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Advances in Polyelectrolytes

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

Deadline for manuscript submissions: closed (10 November 2023) | Viewed by 25514

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Prof. Dr. Ming-Jay Deng

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Guest Editor

Department of Applied Chemistry, Providence University, 200 Taiwan Boulevard, Sec. 7, Taichung 43301, Taiwan
Interests: flexible supercapacitor; gel electrolyte; biomimetic material; energy conservation and energy storage; in situ XAS; machine learning

Prof. Dr. Che-Lun Hung

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Institute of Biomedical Informatics, National Yang Ming Chiao Tung University, Taipei, Taiwan
Interests: smart medicine; deep learning; medical image analysis; bioinformatics computing; high-performance computing
Special Issues, Collections and Topics in MDPI journals

Prof. Dr. Ming-Tsz Chen

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Guest Editor

Department of Applied Chemistry, Providence University, Taichung 02918, Taiwan
Interests: organometallic chemistry; catalysis science; polymerization for biodegradable polymers

Special Issue Information

Dear Colleagues,

Electrolytes have played important roles in energy storage, osmotic pressure and photovoltaic performance. Liquid electrolytes have displayed an outstanding performances in Li-ion batteries in recent decades, with high ionic conductivity and great connections with electrode materials. However, the use of liquid electrolytes often causes risks associated with leakage, evaporation and combustion. Therefore, polyelectrolytes (PELs) are potential candidates to replace liquid electrolyte systems. Besides, PELs have received increasing research attention due to their relevant characteristics, which extend from their liquid electrolytes and solid electrolytes.

Thus, this Special Issue is devoted to the survey of recent progress in this multidisciplinary area of PELs for robotics, wearable devices or self-charged sensor applications. Original contributions and reviews focusing on aspects ranging from their design and production to their characterisation and applications, along with a deep understanding of their physical performance, are welcome. The scope may include, but is not limited to, electrodes, membranes, hydrogels, electrolytes or PEL as process aids.

We think that you could make an excellent contribution to our journal and would like to invite you to submit a paper.

The submission deadline is 5 October 2021. You may send your manuscript immediately or at any point until the deadline. Submitted papers should not be under consideration for publication elsewhere. You can also submit to this special issue two month after the deadline.

Prof. Dr. Ming-Jay Deng
Prof. Dr. Che-Lun Hung
Prof. Dr. Ming-Tsz Chen
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 gel electrolyte
supercapacitors
batteries
metal organic frameworks
machine learning
sensors
phosphors
computer aid
computing methods
biomaterials

Published Papers (10 papers)

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Research

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22 pages, 14996 KiB

Open AccessArticle

Effect of Crosslinking Conditions on the Transport of Protons and Methanol in Crosslinked Polyvinyl Alcohol Membranes Containing the Phosphoric Acid Group

by Zhiwei Wang, Hao Zheng, Jinyao Chen, Wei Wang, Furui Sun and Ya Cao

Polymers 2023, 15(21), 4198; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15214198 - 24 Oct 2023

Viewed by 1188

Abstract

In this investigation, we systematically explored the intricate relationship between the structural attributes of polyvinyl alcohol (PVA) membranes and their multifaceted properties relevant to fuel cell applications, encompassing diverse crosslinking conditions. Employing the solution casting technique, we fabricated crosslinked PVA membranes by utilizing phosphoric acid (PA) as the crosslinking agent, modulating the crosslinking temperature across a range of values. This comprehensive approach aimed to optimize the selection of crosslinking parameters for the advancement of crosslinked polymer materials tailored for fuel cell contexts. A series of meticulously tailored crosslinked PVA membranes were synthesized, each varying in PBTCA content (5–30 wt.%) to establish a systematic framework for elucidating chemical interactions, morphological transformations, and physicochemical attributes pertinent to fuel cell utilization. The manipulation of crosslinking agent concentration and crosslinking temperature engendered a discernible impact on the crosslinking degree, leading to a concomitant reduction in crystallinity. Time-resolved attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) was harnessed to evaluate the dynamics of liquid water adsorption and ionomer swelling kinetics within the array of fabricated PVA films. Notably, the diffusion of water within the PVA membranes adhered faithfully to Fick’s law, with discernible sensitivity to the crosslinking conditions being implemented. Within the evaluated membranes, proton conductivities exhibited a span of between 10⁻³ and 10⁻² S/cm, while methanol permeabilities ranged from 10⁻⁸ to 10⁻⁷ cm²/s. A remarkable revelation surfaced during the course of this study, as it became evident that the structural attributes and properties of the PVA films, under the influence of distinct crosslinking conditions, underwent coherent modifications. These changes were intrinsically linked to alterations in crosslinking degree and crystallinity, reinforcing the interdependence of these parameters in shaping the characteristics of PVA films intended for diverse fuel cell applications. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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15 pages, 2181 KiB

Open AccessArticle

Evaluation of Polymer Gel Electrolytes for Use in MnO₂ Symmetric Flexible Electrochemical Supercapacitors

by Yu-Hao Lin, Wan-Tien Huang, Yi-Ting Huang, Yi-Ni Jhang, Tsung-Ting Shih, Murat Yılmaz and Ming-Jay Deng

Polymers 2023, 15(16), 3438; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15163438 - 17 Aug 2023

Cited by 1 | Viewed by 1054

Abstract

Flexible electrochemical supercapacitors (FESCs) are emerging as innovative energy storage systems, characterized by their stable performance, long cycle life, and portability/foldability. Crucial components of FESCs, such as electrodes and efficient electrolytes, have become the focus of extensive research. Herein, we examine deep eutectic solvent (DES)–based polymer gel systems for their cost-effective accessibility, simple synthesis, excellent biocompatibility, and exceptional thermal and electrochemical stability. We used a mixture a DES, LiClO₄–2-Oxazolidinone as the electroactive species, and a polymer, either polyvinyl alcohol (PVA) or polyacrylamide (PAAM) as a redox additive/plasticizer. This combination facilitates a unique ion-transport process, enhancing the overall electrochemical performance of the polymer gel electrolyte. We manufactured and used LiClO₄–2-Oxazolidinone (LO), polyvinyl alcohol–LiClO₄–2-Oxazolidinone (PVA–LO), and polyacrylamide–LiClO₄–2-Oxazolidinone (PAAM–LO) electrolytes to synthesize an MnO₂ symmetric FESC. To evaluate their performance, we analyzed the MnO₂ symmetric FESC using various electrolytes with cyclic voltammetry (CV), galvanostatic charge–discharge (GCD), and electrochemical impedance spectroscopy (EIS). The FESC featuring the PVA–LO electrolyte demonstrated superior electrochemical and mechanical performances. This solid-state MnO₂ symmetric FESC exhibited a specific capacitance of 121.6 F/g within a potential window of 2.4 V. Due to the excellent ionic conductivity and the wide electrochemical operating voltage range of the PVA–LO electrolyte, a high energy density of 97.3 Wh/kg at 1200 W/kg, and a long-lasting energy storage system (89.7% capacitance retention after 5000 cycles of GCD at 2 A/g) are feasibly achieved. For practical applications, we employed the MnO₂ symmetric FESCs with the PVA–LO electrolyte to power a digital watch and a light-emitting diode, further demonstrating their real-world utility. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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12 pages, 3524 KiB

Open AccessArticle

Behaviour of FITC-Labeled Polyallylamine in Polyelectrolyte Microcapsules

by Alexey V. Dubrovskii, Alexey V. Berezhnov, Aleksandr L. Kim and Sergey A. Tikhonenko

Polymers 2023, 15(16), 3330; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15163330 - 08 Aug 2023

Viewed by 697

Abstract

There are many studies devoted to the application of polyelectrolyte microcapsules (PMC) in various fields; however, there are significantly fewer studies devoted to the study of the polyelectrolyte microcapsules themselves. The study examined the mutual arrangement of the polyelectrolytes in 13-layered PMC capsules composed of (PAH/PSS)₆PAH. The research showed that different layers of the polyelectrolyte microcapsules dissociate equally, as in the case of 13-layered PMC capsules composed of (PAH/PSS)₆PAH with a well-defined shell, and in the case of 7-layered PMC capsules composed of (PAH/PSS)₃PAH, where the shell is absent. The study showed that polyallylamine layers labeled with FITC migrate to the periphery of the microcapsule regardless of the number of layers. This is due to an increase in osmotic pressure caused by the rapid flow of ions from the interior of the microcapsule into the surrounding solution. In addition, FITC-polyallylamine has a lower charge density and less interaction with polystyrene sulfonate in the structure of the microcapsule. Meanwhile, the hydrophilicity of FITC-polyallylamine does not change or decreases slightly. The results suggest that this effect promotes the migration of labeled polyallylamine to a more hydrophilic region of the microcapsule, towards its periphery. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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13 pages, 4069 KiB

Open AccessArticle

Enhancement in Power Conversion Efficiency of Perovskite Solar Cells by Reduced Non-Radiative Recombination Using a Brij C10-Mixed PEDOT:PSS Hole Transport Layer

by Sehyun Jung, Seungsun Choi, Woojin Shin, Hyesung Oh, Jaewon Oh, Mee-Yi Ryu, Wonsik Kim, Soohyung Park and Hyunbok Lee

Polymers 2023, 15(3), 772; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15030772 - 02 Feb 2023

Cited by 2 | Viewed by 1741

Abstract

Interface properties between charge transport and perovskite light-absorbing layers have a significant impact on the power conversion efficiency (PCE) of perovskite solar cells (PSCs). Poly(3,4-ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS) is a polyelectrolyte composite that is widely used as a hole transport layer (HTL) to facilitate hole transport from a perovskite layer to an anode. However, PEDOT:PSS must be modified using a functional additive because PSCs with a pristine PEDOT:PSS HTL do not exhibit a high PCE. Herein, we demonstrate an increase in the PCE of PSCs with a polyethylene glycol hexadecyl ether (Brij C10)-mixed PEDOT:PSS HTL. Photoelectron spectroscopy results show that the Brij C10 content becomes significantly high in the HTL surface composition with an increase in the Brij C10 concentration (0–5 wt%). The enhanced PSC performance, e.g., a PCE increase from 8.05 to 11.40%, is attributed to the reduction in non-radiative recombination at the interface between PEDOT:PSS and perovskite by the insulating Brij C10. These results indicate that the suppression of interface recombination is essential for attaining a high PCE for PSCs. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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10 pages, 2213 KiB

Open AccessArticle

The Effect of Transparent Conducting Oxide Films on WO₃-Based Electrochromic Devices with Conducting Polymer Electrolytes

by Benedict Wen-Cheun Au, Kah-Yoong Chan, Gregory Soon How Thien, Mian-En Yeoh, Mohd Zainizan Sahdan and Hanabe Chowdappa Ananda Murthy

Polymers 2023, 15(1), 238; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15010238 - 03 Jan 2023

Cited by 2 | Viewed by 1771

Abstract

Over the past few decades, electrochromism has been a prominent topic in energy-saving applications, which is based on the mechanism of altering the optical transmittance of EC materials under the effect of a small applied voltage. Thus, tungsten oxide (WO₃) is a significant chemical compound typically applied in electrochromic devices (ECDs) as it is responsible for the optical transmittance variation. In this work, the WO₃ films were produced through a sol–gel spin-coating method. The effect of various transparent conducting oxides (TCOs, which are indium-doped tin oxide (ITO), fluorine-doped tin oxide (FTO) glass substrates, and aluminum-doped zinc oxide (AZO)) was investigated in the construction of ECDs. Based on a conducting polymer polypyrene carbonate electrolyte, ITO and aluminum-doped zinc oxide (AZO)-coated glasses were also examined as counter electrodes. The electrode combination employing FTO and ITO as the TCO and counter electrode, respectively, exhibited the most significant coloration efficiency of 72.53 cm²/C. It had coloring and bleaching transmittance of 14% and 56%, respectively, with a large optical modulation of 42%. In addition to that, ECDs with the AZO counter electrode have the advantage of lower intercalation charges compared to ITO and FTO. Hence, this research offers a new avenue for understanding the role of common TCO and counter electrodes in the development of WO₃-based ECDs with conducting polymer electrolytes. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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9 pages, 4006 KiB

Open AccessArticle

Colorful Luminescence of Conjugated Polyelectrolytes Induced by Molecular Weight

by Kunsheng Wang, Yueqin Shi and Zhengjun Li

Polymers 2022, 14(24), 5372; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14245372 - 08 Dec 2022

Viewed by 1030

Abstract

Due to their distinctive intrinsic advantages, the nanoaggregates of conjugated polyelectrolytes (CPEs) are fascinating and attractive for various luminescence applications. Generally, the emission luminescence of CPEs is determined by the conjugated backbone structure, i.e., different conjugated backbones of CPEs produce emission luminescence with different emission wavelength bands. Here, we polymerized the bis(boronic ester) of benzothiadiazole and an alkyl sulfonate sodium-substituted dibromobenzothiatriazole to provide PBTBTz-SO₃Na with different molecular weights via controlling the ratio of the monomer and the catalyst. Theoretically, the CPEs with the same molecular structure usually display similar photoelectronic performances. However, the resulting PBTBTz-SO₃Na reveal a similar light absorption property, but different luminescence. The higher molecular weight is, the stronger the fluorescence intensity of PBTBTz-SO₃Na that occurs. PBTBTz-SO₃Na with different molecular weights have different colors of luminescence. It is well known that the molecular aggregates often led to weaker luminescent properties for most of the conjugated polymers. However, PBTBTz-SO₃Na exhibits a higher molecular weight with an increasing molecular chain aggregation, i.e., the nanoaggregates of PBTBTz-SO₃Na are beneficial to emission luminescence. This work provides a new possible chemical design of CPEs with a controllable, variable luminescence for further optoelectronics and biomedicine applications. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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13 pages, 1704 KiB

Open AccessArticle

Proton-Conducting Biopolymer Electrolytes Based on Carboxymethyl Cellulose Doped with Ammonium Formate

by M. I. H. Sohaimy and M. I. N. Isa

Polymers 2022, 14(15), 3019; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14153019 - 26 Jul 2022

Cited by 12 | Viewed by 1679

Abstract

In this work, CMC-AFT biopolymer electrolytes system was developed using Carboxymethyl cellulose (CMC) doped with varied amount (10–50 wt.%) of ammonium formate (AFT) in order to study the effect of AFT on the biopolymer-salt system. The chemical structure of the biopolymer was studied using Fourier-Transform infrared (FTIR) and X-ray diffraction (XRD). The interaction between the COO⁻ of CMC and the weakly-bound H⁺ of NH₄⁺ AFT occurred at 1573 cm⁻¹ as seen in FTIR analysis and the amorphous phase was found to increase with the addition of AFT as seen from XRD pattern. Both FTIR and XRD testing indicates that the AFT had disrupted the CMC crystalline structure. The ionic conductivity of the CMC-AFT biopolymer electrolytes increases and achieved the highest value of 1.47 × 10⁻⁴ S·cm⁻¹ with the addition of AFT. The impedance measurement showed that the capacitive and resistive behavior inside the biopolymer diminished when 50 wt.% of AFT was added. Dielectric analysis confirmed the increased number of charge carriers is due to the increase in AFT composition. Further dielectric analysis showed the occurrence of conductivity relaxation peak thus affirmed the charge carriers’ ability to travel further to a longer distances when AFT composition increases from 10 to 50 wt.%. The dielectric properties confirmed the non-Debye behavior of the CMC-AFT biopolymer electrolytes. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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13 pages, 2962 KiB

Open AccessArticle

Enhanced Pseudocapacitive Performance of Symmetric Polypyrrole-MnO₂ Electrode and Polymer Gel Electrolyte

by Wen-Jun Zhuo, Yen-Hua Wang, Chia-Tse Huang and Ming-Jay Deng

Polymers 2021, 13(20), 3577; https://0-doi-org.brum.beds.ac.uk/10.3390/polym13203577 - 16 Oct 2021

Cited by 6 | Viewed by 2212

Abstract

Herein, the nanostructured polypyrrole-coated MnO₂ nanofibers growth on carbon cloth (PPy-MnO₂-CC) to serve as the electrodes used in conjunction with a quasi-ionic liquid-based polymer gel electrolyte (urea-LiClO₄-PVA) for solid-state symmetric supercapacitors (SSCs). The resultant PPy-MnO₂-CC solid-state SSCs exhibited a high specific capacitance of 270 F/g at 1.0 A/g in a stable and wide potential window of 2.1 V with a high energy/power density (165.3 Wh/kg at 1.0 kW/kg and 21.0 kW/kg at 86.4 Wh/kg) along with great cycling stability (capacitance retention of 92.1% retention after 3000 cycles) and rate capability (141 F/g at 20 A/g), exceeding most of the previously reported SSCs. The outstanding performance of the studied 2.1 V PPy-MnO₂-CC flexible SSCs could be attributed to the nanostructured PPy-coated MnO₂ composite electrode and the urea-LiClO₄-PVA polymer gel electrolyte design. In addition, the PPy-MnO₂-CC solid-state SSCs could effectively retain their electrochemical performance at various bending angles, demonstrating their huge potential as power sources for flexible and lightweight electronic devices. This work offers an easy way to design and achieve light weight and high-performance SSCs with enhanced energy/power density. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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20 pages, 6657 KiB

Open AccessFeature PaperReview

A Brief Review of Gel Polymer Electrolytes Using In Situ Polymerization for Lithium-ion Polymer Batteries

by Wookil Chae, Bumsang Kim, Won Sun Ryoo and Taeshik Earmme

Polymers 2023, 15(4), 803; https://0-doi-org.brum.beds.ac.uk/10.3390/polym15040803 - 05 Feb 2023

Cited by 19 | Viewed by 8752

Abstract

Polymer electrolytes (PEs) have been thoroughly investigated due to their advantages that can prevent severe problems of Li-ion batteries, such as electrolyte leakage, flammability, and lithium dendrite growth to enhance thermal and electrochemical stabilities. Gel polymer electrolytes (GPEs) using in situ polymerization are typically prepared by thermal or UV curing methods by initially impregnating liquid precursors inside the electrode. The in situ method can resolve insufficient interfacial problems between electrode and electrolyte compared with the ex situ method, which could led to a poor cycle performance due to high interfacial resistance. In addition to the abovementioned advantage, it can enhance the form factor of bare cells since the precursor can be injected before polymerization prior to the solidification of the desired shapes. These suggest that gel polymer electrolytes prepared by in situ polymerization are a promising material for lithium-ion batteries. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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16 pages, 1219 KiB

Open AccessReview

Towards an All-Solid-State Electrochromic Device: A Review of Solid-State Electrolytes and the Way Forward

by Benedict Wen-Cheun Au and Kah-Yoong Chan

Polymers 2022, 14(12), 2458; https://0-doi-org.brum.beds.ac.uk/10.3390/polym14122458 - 16 Jun 2022

Cited by 9 | Viewed by 3575

Abstract

In order to curb high electricity usage, especially in commercial buildings, smart windows, also known as “switchable” or “smart” glasses, have attracted a significant amount of attention in an effort to achieve energy savings in eco-friendly buildings and transportation systems. Smart windows save energy by regulating the input of solar heat and light and hence cutting down air-conditioning expenses, while maintaining indoor comfort. This is achieved by electrochromism, which is defined as the reversible colour change in electrochromic (EC) materials from transparent to dark blue and vice versa under a small applied voltage. Recent state-of-the-art electrochromic devices (ECD) adopt liquid-based electrolytes as the main source of energy for basic operations. While this has resulted in much success in ECDs as reported in past studies, there remain several drawbacks to this aspect, such as liquid electrolyte leakage and evaporation, not to mention safety concerns related to the harmful nature of electrolyte materials. This paper aims to review the recent advances in various solid electrolytes that are potential solutions to the mentioned problems. Full article

(This article belongs to the Special Issue Advances in Polyelectrolytes)

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