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Advances in Polymerized Ionic Liquids and Their Composites
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Advances in Polymerized Ionic Liquids and Their Composites

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

Deadline for manuscript submissions: closed (31 July 2022) | Viewed by 23148

Special Issue Editor

Dr. Ciprian Iacob

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Guest Editor
1. Institute of Chemical Technology and Polymer Chemistry, Karlsruhe Institute of Technology (KIT), 76131 Karlsruhe, Germany
2. National Research and Development Institute for Cryogenic and Isotopic Technologies, ICSI, Rm. Valcea 240050, Romania
Interests: dielectric polymers; ionic liquids; polymerized ionic liquids; polymer dynamics; dynamics under nano-confinement; dielectric spectroscopy; batteries; rheology of polymers; charge transport; ionic conductivity

Special Issue Information

Dear Colleagues,

Polymerized ionic liquids (PILs) and their composites, as an innovative class of polyelectrolytes, are important and versatile materials that can be tailored to overcome the current challenges in the fields of polymer and material science. These materials combine the attractive mechanical characteristics of polymers with the unique physicochemical properties of low molecular weight ionic liquids (ILs). These properties make PILs and their composites (PILs with metal salts/ metal nanostructures, carbons, silicas, organic compounds, ILs, metal–organic frameworks) appealing candidates for various applications, such as electrochemical energy storage technologies (Li, metal–air, and organic redox flow batteries, fuel cells, supercapacitors, dye-sensitized solar cells), stimuli-responsive materials, carbon materials, and antimicrobial materials, in catalysis, in sensors, in absorption, and in CO2 separation materials. This Special Issue, “Advances in Polymerized Ionic Liquids and Their Composites”, aims to discuss all aspects regarding experimental and theoretical work on the synthesis, design, characterization, and applications of PILs and their composites. We welcome original full articles, short communications, or review articles on fundamental and applied science of PILs and their composites that tackle problems and challenges in energy, the environment, and life science, in order to contribute to the establishment of detailed correlation between material structure–property–performance relationships, processing, and utilization towards application development.

Dr. Ciprian Iacob
Guest Editor

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

  • polymerized ionic liquids
  • batteries
  • fuel cells
  • supercapacitors
  • dye-sensitized solar cells
  • polyelectrolytes membranes
  • composites
  • charge transport
  • catalysis
  • sensors
  • energy
  • electrical energy storage devices
  • ionic conductivity
  • stimuli-responsive materials
  • CO2 separation materials
  • ionogels
  • gas separation
  • electrochemical window

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Published Papers (6 papers)

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Research

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12 pages, 3387 KiB  
Article
Functional Porous Ionic Polymers as Efficient Heterogeneous Catalysts for the Chemical Fixation of CO2 under Mild Conditions
by Zhifeng Dai, Yang Long, Jianliang Liu, Yuanfei Bao, Liping Zheng, Jiacong Ma, Jiayi Liu, Fei Zhang, Yubing Xiong and Ji-Qing Lu
Polymers 2022, 14(13), 2658; https://doi.org/10.3390/polym14132658 - 29 Jun 2022
Cited by 10 | Viewed by 2483
Abstract
The development of efficient and metal-free heterogeneous catalysts for the chemical fixation of CO2 into value-added products is still a challenge. Herein, we reported two kinds of polar group (−COOH, −OH)-functionalized porous ionic polymers (PIPs) that were constructed from the corresponding phosphonium [...] Read more.
The development of efficient and metal-free heterogeneous catalysts for the chemical fixation of CO2 into value-added products is still a challenge. Herein, we reported two kinds of polar group (−COOH, −OH)-functionalized porous ionic polymers (PIPs) that were constructed from the corresponding phosphonium salt monomers (v-PBC and v-PBH) using a solvothermal radical polymerization method. The resulting PIPs (POP-PBC and POP-PBH) can be used as efficient bifunctional heterogeneous catalysts in the cycloaddition reaction of CO2 with epoxides under relatively low temperature, ambient pressure, and metal-free conditions without any additives. It was found that the catalytic activities of the POP-PBC and POP-PBH were comparable with the homogeneous catalysts of Me-PBC and PBH and were higher than that of the POP-PPh3-COOH that was synthesized through a post-modification method, indicating the importance of the high concentration catalytic active sites in the heterogeneous catalysts. Reaction under low CO2 concentration conditions showed that the activity of the POP-PBC (with a conversion of 53.8% and a selectivity of 99.0%) was higher than that of the POP-PBH (with a conversion of 32.3% and a selectivity of 99.0%), verifying the promoting effect of the polar group (−COOH group) in the porous framework. The POP-PBC can also be recycled at least five times without a significant loss of catalytic activity, indicating the high stability and robustness of the PIPs-based heterogeneous catalysts. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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18 pages, 2568 KiB  
Article
Charge Transport and Glassy Dynamics in Blends Based on 1-Butyl-3-vinylbenzylimidazolium Bis(trifluoromethanesulfonyl)imide Ionic Liquid and the Corresponding Polymer
by Maxi Hoffmann, Ciprian Iacob, Gina Kaysan, Mira Simmler, Hermann Nirschl, Gisela Guthausen and Manfred Wilhelm
Polymers 2022, 14(12), 2423; https://doi.org/10.3390/polym14122423 - 15 Jun 2022
Cited by 2 | Viewed by 2589
Abstract
Charge transport, diffusion properties, and glassy dynamics of blends of imidazolium-based ionic liquid (IL) and the corresponding polymer (polyIL) were examined by Pulsed-Field-Gradient Nuclear Magnetic Resonance (PFG-NMR) and rheology coupled with broadband dielectric spectroscopy (rheo-BDS). We found that the mechanical storage modulus [...] Read more.
Charge transport, diffusion properties, and glassy dynamics of blends of imidazolium-based ionic liquid (IL) and the corresponding polymer (polyIL) were examined by Pulsed-Field-Gradient Nuclear Magnetic Resonance (PFG-NMR) and rheology coupled with broadband dielectric spectroscopy (rheo-BDS). We found that the mechanical storage modulus (G′) increases with an increasing amount of polyIL and G′ is a factor of 10,000 higher for the polyIL compared to the monomer (GIL′= 7.5 Pa at 100 rad s−1 and 298 K). Furthermore, the ionic conductivity (σ0) of the IL is a factor 1000 higher than its value for the polymerized monomer with 3.4×10−4 S cm−1 at 298 K. Additionally, we found the Haven Ratio (HR) obtained through PFG-NMR and BDS measurements to be constant around a value of 1.4 for the IL and blends with 30 wt% and 70 wt% polyIL. These results show that blending of the components does not have a strong impact on the charge transport compared to the charge transport in the pure IL at room temperature, but blending results in substantial modifications of the mechanical properties. Furthermore, it is highlighted that the increase in σ0 might be attributed to the addition of a more mobile phase, which also possibly reduces ion-ion correlations in the polyIL. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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17 pages, 2182 KiB  
Article
Swelling and Diffusion in Polymerized Ionic Liquids-Based Hydrogels
by Ann Jastram, Tobias Lindner, Christian Luebbert, Gabriele Sadowski and Udo Kragl
Polymers 2021, 13(11), 1834; https://doi.org/10.3390/polym13111834 - 1 Jun 2021
Cited by 24 | Viewed by 5499
Abstract
Hydrogels are one of the emerging classes of materials in current research. Besides their numerous applications in the medical sector as a drug delivery system or in tissue replacement, they are also suitable as irrigation components or as immobilization matrices in catalysis. For [...] Read more.
Hydrogels are one of the emerging classes of materials in current research. Besides their numerous applications in the medical sector as a drug delivery system or in tissue replacement, they are also suitable as irrigation components or as immobilization matrices in catalysis. For optimal application of these compounds, knowledge of the swelling properties and the diffusion mechanisms occurring in the gels is mandatory. This study is focused on hydrogels synthesized by radical polymerization of imidazolium-based ionic liquids. Both the swelling and diffusion behavior of these hydrogels were investigated via gravimetric swelling as well as sorption experiments implemented in water, ethanol, n-heptane, and tetrahydrofuran. In water and ethanol, strong swelling was observed while the transport mechanism deviated from Fickian-type behavior. By varying the counterion and the chain length of the cation, their influences on the processes were observed. The calculation of the diffusion coefficients delivered values in the range of 10−10 to 10−12 m2 s−1. The gravimetric results were supported by apparent diffusion coefficients measured through diffusion-weighted magnetic resonance imaging. A visualization of the water diffusion front within the hydrogel should help to further elucidate the diffusion processes in the imidazolium-based hydrogels. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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19 pages, 5277 KiB  
Article
Viscoelastic Relaxation of Polymerized Ionic Liquid and Lithium Salt Mixtures: Effect of Salt Concentration
by Arisa Yokokoji, Wakana Kitayama, Kamonthira Wichai, Osamu Urakawa, Atsushi Matsumoto, Visit Vao-Soongnern and Tadashi Inoue
Polymers 2021, 13(11), 1772; https://doi.org/10.3390/polym13111772 - 28 May 2021
Cited by 9 | Viewed by 3919
Abstract
Polymerized ionic liquids (PILs) doped with lithium salts have recently attracted research interests as the polymer component in lithium-ion batteries because of their high ionic mobilities and lithium-ion transference numbers. To date, although the ion transport mechanism in lithium-doped PILs has been considerably [...] Read more.
Polymerized ionic liquids (PILs) doped with lithium salts have recently attracted research interests as the polymer component in lithium-ion batteries because of their high ionic mobilities and lithium-ion transference numbers. To date, although the ion transport mechanism in lithium-doped PILs has been considerably studied, the role of lithium salts on the dynamics of PIL chains remains poorly understood. Herein, we examine the thermal and rheological behaviors of the mixture of poly(1-butyl-3-vinylimidazolium bis(trifluoromethanesulfonyl)imide (PC4-TFSI)/lithium TFSI (LiTFSI) in order to clarify the effect of the addition of LiTFSI. We show that the glass transition temperature Tg and the entanglement density decrease with the increase in LiTFSI concentration wLiTFSI. These results indicate that LiTFSI acts as a plasticizer for PC4-TFSI. Comparison of the frequency dependence of the complex modulus under the iso-frictional condition reveals that the addition of LiTFSI does not modify the stress relaxation mechanism of PC4-TFSI, including its characteristic time scale. This suggests that the doped LiTFSI, component that can be carrier ions, is not so firmly bound to the polymer chain as it modifies the chain dynamics. In addition, a broadening of the loss modulus spectrum in the glass region occurs at high wLiTFSI. This change in the spectrum can be caused by the responses of free TFSI and/or coordination complexes of Li and TFSI. Our detailed rheological analysis can extract the information of the dynamical features for PIL/salt mixtures and may provide helpful knowledge for the control of mechanical properties and ion mobilities in PILs. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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17 pages, 5809 KiB  
Article
The Influences of 1-Butyl-3-Methylimidazolium Tetrafluoroborate on Electrochemical, Thermal and Structural Studies as Ionic Liquid Gel Polymer Electrolyte
by Mariah Zuliana Dzulkipli, Jamilah Karim, Azizan Ahmad, Nurul Akmaliah Dzulkurnain, Mohd Sukor Su’ait, Masahiro Yoshizawa-Fujita, Lee Tian Khoon and Nur Hasyareeda Hassan
Polymers 2021, 13(8), 1277; https://doi.org/10.3390/polym13081277 - 14 Apr 2021
Cited by 17 | Viewed by 4819
Abstract
After decades of development, ionic liquid gel polymer electrolytes (ILGPEs) are currently experiencing a renaissance as a promising electrolyte to be used in electrochemical devices. Their inherent tendency towards poor electrochemical properties have limited their applications and commercialization activities. Henceforth, gel polymer electrolyte [...] Read more.
After decades of development, ionic liquid gel polymer electrolytes (ILGPEs) are currently experiencing a renaissance as a promising electrolyte to be used in electrochemical devices. Their inherent tendency towards poor electrochemical properties have limited their applications and commercialization activities. Henceforth, gel polymer electrolyte (GPE) is being introduced to alleviate the abovementioned issues. In this work, the assessment of the ionic liquid 1-butyl-3-methylimidazolium tetrafluoroborate [BMIM][BF4] in poly (vinylidene fluoride-hexafluoropropylene) (PVDF-HFP) to form ILGPE was done. The relationship of [BMIM][BF4] towards the dielectric properties at different wt. % ratios and temperature was ascertained. The results indicated that [BMIM]BF4 is able to facilitate fast conduction. Moreover, it was found that [BMIM][BF4] could serve as an effective agent in reducing crystallinity and glass transition temperature of the polymer and thus enhanced the ionic conductivity of the samples. Notwithstanding, the ILGPE sample possessed a high thermal stability up to 300 °C and good electrochemical stability of 4.2 V which are beneficial for operation in electrochemical devices. All in all, the correlation between the ionic liquid chemistry and electrochemical performances could provide a valuable insight to rational selection and design for ILGPE electrolytes. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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Review

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17 pages, 2938 KiB  
Review
Recent Advances in Poly(Ionic Liquid)-Based Membranes for CO2 Separation
by Gabriel Bernardo and Hugo Gaspar
Polymers 2023, 15(3), 667; https://doi.org/10.3390/polym15030667 - 28 Jan 2023
Cited by 9 | Viewed by 2458
Abstract
Poly(ionic liquid)-based membranes have been the subject of intensive research in the last 15 years due to their potential for the separation of CO2 from other gases. In this short review, different types of PIL-based membranes for CO2 separation are described [...] Read more.
Poly(ionic liquid)-based membranes have been the subject of intensive research in the last 15 years due to their potential for the separation of CO2 from other gases. In this short review, different types of PIL-based membranes for CO2 separation are described (neat PIL membranes; PIL-IL composite membranes; PIL-polymer blend membranes; PIL-based block copolymer membranes, and PIL-based mixed matrix membranes), and their state-of-the-art separation results for different gas pairs (CO2/N2, CO2/H2, and CO2/CH4) are presented and discussed. This review article is focused on the most relevant research works performed over the last 5 years, that is, since the year 2017 onwards, in the field of poly(ionic liquid)-based membranes for CO2 separation. The micro- and nano-morphological characterization of the membranes is highlighted as a research topic that requires deeper study and understanding. Nowadays there is an array of advanced structural characterization techniques, such as neutron scattering techniques with contrast variation (using selective deuteration), that can be used to probe the micro- and nanostructure of membranes, in length scales ranging from ~1 nm to ~15 μm. Although some of these techniques have been used to study the morphology of PIL-based membranes for electrochemical applications, their use in the study of PIL-based membranes for CO2 separation is still unknown. Full article
(This article belongs to the Special Issue Advances in Polymerized Ionic Liquids and Their Composites)
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