from the Basque Government Industry Department under the ELKARTEK and HAZITEK programs is also acknowledged. JMMD and JLGR acknowledge funding by the Spanish Ministry of Economy and Competitiveness (MINECO) through the project MAT2016-76039-C4-1 and 3-R (including the FEDER financial support) CIBER-BBN is an initiative funded by the VI ...

Polyimide co-polymers have been prepared based on different diamines as co-monomers: a diamine without CN groups and a novel synthesized diamine with two CN groups prepared by polycondensation reaction followed by thermal cyclodehydration. Dielectric spectroscopy measurements were performed and the dielectric complex function, ac conductivity and electric modulus of the co-polymers were investigated as a function of CN group content in the frequency range from 0.1 Hz to 107 Hz at temperatures from 25 to 260 °C. For all samples and temperatures above 150ºC, the dielectric constant increases with increasing temperature due to increaseing conductivity. The α-relaxation is just detected for the sample without CN groups, being this relaxation overlapped by the electrical conductivity contributions in the remaining samples. For the copolymer samples and the polymer with CN groups an important Maxwell-Wagner-Sillars contribution is detected. The mechanisms responsible for the dielectric relaxation, conduction process and electric modulus response have been discussed as a function of the CN groups content present in the samples. ; This work was supported by FEDER through the COMPETE Program and by the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Project PESTC/FIS/UI607/2011 and grants SFRH/BD/ 62507/2009 (A.C.L.) SFRH/BD/68499/2010 (C.M.C.). The authors also thank funding from "Matepro – Optimizing Materials and Processes", ref. NORTE-07-0124-FEDER-000037", co-funded by the "Programa Operacional Regional do Norte" (ON.2 – O Novo Norte), under the "Quadro de Referência Estratégico Nacional" (QREN), through the "Fundo Europeu de Desenvolvimento Regional" (FEDER). RSS acknowledge the support of the Spanish Ministry of Economy and Competitiveness through the project MAT2012-38359-C03-01 (including the FEDER financial support). Authors also thank the Basque Country Government for financial support (ACTIMAT project, ETORTEK Program, IE13-380, and Ayudas para Grupos de Investigación ...

Polyimide copolymers have been prepared based on different diamines as comonomers: a diamine without CN groups and a novel synthesized diamine with two CN groups prepared by polycondensation reaction followed by thermal cyclodehydration. Dielectric spectroscopy measurements were performed, and the dielectric complex function, ac conductivity and electric modulus of the copolymers were investigated as a function of CN group content in the frequency range from 0.1 to 107 Hz at temperatures from 25 to 260 °C. For all samples and temperatures above 150 °C, the dielectric constant increases with increasing temperature due to increasing conductivity. The α-relaxation is just detected for the sample without CN groups, being this relaxation overlapped by the electrical conductivity contributions in the remaining samples. For the copolymer samples and the polymer with CN groups, an important Maxwell–Wagner–Sillars contribution is detected. The mechanisms responsible for the dielectric relaxation, conduction process and electric modulus response have been discussed as a function of the CN group content present in the samples. ; This work was supported by FEDER through the COMPETE Program and by the Portuguese Foundation for Science and Technology (FCT) in the framework of the Strategic Project PESTC/FIS/UI607/2011 and grants SFRH/BD/62507/2009 (A.C.L.) SFRH/BD/68499/2010 (C.M.C.). The authors also thank funding from ''Matepro–Optimizing Materials and Processes,'' ref. NORTE-07-0124-FEDER-000037,'' co-funded by the ''Programa Operacional Regional do Norte'' (ON.2–O Novo Norte), under the ''Quadro de Referencia Estratégico Nacional'' (QREN), through the ''Fundo Europeu de Desenvolvimento Regional'' (FEDER). RSS acknowledges the support of the Spanish Ministry of Economy and Competitiveness through the project MAT2012-38359-C03-01 (includin the FEDER financial support). Authors also thank the Basque Country Government for financial support (ACTIMAT project, ETORTEK Program, IE13-380, and Ayudas para Grupos de Investigación del Sistema Universitario Vasco Program, IT718-13).