Special Issue "Composite Electrolyte & Electrode Membranes for Electrochemical Energy Storage & Conversion Devices"

A special issue of Membranes (ISSN 2077-0375). This special issue belongs to the section "Membrane Applications".

Deadline for manuscript submissions: closed (31 January 2020).

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A printed edition of this Special Issue is available here.

Special Issue Editor

Dr. Giovanni Battista Appetecchi
E-Mail Website
Guest Editor
ENEA (Italian National Agency for New Technologies, Energy and Sustainable Economic Development), Department for Sustainability (SSPT), Division for Sustainable Materials (PROMAS), Materials and Physicochemical Processes Laboratory (MATPRO), Casaccia Research Center, Via Anguillarese 301, 00123 Rome, Italy
Interests: research and development of electrolyte/electrode materials/components for electrochemical energy storage systems; ionic liquids; polymer and gel electrolytes; lithium batteries
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Special Issue Information

Dear Colleagues,

Energy demand is still mainly satisfied by the direct but inefficient and polluting conversion of chemical energy of fossil fuels because of the lack of highly performing energy storage systems. Electrochemical power sources differ from others due to the fact that the energy conversion occurs from chemical into electrical without any intermediate step, resulting in higher energy efficiencies in addition to a much lower environmental impact due to the absence of any gaseous emission. Among the various choices, electrochemical devices, such as batteries, supercapacitors, and fuel cells, are one of the most, if not the most, suitable answers for efficient energy storage and conversion.

Electrode chemistry and formulation play a key role in the performance and safety of electrochemical devices. For instance, electrodes, in addition to electrochemical active species, have to contain passive components (electronic and/or ionic conductor, binder, etc.), which, even if not affecting the energy density, strongly influence the power density, cycling behavior, and reliability of the device. Therefore, although well-known over time, these issues are currently under deep investigation worldwide.

This Special Issue will offer an appealing forum to bring together the latest results obtained by key laboratories presently involved in R and D of composite electrodes for batteries, supercapacitors, and fuel cells. Again, this Special Issue represents an optimal site for welcoming the latest innovations and, accordingly, authors from top laboratories are invited to submit their forthcoming results.

Dr. Giovanni Battista Appetecchi
Guest Editor

Manuscript Submission Information

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Submitted manuscripts should not have been published previously, nor be under consideration for publication elsewhere (except conference proceedings papers). All manuscripts are thoroughly refereed through a single-blind peer-review process. A guide for authors and other relevant information for submission of manuscripts is available on the Instructions for Authors page. Membranes is an international peer-reviewed open access monthly journal published by MDPI.

Please visit the Instructions for Authors page before submitting a manuscript. The Article Processing Charge (APC) for publication in this open access journal is 1800 CHF (Swiss Francs). Submitted papers should be well formatted and use good English. Authors may use MDPI's English editing service prior to publication or during author revisions.

Keywords

  • batteries
  • supercapacitors
  • fuel cells
  • composite electrodes
  • electrode formulation

Published Papers (10 papers)

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Editorial

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Editorial
Composite Electrolyte & Electrode Membranes for Electrochemical Energy Storage & Conversion Devices
Membranes 2020, 10(11), 359; https://doi.org/10.3390/membranes10110359 - 21 Nov 2020
Viewed by 568

Research

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Article
The Use of Succinonitrile as an Electrolyte Additive for Composite-Fiber Membranes in Lithium-Ion Batteries
Membranes 2020, 10(3), 45; https://doi.org/10.3390/membranes10030045 - 17 Mar 2020
Cited by 2 | Viewed by 1198
Abstract
In the present work, the effect of temperature and additives on the ionic conductivity of mixed organic/ionic liquid electrolytes (MOILEs) was investigated by conducting galvanostatic charge/discharge and ionic conductivity experiments. The mixed electrolyte is based on the ionic liquid (IL) (EMI/TFSI/LiTFSI) and organic [...] Read more.
In the present work, the effect of temperature and additives on the ionic conductivity of mixed organic/ionic liquid electrolytes (MOILEs) was investigated by conducting galvanostatic charge/discharge and ionic conductivity experiments. The mixed electrolyte is based on the ionic liquid (IL) (EMI/TFSI/LiTFSI) and organic solvents EC/DMC (1:1 v/v). The effect of electrolyte type on the electrochemical performance of a LiCoO2 cathode and a SnO2/C composite anode in lithium anode (or cathode) half-cells was also investigated. The results demonstrated that the addition of 5 wt.% succinonitrile (SN) resulted in enhanced ionic conductivity of a 60% EMI-TFSI 40% EC/DMC MOILE from ~14 mS·cm−1 to ~26 mS·cm−1 at room temperature. Additionally, at a temperature of 100 °C, an increase in ionic conductivity from ~38 to ~69 mS·cm−1 was observed for the MOILE with 5 wt% SN. The improvement in the ionic conductivity is attributed to the high polarity of SN and its ability to dissolve various types of salts such as LiTFSI. The galvanostatic charge/discharge results showed that the LiCoO2 cathode with the MOILE (without SN) exhibited a 39% specific capacity loss at the 50th cycle while the LiCoO2 cathode in the MOILE with 5 wt.% SN showed a decrease in specific capacity of only 14%. The addition of 5 wt.% SN to the MOILE with a SnO2/C composite-fiber anode resulted in improved cycling performance and rate capability of the SnO2/C composite-membrane anode in lithium anode half-cells. Based on the results reported in this work, a new avenue and promising outcome for the future use of MOILEs with SN in lithium-ion batteries (LIBs) can be opened. Full article
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Article
Composite Nafion Membranes with CaTiO3−δ Additive for Possible Applications in Electrochemical Devices
Membranes 2019, 9(11), 143; https://doi.org/10.3390/membranes9110143 - 31 Oct 2019
Cited by 5 | Viewed by 1044
Abstract
A composite membrane based on a Nafion polymer matrix incorporating a non-stoichiometric calcium titanium oxide (CaTiO3−δ) additive was synthesized and characterized by means of thermal analysis, dynamic mechanical analysis, and broadband dielectric spectroscopy at different filler contents; namely two concentrations of [...] Read more.
A composite membrane based on a Nafion polymer matrix incorporating a non-stoichiometric calcium titanium oxide (CaTiO3−δ) additive was synthesized and characterized by means of thermal analysis, dynamic mechanical analysis, and broadband dielectric spectroscopy at different filler contents; namely two concentrations of 5 and 10 wt.% of the CaTiO3−δ additive, with respect to the dry Nafion content, were considered. The membrane with the lower amount of additive displayed the highest water affinity and the highest conductivity, indicating that a too-high dose of additive can be detrimental for these particular properties. The mechanical properties of the composite membranes are similar to those of the plain Nafion membrane and are even slightly improved by the filler addition. These findings indicate that perovskite oxides can be useful as a water-retention and reinforcing additive in low-humidity proton-exchange membranes. Full article
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Article
LFP-Based Gravure Printed Cathodes for Lithium-Ion Printed Batteries
Membranes 2019, 9(6), 71; https://doi.org/10.3390/membranes9060071 - 07 Jun 2019
Cited by 3 | Viewed by 1176
Abstract
Printed batteries have undergone increased investigation in recent years because of the growing daily use of small electronic devices. With this in mind, industrial gravure printing has emerged as a suitable production technology due to its high speed and quality, and its capability [...] Read more.
Printed batteries have undergone increased investigation in recent years because of the growing daily use of small electronic devices. With this in mind, industrial gravure printing has emerged as a suitable production technology due to its high speed and quality, and its capability to produce any shape of image. The technique is one of the most appealing for the production of functional layers for many different purposes, but it has not been highly investigated. In this study, we propose a LiFePO4 (LFP)-based gravure printed cathode for lithium-ion rechargeable printed batteries and investigate the possibility of employing this printing technique in battery manufacture. Full article
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Article
Gel Polymer Electrolytes Based on Silica-Added Poly(ethylene oxide) Electrospun Membranes for Lithium Batteries
Membranes 2018, 8(4), 126; https://doi.org/10.3390/membranes8040126 - 05 Dec 2018
Cited by 3 | Viewed by 1390
Abstract
Solid polymer electrolytes, in the form of membranes, offering high chemical and mechanical stability, while maintaining good ionic conductivity, are envisaged as a possible solution to improve performances and safety in different lithium cell configurations. In this work, we designed and prepared systems [...] Read more.
Solid polymer electrolytes, in the form of membranes, offering high chemical and mechanical stability, while maintaining good ionic conductivity, are envisaged as a possible solution to improve performances and safety in different lithium cell configurations. In this work, we designed and prepared systems formed using innovative nanocomposite polymer membranes, based on high molecular weight poly(ethylene oxide) (PEO) and silica nanopowders, produced by the electrospinning technique. These membranes were subsequently gelled with solutions based on aprotic ionic liquid, carbonate solvents, and lithium salt. The addition of polysulfide species to the electrolyte solution was also considered, in view of potential applications in lithium-sulfur cells. The morphology of the electrospun pristine membranes was evaluated using scanning electron microscopy. Stability and thermal properties of pristine and gelled systems were investigated uisng differential scanning calorimetry and thermal gravimetric analysis. Electrochemical impedance spectroscopy was used to determine the conductivity of both swelling solutions and gelled membranes, allowing insight into the ion transport mechanism within the proposed composite electrolytes. Full article
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Article
Composite Gel Polymer Electrolytes Based on Organo-Modified Nanoclays: Investigation on Lithium-Ion Transport and Mechanical Properties
Membranes 2018, 8(3), 69; https://doi.org/10.3390/membranes8030069 - 24 Aug 2018
Cited by 19 | Viewed by 1810
Abstract
Composite gel polymer electrolytes (GPEs) based on organo-modified montmorillonite clays have been prepared and investigated. The organo-clay was prepared by intercalation of CTAB molecules in the interlamellar space of sodium smectite clay (SWy) through a cation-exchange reaction. This was used as nanoadditive in [...] Read more.
Composite gel polymer electrolytes (GPEs) based on organo-modified montmorillonite clays have been prepared and investigated. The organo-clay was prepared by intercalation of CTAB molecules in the interlamellar space of sodium smectite clay (SWy) through a cation-exchange reaction. This was used as nanoadditive in polyacrylonitrile/polyethylene-oxide blend polymer, lithium trifluoromethanesulphonate (LiTr) as salt and a mixture of ethylene carbonate/propylene carbonate as plasticizer. GPEs were widely characterized by DSC, SEM, and DMA, while the ion transport properties were investigated by AC impedance spectroscopy and multinuclear NMR spectroscopy. In particular, 7Li and 19F self-diffusion coefficients were measured by the pulse field gradient (PFG) method, and the spin-lattice relaxation times (T1) by the inversion recovery sequence. A complete description of the ions dynamics in so complex systems was achieved, as well as the ion transport number and ionicity index were estimated, proving that the smectite clay surfaces are able to “solvatate” both lithium and triflate ions and to create a preferential pathway for ion conduction. Full article
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Article
High Performance Polymer/Ionic Liquid Thermoplastic Solid Electrolyte Prepared by Solvent Free Processing for Solid State Lithium Metal Batteries
Membranes 2018, 8(3), 55; https://doi.org/10.3390/membranes8030055 - 02 Aug 2018
Cited by 13 | Viewed by 2398
Abstract
A polymer/ionic liquid thermoplastic solid electrolyte based on poly(ethylene oxide) (PEO), modified sepiolite (TPGS-S), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and 1-Butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR14TFSI) ionic liquid is prepared using solvent free extrusion method. Its physical-chemical, electrical, and electrochemical properties are comprehensively studied. The investigated [...] Read more.
A polymer/ionic liquid thermoplastic solid electrolyte based on poly(ethylene oxide) (PEO), modified sepiolite (TPGS-S), lithium bis(trifluoromethanesulfonyl)imide (LiTFSI), and 1-Butyl-1-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide (PYR14TFSI) ionic liquid is prepared using solvent free extrusion method. Its physical-chemical, electrical, and electrochemical properties are comprehensively studied. The investigated solid electrolyte demonstrates high ionic conductivity together with excellent compatibility with lithium metal electrode. Finally, truly Li-LiFePO4 solid state coin cell with the developed thermoplastic solid electrolyte demonstrates promising electrochemical performance during cycling under 0.2 C/0.5 C protocol at 60 °C. Full article
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Article
Ionic Liquid-Based Electrolyte Membranes for Medium-High Temperature Lithium Polymer Batteries
Membranes 2018, 8(3), 41; https://doi.org/10.3390/membranes8030041 - 10 Jul 2018
Cited by 14 | Viewed by 2019
Abstract
Li+-conducting polyethylene oxide-based membranes incorporating N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide are used as electrolyte separators for all-solid-state lithium polymer batteries operating at medium-high temperatures. The incorporation of the ionic liquid remarkably improves the thermal, ion-transport and interfacial properties of the polymer [...] Read more.
Li+-conducting polyethylene oxide-based membranes incorporating N-butyl-N-methylpyrrolidinium bis(trifluoromethanesulfonyl)imide are used as electrolyte separators for all-solid-state lithium polymer batteries operating at medium-high temperatures. The incorporation of the ionic liquid remarkably improves the thermal, ion-transport and interfacial properties of the polymer electrolyte, which, in combination with the wide electrochemical stability even at medium-high temperatures, allows high current rates without any appreciable lithium anode degradation. Battery tests carried out at 80 °C have shown excellent cycling performance and capacity retention, even at high rates, which are never tackled by ionic liquid-free polymer electrolytes. No dendrite growth onto the lithium metal anode was observed. Full article
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Review

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Review
Review of Recent Nuclear Magnetic Resonance Studies of Ion Transport in Polymer Electrolytes
Membranes 2018, 8(4), 120; https://doi.org/10.3390/membranes8040120 - 30 Nov 2018
Cited by 12 | Viewed by 2012
Abstract
Current and future demands for increasing the energy density of batteries without sacrificing safety has led to intensive worldwide research on all solid state Li-based batteries. Given the physical limitations on inorganic ceramic or glassy solid electrolytes, development of polymer electrolytes continues to [...] Read more.
Current and future demands for increasing the energy density of batteries without sacrificing safety has led to intensive worldwide research on all solid state Li-based batteries. Given the physical limitations on inorganic ceramic or glassy solid electrolytes, development of polymer electrolytes continues to be a high priority. This brief review covers several recent alternative approaches to polymer electrolytes based solely on poly(ethylene oxide) (PEO) and the use of nuclear magnetic resonance (NMR) to elucidate structure and ion transport properties in these materials. Full article
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Review
Recent Advances in Poly(vinylidene fluoride) and Its Copolymers for Lithium-Ion Battery Separators
Membranes 2018, 8(3), 45; https://doi.org/10.3390/membranes8030045 - 19 Jul 2018
Cited by 57 | Viewed by 3403
Abstract
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 [...] Read more.
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. Full article
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