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Polymers
Special Issues
Innovative Polymer Electrolytes
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Innovative Polymer Electrolytes

A special issue of Polymers (ISSN 2073-4360). This special issue belongs to the section "Polymer Applications".

Deadline for manuscript submissions: closed (30 July 2020) | Viewed by 27822

Special Issue Editors

Prof. Dr. David Mecerreyes

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Guest Editor
POLYMAT, Joxe Mari Korta Center, University of the Basque Country UPV/EHU, Avda. Tolosa 72, 20018 Donostia-San Sebastian, Spain
Interests: Innovative polymer chemistry; polymeric ionic liquids; redox polymers; polymers for energy (batteries)
Special Issues, Collections and Topics in MDPI journals
Dr. Luca Porcarelli

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Guest Editor
1. POLYMAT, Joxe Mari Korta Center, University of the Basque Country UPV/EHU, Avda. Tolosa 72, 20018 Donostia-San Sebastian, Spain
2. Institute for Frontier Materials, Deakin University, 221 Burwood Hwy, Burwood, 3125 Victoria, Australia
Interests: Innovative polymer chemistry; polymer solid electrolytes; single-ion conductors; energy storage and conversion
Dr. Xiaoen Wang

E-Mail Website
Guest Editor
Institute for Frontier Materials, Deakin University, 221 Burwood Hwy, Burwood, 3125 Victoria, Australia
Interests: polymer electrolytes; nanocomposites; Li-/Na-ion batteries; proton exchange membranes and fuel cells

Special Issue Information

Dear Colleagues,

Polymer electrolytes are an innovative class of materials combining ion-transport properties analogous to conventional salt solutions with the unique mechanical properties of polymers. Polymer electrolytes play an important role in a large number of solid-state electrochemical devices in energy and medicine. The non-exhaustive list of devices includes (bio)sensors, actuators, ion pumps, electrochromics, light-emitting electrochemical cells, solar cells, and batteries. Due to growing interest in this field, this Special Issue aims to publish high-quality original research papers on the synthesis and application of innovative polymer electrolytes.

Prof. Dr. David Mecerreyes
Dr. Luca Porcarelli
Dr. Xiaoen Wang
Guest Editors

Manuscript Submission Information

Manuscripts should be submitted online at www.mdpi.com by registering and logging in to this website. Once you are registered, click here to go to the submission form. Manuscripts can be submitted until the deadline. All submissions that pass pre-check are peer-reviewed. Accepted papers will be published continuously in the journal (as soon as accepted) and will be listed together on the special issue website. Research articles, review articles as well as short communications are invited. For planned papers, a title and short abstract (about 100 words) can be sent to the Editorial Office for announcement on this website.

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. Polymers is an international peer-reviewed open access semimonthly 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 2700 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

  • Polymer electrolytes
  • solid-state
  • electrochemical devices
  • sensors
  • actuators
  • ion pumps
  • electrochromic
  • light-emitting electrochemical cells
  • solar cells
  • batteries
  • synthesis

Published Papers (6 papers)

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Research

18 pages, 3355 KiB  
Article
Mixed Ionic-Electronic Conductors Based on PEDOT:PolyDADMA and Organic Ionic Plastic Crystals
by Rafael Del Olmo, Nerea Casado, Jorge L. Olmedo-Martínez, Xiaoen Wang and Maria Forsyth
Polymers 2020, 12(9), 1981; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12091981 - 31 Aug 2020
Cited by 14 | Viewed by 5264
Abstract
Mixed ionic-electronic conductors, such as poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) are postulated to be the next generation materials in energy storage and electronic devices. Although many studies have aimed to enhance the electronic conductivity and mechanical properties of these materials, there has been little focus [...] Read more.
Mixed ionic-electronic conductors, such as poly(3,4-ethylenedioxythiophene): poly(styrenesulfonate) (PEDOT:PSS) are postulated to be the next generation materials in energy storage and electronic devices. Although many studies have aimed to enhance the electronic conductivity and mechanical properties of these materials, there has been little focus on ionic conductivity. In this work, blends based on PEDOT stabilized by the polyelectrolyte poly(diallyldimethylammonium) (PolyDADMA X) are reported, where the X anion is either chloride (Cl), bis(fluorosulfonyl)imide (FSI), bis(trifluoromethylsulfonyl)imide (TFSI), triflate (CF3SO3) or tosylate (Tos). Electronic conductivity values of 0.6 S cm−1 were achieved in films of PEDOT:PolyDADMA FSI (without any post-treatment), with an ionic conductivity of 5 × 10−6 S cm−1 at 70 °C. Organic ionic plastic crystals (OIPCs) based on the cation N-ethyl-N-methylpyrrolidinium (C2mpyr+) with similar anions were added to synergistically enhance both electronic and ionic conductivities. PEDOT:PolyDADMA X / [C2mpyr][X] composites (80/20 wt%) resulted in higher ionic conductivity values (e.g., 2 × 10−5 S cm−1 at 70 °C for PEDOT:PolyDADMA FSI/[C2mpyr][FSI]) and improved electrochemical performance versus the neat PEDOT:PolyDADMA X with no OIPC. Herein, new materials are presented and discussed including new PEDOT:PolyDADMA and organic ionic plastic crystal blends highlighting their promising properties for energy storage applications. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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12 pages, 3450 KiB  
Article
Solid Polymer Electrolytes with Flexible Framework of SiO2 Nanofibers for Highly Safe Solid Lithium Batteries
by Jin Cui, Zehao Zhou, Mengyang Jia, Xin Chen, Chuan Shi, Ning Zhao and Xiangxin Guo
Polymers 2020, 12(6), 1324; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12061324 - 10 Jun 2020
Cited by 55 | Viewed by 4556
Abstract
Composite electrolytes consisting of polymers and three-dimensional (3D) fillers are considered to be promising electrolytes for solid lithium batteries owing to their virtues of continuous lithium-ion pathways and good mechanical properties. In the present study, an electrolyte with polyethylene oxide–lithium (bis trifluoromethyl) sulfate–succinonitrile [...] Read more.
Composite electrolytes consisting of polymers and three-dimensional (3D) fillers are considered to be promising electrolytes for solid lithium batteries owing to their virtues of continuous lithium-ion pathways and good mechanical properties. In the present study, an electrolyte with polyethylene oxide–lithium (bis trifluoromethyl) sulfate–succinonitrile (PLS) and frameworks of three-dimensional SiO2 nanofibers (3D SiO2 NFs) was prepared. Taking advantage of the highly conductive interfaces between 3D SiO2 NFs and PLS, the total conductivity of the electrolyte at 30 °C was approximately 9.32 × 10−5 S cm−1. With a thickness of 27 μm and a tensile strength of 7.4 MPa, the electrolyte achieved an area specific resistance of 29.0 Ω cm2. Moreover, such a 3D configuration could homogenize the electrical field, which was beneficial for suppressing dendrite growth. Consequently, Li/LiFePO4 cells assembled with PLS and 3D SiO2 NFs (PLS/3D SiO2 NFs), which delivered an original specific capacity of 167.9 mAh g−1, only suffered 3.28% capacity degradation after 100 cycles. In particular, these cells automatically shut down when PLS was decomposed above 400 °C, and the electrodes were separated by the solid framework of 3D SiO2 NFs. Therefore, the solid lithium batteries based on composite electrolytes reported here offer high safety at elevated temperatures. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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18 pages, 4701 KiB  
Article
Designing Imidazolium Poly(amide-amide) and Poly(amide-imide) Ionenes and Their Interactions with Mono- and Tris(imidazolium) Ionic Liquids
by Kathryn E. O’Harra, Danielle M. Noll, Irshad Kammakakam, Emily M. DeVriese, Gala Solis, Enrique M. Jackson and Jason E. Bara
Polymers 2020, 12(6), 1254; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12061254 - 30 May 2020
Cited by 7 | Viewed by 3705
Abstract
Here we introduce the synthesis and thermal properties of a series of sophisticated imidazolium ionenes with alternating amide-amide or amide-imide backbone functionality, and investigate the structural effects of mono(imidazolium) and unprecedented tris(imidazolium) ionic liquids (ILs) in these ionenes. The new set of poly(amide-amide) [...] Read more.
Here we introduce the synthesis and thermal properties of a series of sophisticated imidazolium ionenes with alternating amide-amide or amide-imide backbone functionality, and investigate the structural effects of mono(imidazolium) and unprecedented tris(imidazolium) ionic liquids (ILs) in these ionenes. The new set of poly(amide-amide) (PAA) and poly(amide-imide) (PAI) ionenes represent the intersection of conventional high-performance polymers with the ionene archetype–presenting polymers with alternating functional and ionic elements precisely sequenced along the backbone. The effects of polymer composition on the thermal properties and morphology were analyzed. Five distinct polymer backbones were synthesized and combined with a stoichiometric equivalent of the IL 1-benzyl-3-methylimidazolium bistriflimide ([Bnmim][Tf2N]), which were studied to probe the self-assembly, structuring, and contributions of intermolecular forces when IL is added. Furthermore, three polyamide (PA) or polyimide (PI) ionenes with simpler xylyl linkages were interfaced with [Bnmim][Tf2N] as well as a novel amide-linked tris(imidazolium) IL, to demonstrate the structural changes imparted by the inclusion of functional, ionic additives dispersed within the ionene matrix. This work highlights the possibilities for utilizing concepts from small molecules which exhibit supramolecular self-assembly to guide creative design and manipulate the structuring of ionenes. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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14 pages, 2126 KiB  
Article
Poly (Ethylene Oxide)-Based Block Copolymer Electrolytes Formed via Ligand-Free Iron-Mediated Atom Transfer Radical Polymerization
by Sibo Li, Mengying Tian, Jirong Wang, Feipeng Du, Liang Li and Zhigang Xue
Polymers 2020, 12(4), 763; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12040763 - 01 Apr 2020
Cited by 3 | Viewed by 3894
Abstract
The Br-terminated poly (ethylene oxide) (PEO-Br) is used as a green and efficient macroinitiator in bulk Fe-catalyzed atom transfer radical polymerization (ATRP) without the addition of any organic ligands. The polymerization rate is able to be mediated by PEO-Br with various molecular weights, [...] Read more.
The Br-terminated poly (ethylene oxide) (PEO-Br) is used as a green and efficient macroinitiator in bulk Fe-catalyzed atom transfer radical polymerization (ATRP) without the addition of any organic ligands. The polymerization rate is able to be mediated by PEO-Br with various molecular weights, and the decrease in redox potential of FeBr2 in cyclic voltammetry (CV) curves indicates that an increased coordination effect is deteriorated with the depressing reaction activity in the longer ethylene oxide (EO) chain in PEO-Br. In combination with the study of different catalysts and catalytic contents, the methyl metharylate (MMA) or poly (ethylene glycol) monomethacrylate (PEGMA) was successfully polymerized with PEO-Br as an initiator. This copolymer obtained from PEGMA polymerization can be further employed as a polymer matrix to form the polymer electrolyte (PE). The higher ionic conductivity of PE was obtained by using a high molecular weight of copolymer. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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16 pages, 4178 KiB  
Article
Tuning the Properties of a UV-Polymerized, Cross-Linked Solid Polymer Electrolyte for Lithium Batteries
by Preston Sutton, Martino Airoldi, Luca Porcarelli, Jorge L. Olmedo-Martínez, Clément Mugemana, Nico Bruns, David Mecerreyes, Ullrich Steiner and Ilja Gunkel
Polymers 2020, 12(3), 595; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12030595 - 05 Mar 2020
Cited by 20 | Viewed by 5606
Abstract
Lithium metal anodes have been pursued for decades as a way to significantly increase the energy density of lithium-ion batteries. However, safety risks caused by flammable liquid electrolytes and short circuits due to lithium dendrite formation during cell cycling have so far prevented [...] Read more.
Lithium metal anodes have been pursued for decades as a way to significantly increase the energy density of lithium-ion batteries. However, safety risks caused by flammable liquid electrolytes and short circuits due to lithium dendrite formation during cell cycling have so far prevented the use of lithium metal in commercial batteries. Solid polymer electrolytes (SPEs) offer a potential solution if their mechanical properties and ionic conductivity can be simultaneously engineered. Here, we introduce a family of SPEs that are scalable and easy to prepare with a photopolymerization process, synthesized from amphiphilic acrylic polymer conetworks based on poly(ethylene glycol), 2-hydroxy-ethylacrylate, norbornyl acrylate, and either lithium bis (trifluoromethanesulfonyl) imide (LiTFSI) or a single-ion polymethacrylate as lithium-ion source. Several conetworks were synthesized and cycled, and their ionic conductivity, mechanical properties, and lithium transference number were characterized. A single-ion-conducting polymer electrolyte shows the best compromise between the different properties and extends the calendar life of the cell. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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13 pages, 3443 KiB  
Article
Improving the Electrochemical Performance and Stability of Polypyrrole by Polymerizing Ionic Liquids
by Arko Kesküla, Ivo Heinmaa, Tarmo Tamm, Nihan Aydemir, Jadranka Travas-Sejdic, Anna-Liisa Peikolainen and Rudolf Kiefer
Polymers 2020, 12(1), 136; https://0-doi-org.brum.beds.ac.uk/10.3390/polym12010136 - 06 Jan 2020
Cited by 9 | Viewed by 3693
Abstract
Polypyrrole (PPy) based electroactive materials are important building blocks for the development of flexible electronics, bio-sensors and actuator devices. As the properties and behavior of PPy depends strongly on the operating environment—electrolyte, solvent, etc., it is desirable to plant immobile ionic species into [...] Read more.
Polypyrrole (PPy) based electroactive materials are important building blocks for the development of flexible electronics, bio-sensors and actuator devices. As the properties and behavior of PPy depends strongly on the operating environment—electrolyte, solvent, etc., it is desirable to plant immobile ionic species into PPy films to ensure stable response. A premade ionic polymer is not optimal in many cases, as it enforces its own structure on the conducting polymer, therefore, polymerization during fabrication is preferred. Pyrrole (Py) was electropolymerized at low temperature together with a polymerizable ionic liquid (PIL) monomer in a one-step polymerization, to form a stable film on the working electrode. The structure and morphology of the PPyPIL films were investigated by scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), Fourier-transform infrared (FTIR) spectroscopy and solid-state NMR (ssNMR) spectroscopy. The spectroscopy results confirmed the successful polymerization of Py to PPy and PIL monomer to PIL. The presence of (TFSI–) anions that balance the charge in PPyPIL was confirmed by EDX analysis. The electrical properties of PPyPIL in lithium bis(trifluoromethanesulfonyl)-imide (LiTFSI) aqueous and propylene carbonate solutions were examined with cyclic voltammetry (CV), chronoamperometry, and chronopotentiometry. The blend of PPyPIL had mixed electronic/ionic conductive properties that were strongly influenced by the solvent. In aqueous electrolyte, the electrical conductivity was 30 times lower and the diffusion coefficient 1.5 times higher than in the organic electrolyte. Importantly, the capacity, current density, and charge density were found to stay consistent, independent of the choice of solvent. Full article
(This article belongs to the Special Issue Innovative Polymer Electrolytes)
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