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Copolymers: Preparation and Applications
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Copolymers: Preparation and Applications

A special issue of Molecules (ISSN 1420-3049). This special issue belongs to the section "Materials Chemistry".

Deadline for manuscript submissions: closed (28 February 2021) | Viewed by 12101

Special Issue Editor

Prof. Dr. Andrew G. Tennyson

E-Mail Website
Guest Editor
Clemson University Center for Optical Materials Science, Departments of Chemistry and Engineering Technologies & Materials Science and Engineering 91 Technology Drive, 483 Hunter Labs Anderson, SC 29625 Clemson, SC 29634
Interests: organometallic chemistry; bioinorganic chemistry; sustainable chemistry; redox catalysis; photocatalysis; reactive oxygen species; sulfur; organic/organometallic polymers; inorganic materials

Special Issue Information

Dear Colleagues,

Polymers have propelled revolutionary advances in human civilization by providing access to a wide variety of materials whose properties can be rationally tuned at the molecular level in a controlled manner. If more than one type of monomer is polymerized, the resulting copolymer can exhibit properties that are a blend of the two original polymers or may be totally unlike either. Copolymers provide a convenient architecture for the orthogonal control of material structures, properties, and functions. This Special Issue of Molecules is dedicated to all aspects of the syntheses of copolymers and their applications, and researchers working in these areas are welcome to submit their original works and reviews for publication in this Special Issue. Submissions may cover any facet of the preparation and application of copolymers; cross-disciplinary studies and those emphasizing controllable copolymer microstructures and tunable copolymer properties/functions are particularly welcome.

Prof. Andrew G. Tennyson
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. Molecules 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

  • Copolymer
  • Microstructure
  • Structure–function relationships
  • Structure–property relationships
  • Copolymer regiocontrol
  • Copolymer stereocontrol
  • Switchable polymerization catalyst
  • Orthogonal polymerization
  • Conjugated polymer
  • Organic photovoltaics
  • Organic electronics
  • Biomaterials
  • Structural materials

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Published Papers (3 papers)

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Research

18 pages, 5840 KiB  
Article
Comparative Analysis of Ethylene/Diene Copolymerization and Ethylene/Propylene/Diene Terpolymerization Using Ansa-Zirconocene Catalyst with Alkylaluminum/Borate Activator: The Effect of Conjugated and Nonconjugated Dienes on Catalytic Behavior and Polymer Microstructure
by Amjad Ali, Muhammad Khurram Tufail, Muhammad Imran Jamil, Waleed Yaseen, Nafees Iqbal, Munir Hussain, Asad Ali, Tariq Aziz, Zhiqiang Fan and Li Guo
Molecules 2021, 26(7), 2037; https://doi.org/10.3390/molecules26072037 - 2 Apr 2021
Cited by 25 | Viewed by 3877
Abstract
The copolymerization of ethylene‒diene conjugates (butadiene (BD), isoprene (IP) and nonconjugates (5-ethylidene-2-norbornene (ENB), vinyl norbornene VNB, 4-vinylcyclohexene (VCH) and 1, 4-hexadiene (HD)), and terpolymerization of ethylene-propylene-diene conjugates (BD, IP) and nonconjugates (ENB, VNB, VCH and HD) using two traditional catalysts of C2 [...] Read more.
The copolymerization of ethylene‒diene conjugates (butadiene (BD), isoprene (IP) and nonconjugates (5-ethylidene-2-norbornene (ENB), vinyl norbornene VNB, 4-vinylcyclohexene (VCH) and 1, 4-hexadiene (HD)), and terpolymerization of ethylene-propylene-diene conjugates (BD, IP) and nonconjugates (ENB, VNB, VCH and HD) using two traditional catalysts of C2-symmetric metallocene—silylene-bridged rac-Me2Si(2-Me-4-Ph-Ind)2ZrCl2 (complex A) and ethylene-bridged rac-Et(Ind)2ZrCl2 (complex B)—with a [Ph3C][B(C6F5)4] borate/TIBA co-catalyst, were intensively studied. Compared to that in the copolymerization of ethylene diene, the catalytic activity was more significant in E/P/diene terpolymerization. We obtained a maximum yield of both metallocene catalysts with conjugated diene between 3.00 × 106 g/molMt·h and 5.00 × 106 g/molMt·h. ENB had the highest deactivation impact on complex A, and HD had the most substantial deactivation effect on complex B. A 1H NMR study suggests that dienes were incorporated into the co/ter polymers’ backbone through regioselectivity. ENB and VNB, inserted by the edo double bond, left the ethylidene double bond intact, so VCH had an exo double bond. Complex A’s methyl and phenyl groups rendered it structurally stable and exhibited a dihedral angle greater than that of complex B, resulting in 1, 2 isoprene insertion higher than 1, 4 isoprene that is usually incapable of polymerization coordination. High efficiency in terms of co- and ter- monomer incorporation with higher molecular weight was found for complex 1. The rate of incorporation of ethylene and propylene in the terpolymer backbone structure may also be altered by the conjugated and nonconjugated dienes. 13C-NMR, 1H-NMR, and GPC techniques were used to characterize the polymers obtained. Full article
(This article belongs to the Special Issue Copolymers: Preparation and Applications)
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10 pages, 16270 KiB  
Article
Precise Synthesis and Thin Film Self-Assembly of PLLA-b-PS Bottlebrush Block Copolymers
by Eunkyung Ji, Cian Cummins and Guillaume Fleury
Molecules 2021, 26(5), 1412; https://doi.org/10.3390/molecules26051412 - 5 Mar 2021
Cited by 9 | Viewed by 3352
Abstract
The ability of bottlebrush block copolymers (BBCPs) to self-assemble into ordered large periodic structures could greatly expand the scope of photonic and membrane technologies. In this paper, we describe a two-step synthesis of poly(l-lactide)-b-polystyrene (PLLA-b-PS) BBCPs and [...] Read more.
The ability of bottlebrush block copolymers (BBCPs) to self-assemble into ordered large periodic structures could greatly expand the scope of photonic and membrane technologies. In this paper, we describe a two-step synthesis of poly(l-lactide)-b-polystyrene (PLLA-b-PS) BBCPs and their rapid thin-film self-assembly. PLLA chains were grown from exo-5-norbornene-2-methanol via ring-opening polymerization (ROP) of l-lactide to produce norbornene-terminated PLLA. Norbonene-terminated PS was prepared using anionic polymerization followed by a termination reaction with exo-5-norbornene-2-carbonyl chloride. PLLA-b-PS BBCPs were prepared from these two norbornenyl macromonomers by a one-pot sequential ring opening metathesis polymerization (ROMP). PLLA-b-PS BBCPs thin-films exhibited cylindrical and lamellar morphologies depending on the relative block volume fractions, with domain sizes of 46–58 nm and periodicities of 70–102 nm. Additionally, nanoporous templates were produced by the selective etching of PLLA blocks from ordered structures. The findings described in this work provide further insight into the controlled synthesis of BBCPs leading to various possible morphologies for applications requiring large periodicities. Moreover, the rapid thin film patterning strategy demonstrated (>5 min) highlights the advantages of using PLLA-b-PS BBCP materials beyond their linear BCP analogues in terms of both dimensions achievable and reduced processing time. Full article
(This article belongs to the Special Issue Copolymers: Preparation and Applications)
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Graphical abstract

16 pages, 6527 KiB  
Article
Synthesis of Block Copolymer Brush by RAFT and Click Chemistry and Its Self-Assembly as a Thin Film
by Hajeeth Thankappan, Mona Semsarilar, Suming Li, Yung Chang, Denis Bouyer and Damien Quemener
Molecules 2020, 25(20), 4774; https://doi.org/10.3390/molecules25204774 - 17 Oct 2020
Cited by 5 | Viewed by 4049
Abstract
A well-defined block copolymer brush poly(glycidyl methacrylate)-graft-(poly(methyl methacrylate)-block- poly(oligo(ethylene glycol) methyl ether methacrylate)) (PGMA-g-(PMMA-b-POEGMA)) is synthesized via grafting from an approach based on a combination of click chemistry and reversible addition-fragmentation chain transfer (RAFT) polymerization. [...] Read more.
A well-defined block copolymer brush poly(glycidyl methacrylate)-graft-(poly(methyl methacrylate)-block- poly(oligo(ethylene glycol) methyl ether methacrylate)) (PGMA-g-(PMMA-b-POEGMA)) is synthesized via grafting from an approach based on a combination of click chemistry and reversible addition-fragmentation chain transfer (RAFT) polymerization. The resulting block copolymer brushes were characterized by 1H-NMR and size exclusion chromatography (SEC). The self-assembly of the block copolymer brush was then investigated under selective solvent conditions in three systems: THF/water, THF/CH3OH, and DMSO/CHCl3. PGMA-g-(PMMA-b-POEGMA) was found to self-assemble into spherical micelle structures as analyzed by transmission electron microscopy (TEM) and dynamic light scattering (DLS). The average size of the particles was much smaller in THF/CH3OH and DMSO/CHCl3 as compared with the THF/water system. Thin film of block copolymer brushes with tunable surface properties was then prepared by the spin-coating technique. The thickness of the thin film was confirmed by scanning electron microscopy (SEM). Atom force microscopy (AFM) analysis revealed a spherical morphology when the block copolymer brush was treated with poor solvents for the backbone and hydrophobic side chains. The contact angle measurements were used to confirm the surface rearrangements of the block copolymer brushes. Full article
(This article belongs to the Special Issue Copolymers: Preparation and Applications)
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