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A special issue of Micromachines (ISSN 2072-666X). This special issue belongs to the section "D：Materials and Processing".

Deadline for manuscript submissions: closed (31 August 2018) | Viewed by 67873

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Special Issue Editors

Prof. Dr. Dmitry Volodkin

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Guest Editor

College of Science and Technology, Nottingham Trent University, Clifton Lane, Nottingham NG11 8NS, UK
Interests: polymer self-assembly; encapsulation and release of bioactive molecules; microfluidics; raman microscopy; hard and soft templating; polymer scaffolds; cell-surface engineering; 2D and 3D cell culture
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Dr. Anna Vikulina

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Postdoctoral research fellow, College of Science and Technology, Nottingham Trent University, Clifton Lane, Nottingham NG11 8NS, UK
Interests: lipid assembly; lipid chemistry and analysis; liposomes; molecular transport; diffusion phenomenon; controlled release; drug delivery; biomedical applications

Special Issue Information

Dear Colleagues,

Nowadays, polymer self-assembly has become extremely attractive for both biological (drug delivery, tissue engineering, scaffolds) and non-biological (packaging, semiconductors) applications. In nature, a number of key biological processes are driven by polymer self-assembly, for instance protein folding. Impressive morphologies can be assembled from polymers thanks to a diverse range of interactions involved, e.g., electrostatics, hydrophobic, hots-guest interactions, etc. Both 2D and 3D tailor-made assemblies can be designed through modern powerful techniques and approaches such as the layer-by-layer and the Langmuir-Blodgett deposition, hard and soft templating.

This Special Issue highlights contributions (research papers, short communications, review articles) that focus on recent developments in polymer self-assembly for both fundamental understanding the assembly phenomenon and real applications. Particular attention is paid to:

microfluidic-assisted self-assembly
design of (bio)polymer based devices and films
colloidal particles and multilayers
core-shell structures
bio-functional self-assembled structures
hybrid polymer assemblies with lipids and nanoparticles
polymer mobility and structure of self-assemblies
mechanism of polymer self-assembly

Contributions related to new technologies and material aspects of polymer assemblies are very welcome.

Prof. Dr. Dmitry Volodkin
Dr. Anna Vikulina
Guest Editors

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Keywords

Self-assembly
Polymer
Multilayers
Core-shell
Hybrid Materials
Lipids
Nanoparticles
Biopolymers

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Related Special Issue

Hybrid and Polymer Assemblies in Micromachines (6 articles)

Published Papers (11 papers)

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Editorial

Jump to: Research, Review

2 pages, 145 KiB

Open AccessEditorial

Editorial for the Special Issue on Self-Assembly of Polymers

by Anna S. Vikulina and Dmitry Volodkin

Micromachines 2019, 10(8), 519; https://doi.org/10.3390/mi10080519 - 5 Aug 2019

Viewed by 2473

Abstract

The self-assembly of polymers is a powerful tool for producing various functional materials with a high precision from nano- to macroscale [...] Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

Research

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10 pages, 1603 KiB

Open AccessArticle

Marine Polysaccharide-Collagen Coatings on Ti6Al4V Alloy Formed by Self-Assembly

by Karl Norris, Oksana I. Mishukova, Agata Zykwinska, Sylvia Colliec-Jouault, Corinne Sinquin, Andrei Koptioug, Stéphane Cuenot, Jemma G. Kerns, Maria A. Surmeneva, Roman A. Surmenev and Timothy E.L. Douglas

Micromachines 2019, 10(1), 68; https://doi.org/10.3390/mi10010068 - 19 Jan 2019

Cited by 12 | Viewed by 4223

Abstract

Polysaccharides of marine origin are gaining interest as biomaterial components. Bacteria derived from deep-sea hydrothermal vents can produce sulfated exopolysaccharides (EPS), which can influence cell behavior. The use of such polysaccharides as components of organic, collagen fibril-based coatings on biomaterial surfaces remains unexplored. In this study, collagen fibril coatings enriched with HE800 and GY785 EPS derivatives were deposited on titanium alloy (Ti6Al4V) scaffolds produced by rapid prototyping and subjected to physicochemical and cell biological characterization. Coatings were formed by a self-assembly process whereby polysaccharides were added to acidic collagen molecule solution, followed by neutralization to induced self-assembly of collagen fibrils. Fibril formation resulted in collagen hydrogel formation. Hydrogels formed directly on Ti6Al4V surfaces, and fibrils adsorbed onto the surface. Scanning electron microscopy (SEM) analysis of collagen fibril coatings revealed association of polysaccharides with fibrils. Cell biological characterization revealed good cell adhesion and growth on bare Ti6Al4V surfaces, as well as coatings of collagen fibrils only and collagen fibrils enhanced with HE800 and GY785 EPS derivatives. Hence, the use of both EPS derivatives as coating components is feasible. Further work should focus on cell differentiation. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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15 pages, 3653 KiB

Open AccessArticle

Internal Structure of Matrix-Type Multilayer Capsules Templated on Porous Vaterite CaCO₃ Crystals as Probed by Staining with a Fluorescence Dye

by Lucas Jeannot, Michael Bell, Ryan Ashwell, Dmitry Volodkin and Anna S. Vikulina

Micromachines 2018, 9(11), 547; https://doi.org/10.3390/mi9110547 - 25 Oct 2018

Cited by 24 | Viewed by 4812

Abstract

Multilayer capsules templated on decomposable vaterite CaCO₃ crystals are widely used as vehicles for drug delivery. The capsule represents typically not a hollow but matrix-like structure due to polymer diffusion into the porous crystals during multilayer deposition. The capsule formation mechanism is not well-studied but its understanding is crucial to tune capsule structure for a proper drug release performance. This study proposes new approach to noninvasively probe and adjust internal capsule structure. Polymer capsules made of poly(styrene-sulfonate) (PSS) and poly(diallyldimethylammonium chloride) (PDAD) have been stained with fluorescence dye rhodamine 6G. Physical-chemical aspects of intermolecular interactions required to validate the approach and adjust capsule structure are addressed. The capsules consist of a defined shell (typically 0.5–2 µm) and an internal matrix of PSS-PDAD complex (typically 10–40% of a total capsule volume). An increase of ionic strength and polymer deposition time leads to the thickening of the capsule shell and formation of a denser internal matrix, respectively. This is explained by effects of a polymer conformation and limitations in polymer diffusion through the crystal pores. We believe that the design of the capsules with desired internal structure will allow achieving effective encapsulation and controlled/programmed release of bioactives for advanced drug delivery applications. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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16 pages, 4866 KiB

Open AccessArticle

Self-Assembled Mucin-Containing Microcarriers via Hard Templating on CaCO₃ Crystals

by Nadezhda G. Balabushevich, Ekaterina A. Sholina, Elena V. Mikhalchik, Lyubov Y. Filatova, Anna S. Vikulina and Dmitry Volodkin

Micromachines 2018, 9(6), 307; https://doi.org/10.3390/mi9060307 - 19 Jun 2018

Cited by 45 | Viewed by 6504

Abstract

Porous vaterite crystals of CaCO₃ are extensively used for the fabrication of self-assembled polymer-based microparticles (capsules, beads, etc.) utilized for drug delivery and controlled release. The nature of the polymer used plays a crucial role and discovery of new perspective biopolymers is essential to assemble microparticles with desired characteristics, such as biocompatibility, drug loading efficiency/capacity, release rate, and stability. Glycoprotein mucin is tested here as a good candidate to assemble the microparticles because of high charge due to sialic acids, mucoadhesive properties, and a tendency to self-assemble, forming gels. Mucin loading into the crystals via co-synthesis is twice as effective as via adsorption into preformed crystals. Desialylated mucin has weaker binding to the crystals most probably due to electrostatic interactions between sialic acids and calcium ions on the crystal surface. Improved loading of low-molecular-weight inhibitor aprotinin into the mucin-containing crystals is demonstrated. Multilayer capsules (mucin/protamine)₃ have been made by the layer-by-layer self-assembly. Interestingly, the deposition of single mucin layers (mucin/water)₃ has also been proven, however, the capsules were unstable, most probably due to additional (to hydrogen bonding) electrostatic interactions in the case of the two polymers used. Finally, approaches to load biologically-active compounds (BACs) into the mucin-containing microparticles are discussed. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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18 pages, 6759 KiB

Open AccessArticle

A Facile Interfacial Self-Assembly of Crystalline Colloidal Monolayers by Tension Gradient

by Dong Feng, Ding Weng and Jiadao Wang

Micromachines 2018, 9(6), 297; https://doi.org/10.3390/mi9060297 - 13 Jun 2018

Cited by 14 | Viewed by 6127

Abstract

Many self-assembly approaches of colloidal monolayers have flourished but with some shortages, such as complexity, time-consumption, parameter sensitivity, and high-cost. This paper presents a facile, rapid, well-controlled, and low-cost method to prepare monolayers by directly adding silica particle suspensions containing water and ethanol to different liquids. A detailed analysis of the self-assembly process was conducted. The particles dove into water firstly, then moved up under the effect of the buoyancy and the tension gradient. The tension gradient induced the Marangoni convection and the relative motion between the water and the particles. At last, the particles were adsorbed at the air-water interface to minimize the free energy. The quality of the monolayers depended on the addition of sodium dodecyl sulfonate or ethanol in the water subphase. An interfacial polymerization of ethyl 2-cyanoacrylate was used to determine the contact angles of the particles at different subphase surfaces. The value of the detachment energy was positively associated with the contact angle and the surface tension. When the detachment energy decreased to a certain value, some particles detached from the surface, leading to the formation of a quasi-double layer. We also observed that the content of ethanol in suspensions influenced the arrangement of particles. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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21 pages, 6547 KiB

Open AccessArticle

High-Precision Solvent Vapor Annealing for Block Copolymer Thin Films

by Gunnar Nelson, Chloe S. Drapes, Meagan A. Grant, Ryan Gnabasik, Jeffrey Wong and Andrew Baruth

Micromachines 2018, 9(6), 271; https://doi.org/10.3390/mi9060271 - 29 May 2018

Cited by 17 | Viewed by 6469

Abstract

Despite its efficacy in producing well-ordered, periodic nanostructures, the intricate role multiple parameters play in solvent vapor annealing has not been fully established. In solvent vapor annealing a thin polymer film is exposed to a vapor of solvent(s) thus forming a swollen and mobile layer to direct the self-assembly process at the nanoscale. Recent developments in both theory and experiments have directly identified critical parameters that govern this process, but controlling them in any systematic way has proven non-trivial. These identified parameters include vapor pressure, solvent concentration in the film, and the solvent evaporation rate. To explore their role, a purpose-built solvent vapor annealing chamber was designed and constructed. The all-metal chamber is designed to be inert to solvent exposure. Computer-controlled, pneumatically actuated valves allow for precision timing in the introduction and withdrawal of solvent vapor from the film. The mass flow controller-regulated inlet, chamber pressure gauges, in situ spectral reflectance-based thickness monitoring, and low flow micrometer relief valve give real-time monitoring and control during the annealing and evaporation phases with unprecedented precision and accuracy. The reliable and repeatable alignment of polylactide cylinders formed from polystyrene-b-polylactide, where cylinders stand perpendicular to the substrate and span the thickness of the film, provides one illustrative example. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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15 pages, 3742 KiB

Open AccessArticle

Self-Assembly Behavior and pH-Stimuli-Responsive Property of POSS-Based Amphiphilic Block Copolymers in Solution

by Yiting Xu, Kaiwei He, Hongchao Wang, Meng Li, Tong Shen, Xinyu Liu, Conghui Yuan and Lizong Dai

Micromachines 2018, 9(6), 258; https://doi.org/10.3390/mi9060258 - 24 May 2018

Cited by 10 | Viewed by 4308

Abstract

Stimuli-responsive polymeric systems containing special responsive moieties can undergo alteration of chemical structures and physical properties in response to external stimulus. We synthesized a hybrid amphiphilic block copolymer containing methoxy polyethylene glycol (MePEG), methacrylate isobutyl polyhedral oligomeric silsesquioxane (MAPOSS) and 2-(diisopropylamino)ethyl methacrylate (DPA) named MePEG-b-P(MAPOSS-co-DPA) via atom transfer radical polymerization (ATRP). Spherical micelles with a core-shell structure were obtained by a self-assembly process based on MePEG-b-P(MAPOSS-co-DPA), which showed a pH-responsive property. The influence of hydrophobic chain length on the self-assembly behavior was also studied. The pyrene release properties of micelles and their ability of antifouling were further studied. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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12 pages, 13384 KiB

Open AccessArticle

Microstructure Formation of Functional Polymers by Evaporative Self-Assembly under Flexible Geometric Confinement

by Xiangmeng Li, Xijing Zhu and Huifen Wei

Micromachines 2018, 9(3), 124; https://doi.org/10.3390/mi9030124 - 12 Mar 2018

Cited by 3 | Viewed by 5518

Abstract

Polymer microstructures are widely used in optics, flexible electronics, and so forth. We demonstrate a cost-effective bottom-up manner for patterning polymer microstructures by evaporative self-assembly under a flexible geometric confinement at a high temperature. Two-parallel-plates confinement would become curve-to-flat shape geometric confinement as the polydimethylsiloxane (PDMS) cover plate deformed during solvent swelling. We found that a flexible cover plate would be favorable for the formation of gradient microstructures, with various periodicities and widths obtained at varied heights of clearance. After thermal annealing, the edge of the PMMA (Poly-methylmethacrylate) microstructures would become smooth, while the RR-P3HT (regioregular-poly(3-hexylthiophene)) might generate nanocrystals. The morphologies of RR-P3HT structures included thick films, straight lines, hierarchical stripes, incomplete stripes, and regular dots. Finally, a simple field-effect transistor (FET) device was demonstrated with the RR-P3HT micropattern as an active layer. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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Review

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21 pages, 3741 KiB

Open AccessReview

Porous Alginate Scaffolds Assembled Using Vaterite CaCO₃ Crystals

by Alena Sergeeva, Anna S. Vikulina and Dmitry Volodkin

Micromachines 2019, 10(6), 357; https://doi.org/10.3390/mi10060357 - 29 May 2019

Cited by 60 | Viewed by 8315

Abstract

Formulation of multifunctional biopolymer-based scaffolds is one of the major focuses in modern tissue engineering and regenerative medicine. Besides proper mechanical/chemical properties, an ideal scaffold should: (i) possess a well-tuned porous internal structure for cell seeding/growth and (ii) host bioactive molecules to be protected against biodegradation and presented to cells when required. Alginate hydrogels were extensively developed to serve as scaffolds, and recent advances in the hydrogel formulation demonstrate their applicability as “ideal” soft scaffolds. This review focuses on advanced porous alginate scaffolds (PAS) fabricated using hard templating on vaterite CaCO₃ crystals. These novel tailor-made soft structures can be prepared at physiologically relevant conditions offering a high level of control over their internal structure and high performance for loading/release of bioactive macromolecules. The novel approach to assemble PAS is compared with traditional methods used for fabrication of porous alginate hydrogels. Finally, future perspectives and applications of PAS for advanced cell culture, tissue engineering, and drug testing are discussed. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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23 pages, 2313 KiB

Open AccessReview

Biocatalysis by Transglutaminases: A Review of Biotechnological Applications

by Maria Pia Savoca, Elisa Tonoli, Adeola G. Atobatele and Elisabetta A. M. Verderio

Micromachines 2018, 9(11), 562; https://doi.org/10.3390/mi9110562 - 31 Oct 2018

Cited by 79 | Viewed by 9074

Abstract

The biocatalytic activity of transglutaminases (TGs) leads to the synthesis of new covalent isopeptide bonds (crosslinks) between peptide-bound glutamine and lysine residues, but also the transamidation of primary amines to glutamine residues, which ultimately can result into protein polymerisation. Operating with a cysteine/histidine/aspartic acid (Cys/His/Asp) catalytic triad, TGs induce the post-translational modification of proteins at both physiological and pathological conditions (e.g., accumulation of matrices in tissue fibrosis). Because of the disparate biotechnological applications, this large family of protein-remodelling enzymes have stimulated an escalation of interest. In the past 50 years, both mammalian and microbial TGs polymerising activity has been exploited in the food industry for the improvement of aliments’ quality, texture, and nutritive value, other than to enhance the food appearance and increased marketability. At the same time, the ability of TGs to crosslink extracellular matrix proteins, like collagen, as well as synthetic biopolymers, has led to multiple applications in biomedicine, such as the production of biocompatible scaffolds and hydrogels for tissue engineering and drug delivery, or DNA-protein bio-conjugation and antibody functionalisation. Here, we summarise the most recent advances in the field, focusing on the utilisation of TGs-mediated protein multimerisation in biotechnological and bioengineering applications. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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18 pages, 5655 KiB

Open AccessReview

Progress in Photo-Responsive Polypeptide Derived Nano-Assemblies

by Lu Yang, Houliang Tang and Hao Sun

Micromachines 2018, 9(6), 296; https://doi.org/10.3390/mi9060296 - 13 Jun 2018

Cited by 32 | Viewed by 8420

Abstract

Stimuli-responsive polymeric materials have attracted significant attention in a variety of high-value-added and industrial applications during the past decade. Among various stimuli, light is of particular interest as a stimulus because of its unique advantages, such as precisely spatiotemporal control, mild conditions, ease of use, and tunability. In recent years, a lot of effort towards the synthesis of a biocompatible and biodegradable polypeptide has resulted in many examples of photo-responsive nanoparticles. Depending on the specific photochemistry, those polypeptide derived nano-assemblies are capable of crosslinking, disassembling, or morphing into other shapes upon light irradiation. In this mini-review, we aim to assess the current state of photo-responsive polypeptide based nanomaterials. Firstly, those ‘smart’ nanomaterials will be categorized by their photo-triggered events (i.e., crosslinking, degradation, and isomerization), which are inherently governed by photo-sensitive functionalities, including O-nitrobenzyl, coumarin, azobenzene, cinnamyl, and spiropyran. In addition, the properties and applications of those polypeptide nanomaterials will be highlighted as well. Finally, the current challenges and future directions of this subject will be evaluated. Full article

(This article belongs to the Special Issue Self-Assembly of Polymers)

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