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Advances and Applications of Block Copolymers II

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

Deadline for manuscript submissions: 15 September 2025 | Viewed by 11910

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Dr. Nikolaos Politakos

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POLYMAT and Departamento de Química Aplicada, Facultad de Ciencias Químicas, University of the Basque Country UPV/EHU, Joxe Mari Korta Zentroa, Tolosa Etorbidea 72, 20018 San Sebastián, Spain
Interests: chemical modification reactions; preparation of composite materials; synthesis of hydrogels for wound healing
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Prof. Dr. Apostolos Avgeropoulos

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Laboratory of Polymer Science & Engineering, Department of Materials Science Engineering, University of Ioannina, University Campus-Dourouti, 45110 Ioannina, Greece
Interests: living polymerization methods (anionic and living radical) of linear and non-linear polymers; molecular characterization in solution; self assembly of various types of polymers; structure/properties relationship; various modification reactions for polymers; superhydrophobic and super hydrophilic materials; conjugated polymers; nanopatterning of nanostructures
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Special Issue Information

Dear Colleagues,

Over the years, research on polymers have significanlty increased, providing new insights into their applications for improving existing technologies and systems. A wide array of polymerization techniques are available which can polymerize most monomers, thereby leading to the formation of block copolymers (BCPs) that possess various advanced properties such as self-healing, self-assembly, high biocompatibility, and responsiveness.

Numerous studies have already been published on the potential applications and advantages of BCPs which have substantial scientific, societal, as well as economic impacts. Nevertheless, many challenges in their development and utilization remain to be tackled, such as issues related to the synthetic procedure, scale-up, using biocompatible materials, and high technological applications.

This Special Issue, ‘Advances and Applications of Block Copolymers II’ invites submissions of review articles, original research manuscripts, and short communications that undercore the recent progess achieved in developing and using BCPs. The keywords presented below indicate some potential topics of interest; however, the list is not exhaustive, and papers addressing any other relevant aspects of BCPs will be accepted as well.

Dr. Nikolaos Politakos
Prof. Dr. Apostolos Avgeropoulos
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

polymers
copolymers
block copolymers
controlled synthesis
anionic polymerization
RAFT polymerization
ATRP polymerization
emulsion polymerization
molecular characterization
morphological characterization
terpolymers
hybrid materials
polypeptides
polymeric chimeras
composite materials
self-assembly
polymer brushes
biopolymers
biocompatibility
smart materials
responsive properties
hydrogels
drug delivery
computational chemistry
structure–property relationship
polymer nano/micro particles
self-healing materials
recyclability

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Published Papers (9 papers)

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18 pages, 4872 KiB

Open AccessArticle

Optimizing the Synthesis of CO₂-Responsive Polymers: A Kinetic Model Approach for Scaling Up

by Emil Pashayev and Prokopios Georgopanos

Polymers 2025, 17(8), 1115; https://doi.org/10.3390/polym17081115 - 20 Apr 2025

Viewed by 180

Abstract

The kinetic model is a crucial tool for optimizing polymer synthesis protocols and facilitating the scaled-up production processes of the CO₂-responsive polymer poly(N-[3-(dimethylamino)propyl]-acrylamide)-b-poly(methyl methacrylate)(PDMAPAm-b-PMMA), which is supposed to be implemented in direct air capture (DAC) technology. This study presents a simulation of the kinetic model developed for the Reversible Addition−Fragmentation Chain-Transfer (RAFT) polymerization of N-[3-(dimethylamino)propyl]-acrylamide (DMAPAm), alongside an investigation into the kinetics of this polymerization using the simulation as an analytical tool, as well as the application of the simulation for the upscaling of RAFT polymerization. Ultimately, the kinetic model was validated through two kinetic experiments, confirming its reliability. It was subsequently employed to optimize the synthesis recipe and to predict the properties of PDMAPAm homopolymers, thereby supporting the upscaling of PDMAPAm-b-PMMA diblock copolymer synthesis. In the end, the preliminary results of the CO₂-responsiveness of the diblock copolymer were determined with a simple experiment. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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16 pages, 12999 KiB

Open AccessArticle

One-Pot Synthesis of Amphiphilic Linear and Hyperbranched Polyelectrolytes and Their Stimuli-Responsive Self-Assembly in Aqueous Solutions

by Angelica Maria Gerardos, Aleksander Forys, Barbara Trzebicka and Stergios Pispas

Polymers 2025, 17(5), 701; https://doi.org/10.3390/polym17050701 - 6 Mar 2025

Viewed by 611

Abstract

Stimuli-responsive polymeric nanostructures are compelling vectors for a wide range of application opportunities. The objective we sought was to broaden the array of self-assembling amphiphilic copolymers with stimuli-responsive characteristics by introducing a hydrophilic tunable monomer, (2-dimethylamino)ethyl methacrylate (DMAEMA), together with a hydrophilic one, lauryl methacrylate (LMA), within linear and branched copolymer topologies. Size exclusion chromatography was used to evaluate the resultant linear and hyperbranched copolymers’ molecular weight and dispersity, and FT-IR and ¹H-NMR spectroscopy techniques were used to delineate their chemical structure. The structural changes in the obtained self-organized supramolecular structures were thoroughly investigated using aqueous media with varying pH and salinity by dynamic light scattering (DLS), fluorescence spectroscopy (FS), and transmission electron microscopy (TEM). The nanoscale assemblies formed by the amphiphiles indicate significant potential for applications within the field of nanotechnology. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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15 pages, 9544 KiB

Open AccessArticle

Preparation and Characterization of Melamine Aniline Formaldehyde-Organo Clay Nanocomposite Foams (MAFOCF) as a Novel Thermal Insulation Material

by Ahmet Gürses and Elif Şahin

Polymers 2024, 16(24), 3578; https://doi.org/10.3390/polym16243578 - 21 Dec 2024

Viewed by 749

Abstract

The main purpose of this study is to prepare a melamine aniline formaldehyde foam, an MAF copolymer, with lower water sensitivity and non-flammability properties obtained by the condensation reaction of melamine, aniline, and formaldehyde. In addition, the preparation of MAFF composites with organoclay reinforcement was determined as a secondary target in order to obtain better mechanical strength, heat, and sound insulation properties. For the synthesis of foams, the microwave irradiation technique, which offers advantages such as faster reactions, high yields and purities, and reduced curing times, was used together with the heating technique and the effect of organoclay content on the structural and textural properties of foams and both heat insulation and mechanical stability was investigated. Virgin melamine formaldehyde foam, MFF, melamine aniline formaldehyde foam, MAFFF, and melamine aniline formaldehyde–organoclay nanocomposite foams prepared with various organoclay contents, MAFOCFs, were characterized by HRTEM, FTIR, SEM, and XRD techniques. From spectroscopic and microscopic analyses, it was observed that organoclay flakes could be exfoliated without much change in the resin matrix with increasing clay content. In addition, it was determined that aniline formaldehyde, which is thought to enter the main polymer network as a bridge, caused textural changes in the polymeric matrix, and organoclay reinforcement also affected these changes. Although the highest compressive strength was obtained in MAFOCF5 foam with high organoclay content (0.40 MPa), it was determined that the compressive strengths in the nanocomposites were generally quite high despite their low bulk densities. In the prepared nanocomposite with 0.30% organoclay content (MAFOCF2), 0.33 MPa compressive strength and 0.051 thermal conductivity coefficient were measured. For virgin polymers and composites, bulk density, thermal conductivity, and compressive strength values were determined in the order of magnitude as MFF > MAFOCF1 > MAFOCF5 > MAFOCF6 > MAFF > MAFOCF3 > MAFOCF2 > MAFOCF4; MFF > MAFF > MAFOCF6 > MAFOCF5 > MAFOCF1 > MAFOCF4 > MAFOCF3 > MAFOCF2 and MAFOCF5 > MAFOCF4 > MAFOCF2 > MAFF > MAFOCF6 > MFF > MAFOCF1 > MAFOCF3. As a result, both compressive strength and thermal conductivity values indicate that nanocomposite foam with 0.20 wt% organoclay content can be a promising new insulation material. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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15 pages, 2336 KiB

Open AccessArticle

On the Properties of Styrene–Maleic Acid Copolymer–Lipid Nanoparticles: A Solution NMR Perspective

by Vladislav V. Motov, Erik F. Kot, Svetlana O. Kislova, Eduard V. Bocharov, Alexander S. Arseniev, Ivan A. Boldyrev, Sergey A. Goncharuk and Konstantin S. Mineev

Polymers 2024, 16(21), 3009; https://doi.org/10.3390/polym16213009 - 26 Oct 2024

Viewed by 1479

Abstract

The production of functionally active membrane proteins (MPs) in an adequate membrane environment is a key step in structural biology. Polymer–lipid particles based on styrene and maleic acid (SMA) represent a promising type of membrane mimic, as they can extract properly folded MPs directly from their native lipid environment. However, the original SMA polymer is sensitive to acidic pH levels, which has led to the development of several modifications: SMA-EA, SMA-QA, and others. Here, we introduce a novel SMA derivative with a negatively charged taurine moiety, SMA-tau, and investigate the formation and characteristics of lipid–SMA-EA and lipid–SMA-tau membrane-mimicking particles. Our findings demonstrate that both polymers can form nanodiscs with a patch of lipid bilayer that can undergo phase transitions at temperatures close to those of the lipid bilayer membranes. Finally, we discuss the potential applications of these SMAs for NMR spectroscopy. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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19 pages, 2379 KiB

Open AccessEditor’s ChoiceArticle

Spectroscopic and Thermal Characterisation of Interpenetrating Hydrogel Networks (IHNs) Based on Polymethacrylates and Pluronics, and Their Physicochemical Stability under Aqueous Conditions

by David S. Jones, Marion Westwood, Shu Li and Gavin P. Andrews

Polymers 2024, 16(19), 2796; https://doi.org/10.3390/polym16192796 - 1 Oct 2024

Viewed by 967

Abstract

This study describes the physicochemical characterisation of interpenetrating hydrogel networks (IHNs) composed of either poly(hydroxyethylmethacrylate, p(HEMA)) or poly(methacrylic acid, p(MAA)), and Pluronic block copolymers (grades F127, P123 and L121). IHNs were prepared by mixing the acrylate monomer with Pluronic block copolymers followed by free radical polymerisation. p(HEMA)–Pluronic blends were immiscible, evident from a lack of interaction between the two components (Raman spectroscopy) and the presence of the glass transitions (differential scanning calorimetry, DSC) of the two components. Conversely, IHNs of p(MAA) and each Pluronic were miscible, displaying a single glass transition and secondary bonding between the carbonyl group of p(MAA) and the ether groups in the Pluronic block copolymers (Raman and ATR-FTIR spectroscopy). The effect of storage of the IHNs in Tris buffer on the physical state of each Pluronic and on the loss of Pluronic from the IHNs were studied using DSC and gravimetric analysis, respectively. Pluronic loss from the IHNs was dependent on the grade of Pluronic, time of immersion in Tris buffer, and the nature of the IHN (p(HEMA) or p(MAA)). At equilibrium, the loss was greater from p(HEMA) than from p(MAA) IHNs, whereas increasing ratio of poly(propylene oxide) to poly(ethylene oxide) decreased Pluronic loss. The retention of each Pluronic grade was shown to be primarily due to its micellization; however, hydrogen bonding between Pluronic and p(MAA) (but not p(HEMA)) IHNs contributed to their retention. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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22 pages, 12390 KiB

Open AccessArticle

Preparation and Structural-Thermodynamical Investigation of Renewable Copolyesters Based on Poly (Ethylene Succinate) and Polyisosorbide

by Chaima Bouyahya, Panagiotis A. Klonos, Alexandra Zamboulis, Eleftheria Xanthopoulou, Nina Maria Ainali, Mustapha Majdoub, Apostolos Kyritsis and Dimitrios N. Bikiaris

Polymers 2024, 16(15), 2173; https://doi.org/10.3390/polym16152173 - 30 Jul 2024

Cited by 1 | Viewed by 1204

Abstract

A series of novel renewable copolymers based on poly(ethylene succinate) (PESu) and poly(isosorbide succinate) (PISSu), with the Isosorbide (Is)/PESu molar ratio varying from 5/95 to 75/25, were synthesized in-situ and studied in this work. A sum of characterization techniques was employed here for the structural and thermo-dynamical characterization. The sophisticated technique of dielectric spectroscopy, along with proper analysis, enabled the molecular dynamics mapping of both the local and segmental types, which is presented for such materials for the first time. With increasing the Is fraction, shorter copolymeric entities were gradually formed. Based on the overall findings, the systems were found to be homogeneous, e.g., exhibiting single glass transitions, with the two polymer segments being found to be excellently distributed. The latter is indirect, although strong, evidence for the successful copolymerization. The thermal degradation mechanism for the copolymers was exhaustingly explored employing analytical pyrolysis. The systems exhibited, in general, good thermal stability, according to the thermogravimetric analysis. Confirming one of the initial scopes for the present systems, isosorbide plays here the role of hardener (PISSu) over the soft polymer (PESu), and this is reflected in the monotonic increase of the glass transition temperature, T_g, from −16 to ~56 °C. The introduction of Is results in an increase in constraints (hardening of the matrix), while there seems to be an overall densification of the polymer (decrease of the free volume). Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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11 pages, 7386 KiB

Open AccessArticle

Directed Self-Assembly of Cylinder-Forming Block Copolymers Using Pillar Topographic Patterns

by June Huh

Polymers 2024, 16(7), 881; https://doi.org/10.3390/polym16070881 - 23 Mar 2024

Cited by 1 | Viewed by 2534

Abstract

We conducted a computational study on the self-assembly behavior of cylinder-forming block copolymers, directed by a guide pattern of hexagonally or tetragonally arrayed pillars, using mesoscale density functional theory simulations. By adjusting the spacing (

L_{p}

) and diameter (D) [...] Read more.

L_{p}

) and diameter (D) of the pillars in relation to the intrinsic cylinder-to-cylinder distance (

L_{2}

) of the cylinder-forming block copolymer, we investigated the efficiency of multiple-replicating cylinders, generated by the block copolymer, through the pillar-directed self-assembly process. The simulations demonstrated that at specific values of normalized parameters

{\tilde{L}}_{2} = L_{2} / L_{p}

and

\tilde{D} = D / L_{p}

coupled with suitable surface fields, triple and quadruple replications are achievable with a hexagonally arrayed pillar pattern, while only double replication is attainable with a tetragonally arrayed pillar pattern. This work, offering an extensive structure map encompassing a wide range of possible parameter spaces, including

{\tilde{L}}_{2}

and

\tilde{D}

, serves as a valuable guide for designing the contact hole patterning essential in nanoelectronics applications. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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15 pages, 2370 KiB

Open AccessArticle

Investigation of Crystallization, Morphology, and Mechanical Properties of Polypropylene/Polypropylene-Polyethylene Block Copolymer Blends

by Wenjun Shao, Li-Zhi Liu, Ying Wang, Yuanxia Wang, Ying Shi and Lixin Song

Polymers 2023, 15(24), 4680; https://doi.org/10.3390/polym15244680 - 12 Dec 2023

Cited by 6 | Viewed by 2973

Abstract

Polyethylene (PE)-based elastomers are the ideal choice for enhancing the compatibility of polypropylene/polyethylene (PP/PE) blends and improving the mechanical properties of PP-based materials. However, the issue of blend systems lies in the interplay between the crystallization processes. Therefore, we investigated the crystallization behavior during the cooling process of a new generation of PP/PE block copolymers (PP-b-PE) and random polypropylene (PPR, a copolymer of propylene and a small amount of ethylene or an alpha-olefin) blends using in-situ X-ray diffraction/scattering and differential scanning calorimetry (DSC) techniques. We also conducted mechanical performance tests on PPR/PP-b-PE blends at room temperature and low temperature (−5 °C). The results indicate that during the cooling process, the PP phase of PP-b-PE will follow the PPR to crystallize in advance and form a eutectic mixture, thereby enhancing the compatibility of PP/PE. Moreover, the PPR/PP-b-PE blend will form stable β-(300) crystals with excellent mechanical properties. Due to the improved compatibility of PP/PE with PP-b-PE, PE crystals are dispersed within PP crystals, providing bonding that improves the toughness of PPR under the low stiffness failure conditions of PPR/PP-b-PE blends, thereby enhancing their impact performance at low and room temperatures. This research has great significance for both recycling waste plastics and enhancing the low-temperature toughness of PPR. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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22 pages, 4903 KiB

Open AccessReview

Hybrid Materials Based on Self-Assembled Block Copolymers and Magnetic Nanoparticles—A Review

by Galder Kortaberria

Polymers 2025, 17(10), 1292; https://doi.org/10.3390/polym17101292 - 8 May 2025

Viewed by 285

Abstract

In this review work, the different routes and methods for preparing hybrid materials based on nanostructured block copolymers (BCPs) and magnetic nanoparticles (MNPs) are analyzed, as they can be potentially employed in different sectors like biomedicine, electronic or optoelectronic devices, data storing devices, etc. The first procedure for their preparation consists of the nanostructuring of BCPs in the presence of previously synthesized NPs by modifying their surface for increasing compatibility with the matrix or employing magnetic fields for NP orientation, which can also promote the orientation of nanodomains. Surface modification with surfactants led to the selective confinement of NPs depending on the interaction (mainly hydrogen bonding) degree and their intensity. Surface modification with brushes can be performed by three methods, including grafting from, grafting to, or grafting through. Those methods are compared in terms of success for the positioning and confinement of NPs in the desired domains, showing the crucial importance of brush length and grafting density, as well as of NP amount and modification degree in the self-assembled morphology. Regarding the use of external magnetic fields, the importance of relative amounts of MNPs and BCPs employed and that of the magnetic field intensity for the orientation of the NPs and the nearby BCP domains is shown. The second procedure, consisting of the in situ synthesis of NPs inside the nanodomains by a reduction in the respective metallic ions or employing metal-containing BCPs for the generation of MNP patterns or arrays, is also shown. In all cases, the transference of magnetic properties to the nanocomposite was successful. Finally, a brief summary of some aspects about the use of BCPs for the synthesis, encapsulation, and release of MNPs is shown, as they present potential biomedical applications such as cancer treatment, among others. Full article

(This article belongs to the Special Issue Advances and Applications of Block Copolymers II)

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