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Macromolecular Self-Assembly Materials: From Modeling to Advanced Application

A special issue of Materials (ISSN 1996-1944). This special issue belongs to the section "Biomaterials".

Deadline for manuscript submissions: closed (31 January 2020) | Viewed by 24648

Special Issue Editors


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Guest Editor
Dipartimento di Scienze Matematiche e Informatiche, Scienze Fisiche e Scienze della Terra, Università di Messina, Messina, Italy
Interests: integrated spectroscopic techniques; climate modeling; weather modelling; complex systems
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Consiglio Nazionale delle Ricerche, Istituto Processi Chimico-Fisici, (CNR–IPCF), 98158 Messina, Italy
Interests: structure and interactuion in nano-colloids (polymers and block copolymers; dendrimers; lipids; proteins); self-assembly in nanostructured (and hybrid) materials; interaction of nanoparticles with model bio-membranes and biomaterials
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Recently, material systems obtained by the self-assembly processes of nanostructures stimulated the development of a new generation of advanced functional materials in a wide range of disciplines, including material science and engineering, environmental science, pharmaceutical, biotechnology and nanomedicine, cosmetics, and food and agricultural science. The synthesis of novel chemical structures and the efficient use of soft and supramolecular interactions can generate novel structural properties and new protocols for the design of novel materials with nanoscale ordered morphologies suitable for advanced applications in nanotechnology. Novel theoretical and experimental approaches in nano-structures self-assembly are necessary in order to form a knowledge basis for the modern scientific community. Researchers are invited to contribute original research and review articles that investigate the self-assembly processes of material science, with the aim to propose prominent examples of the bottom-up approach, where the assemblies of different components and their integrated actions allow for the performance of highly specific functions suitable for novel and smart applications in material science and biotechnology.

Prof. Dr. Salvatore Magazu
Dr. Domenico Lombardo
Guest Editors

Manuscript Submission Information

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Keywords

  • Self-assembly
  • Supramolecular chemistry
  • Synthesis of nanoparticles and smart materials
  • Modeling and simulation of nanomaterials
  • Hybrid (organic-inorganic) materials
  • Surfactants, amphiphiles, and liquid crystals
  • Drug delivery
  • Tissue engineering
  • Complex systems

Published Papers (6 papers)

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Editorial

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3 pages, 180 KiB  
Editorial
Editorial-Special Issue “Macromolecular Self-Assembly Materials: From Modeling to Advanced Applications”
by Salvatore Magazù and Domenico Lombardo
Materials 2020, 13(6), 1458; https://doi.org/10.3390/ma13061458 - 23 Mar 2020
Cited by 1 | Viewed by 1652
Abstract
Materials self-assembly represents a key strategy for the design and fabrication of nanostructured systems and has become a fundamental approach for the construction of advanced nanomaterials [...] Full article

Research

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16 pages, 3956 KiB  
Article
Self-Assembly Processes in Hydrated Montmorillonite by FTIR Investigations
by Maria Teresa Caccamo, Giuseppe Mavilia, Letterio Mavilia, Domenico Lombardo and Salvatore Magazù
Materials 2020, 13(5), 1100; https://doi.org/10.3390/ma13051100 - 2 Mar 2020
Cited by 47 | Viewed by 3651
Abstract
Experimental findings obtained by FTIR and Raman spectroscopies on montmorillonite-water mixtures at three concentration values are presented. To get some insight into the hydrogen bond network of water within the montmorillonite network, FTIR and Raman spectra have been collected as a function of [...] Read more.
Experimental findings obtained by FTIR and Raman spectroscopies on montmorillonite-water mixtures at three concentration values are presented. To get some insight into the hydrogen bond network of water within the montmorillonite network, FTIR and Raman spectra have been collected as a function of time and then analyzed following two complementary approaches: An analysis of the intramolecular OH stretching mode in the spectral range of 2700–3900 cm−1 in terms of two Gaussian components, and an analysis of the same OH stretching mode by wavelet cross-correlation. The FTIR and Raman investigations have been carried as a function of time for a montmorillonite-water weight composition (wt%) of 20–80%, 25–75%, and 35–65%, until the dehydrated state where the samples appear as a homogeneous rigid layer of clay. In particular, for both the FTIR and Raman spectra, the decomposition of the OH stretching band into a “closed” and an “open” contribution and the spectral wavelet analysis allow us to extract quantitative information on the time behavior of the system water content. It emerges that, the total water contribution inside the montmorillonite structure decreases as a function of time. However, the relative weight of the ordered water contribution diminishes more rapidly while the relative weight of the disordered water contribution increases, indicating that a residual water content, characterized by a highly structural disorder, rests entrapped in the montmorillonite layer structure for a longer time. From the present study, it can be inferred that the montmorillonite dehydration process promotes the layer self-assembly. Full article
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14 pages, 765 KiB  
Article
Evidence of Structural Inhomogeneities in Hard-Soft Dimeric Particles without Attractive Interactions
by Gianmarco Munaò and Franz Saija
Materials 2020, 13(1), 84; https://doi.org/10.3390/ma13010084 - 23 Dec 2019
Cited by 2 | Viewed by 2234
Abstract
We perform Monte Carlo simulations of a simple hard-soft dimeric model constituted by two tangent spheres experiencing different interactions. Specifically, two hard spheres belonging to different dimers interact via a bare hard-core repulsion, whereas two soft spheres experience a softly repulsive Hertzian interaction. [...] Read more.
We perform Monte Carlo simulations of a simple hard-soft dimeric model constituted by two tangent spheres experiencing different interactions. Specifically, two hard spheres belonging to different dimers interact via a bare hard-core repulsion, whereas two soft spheres experience a softly repulsive Hertzian interaction. The cross correlations are soft as well. By exploring a wide range of temperatures and densities we investigate the capability of this model to document the existence of structural inhomogeneities indicating the possible onset of aggregates, even if no attraction is set. The fluid phase behavior is studied by analyzing structural and thermodynamical properties of the observed structures, in particular by computing radial distribution functions, structure factors and cluster size distributions. The numerical results are supported by integral equation theories of molecular liquids which allow for a finer and faster spanning of the temperature-density diagram. Our results may serve as a framework for a more systematic investigation of self-assembled structures of functionalized hard-soft dimers able to aggregate in a variety of structures widely oberved in colloidal dispersion. Full article
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14 pages, 4576 KiB  
Article
A Photoelectrochemical Study of Bioinspired 2-Styryl-1-Benzopyrylium Cations on TiO2 Nanoparticle Layer for Application in Dye-Sensitized Solar Cells
by Giuseppe Calogero, Ilaria Citro, Gioacchino Calandra Sebastianella, Gaetano Di Marco, Ana Marta Diniz, A. Jorge Parola and Fernando Pina
Materials 2019, 12(24), 4060; https://doi.org/10.3390/ma12244060 - 5 Dec 2019
Cited by 7 | Viewed by 2220
Abstract
In the present work, five 2-styryl-1-benzopyrylium salts and their relative self-assembly processes towards TiO2 nanocrystalline layers were evaluated as photosensitizers in dye-sensitized solar cells (DSSCs). Integration of these 2-styryl-1-benzopyrylium salts with the semiconductor allow for the performance of highly specific functions suitable [...] Read more.
In the present work, five 2-styryl-1-benzopyrylium salts and their relative self-assembly processes towards TiO2 nanocrystalline layers were evaluated as photosensitizers in dye-sensitized solar cells (DSSCs). Integration of these 2-styryl-1-benzopyrylium salts with the semiconductor allow for the performance of highly specific functions suitable for smart applications in material science. Spectroscopic and photoelectrochemical measurements conducted on these five bio-inspired dyes, in solution and upon adsorption onto titanium dioxide films, allowed detailed discussion of the anchoring ability of the different donor groups decorating the 2-styryl-1-benzopyrylium core and have demonstrated their ability as photosensitizers. Our results suggest that the introduction of a dimethylamino group in position 4′ of the 2-styryl-1-benzopyrylium skeleton can alter the conjugation of the molecule leading to larger absorption in the visible region and a stronger electron injection of the dye into the conduction band of TiO2. Moreover, our experimental data have been supported by theoretical calculations with the aim to study the energy of the excited states of the five compounds. In this specific case, the simulations reported contributed to better describe the properties of the compounds used and to help create the necessary basis for the design of new and targeted bio-inspired molecules. Full article
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13 pages, 5103 KiB  
Article
Preparation and Deep Characterization of Composite/Hybrid Multi-Scale and Multi-Domain Polymeric Microparticles
by Wei Yu, Nikunjkumar Visaveliya, Christophe A. Serra, J. Michael Köhler, Shukai Ding, Michel Bouquey, René Muller, Marc Schmutz and Isabelle Kraus
Materials 2019, 12(23), 3921; https://doi.org/10.3390/ma12233921 - 27 Nov 2019
Cited by 10 | Viewed by 2986
Abstract
Polymeric microparticles were produced following a three-step procedure involving (i) the production of an aqueous nanoemulsion of tri and monofunctional acrylate-based monomers droplets by an elongational-flow microemulsifier, (ii) the production of a nanosuspension upon the continuous-flow UV-initiated miniemulsion polymerization of the above nanoemulsion [...] Read more.
Polymeric microparticles were produced following a three-step procedure involving (i) the production of an aqueous nanoemulsion of tri and monofunctional acrylate-based monomers droplets by an elongational-flow microemulsifier, (ii) the production of a nanosuspension upon the continuous-flow UV-initiated miniemulsion polymerization of the above nanoemulsion and (iii) the production of core-shell polymeric microparticles by means of a microfluidic capillaries-based double droplets generator; the core phase was composed of the above nanosuspension admixed with a water-soluble monomer and gold salt, the shell phase comprised a trifunctional monomer, diethylene glycol and a silver salt; both phases were photopolymerized on-the-fly upon droplet formation. Resulting microparticles were extensively analyzed by energy dispersive X-rays spectrometry and scanning electron microscopy to reveal the core-shell morphology, the presence of silver nanoparticles in the shell, organic nanoparticles in the core but failed to reveal the presence of the gold nanoparticles in the core presumably due to their too small size (c.a. 2.5 nm). Nevertheless, the reddish appearance of the as such prepared polymer microparticles emphasized that this three-step procedure allowed the easy elaboration of composite/hybrid multi-scale and multi-domain polymeric microparticles. Full article
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Review

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42 pages, 16087 KiB  
Review
Self-Assembly of Organic Nanomaterials and Biomaterials: The Bottom-Up Approach for Functional Nanostructures Formation and Advanced Applications
by Domenico Lombardo, Pietro Calandra, Luigi Pasqua and Salvatore Magazù
Materials 2020, 13(5), 1048; https://doi.org/10.3390/ma13051048 - 26 Feb 2020
Cited by 97 | Viewed by 11139
Abstract
In this paper, we survey recent advances in the self-assembly processes of novel functional platforms for nanomaterials and biomaterials applications. We provide an organized overview, by analyzing the main factors that influence the formation of organic nanostructured systems, while putting into evidence the [...] Read more.
In this paper, we survey recent advances in the self-assembly processes of novel functional platforms for nanomaterials and biomaterials applications. We provide an organized overview, by analyzing the main factors that influence the formation of organic nanostructured systems, while putting into evidence the main challenges, limitations and emerging approaches in the various fields of nanotechology and biotechnology. We outline how the building blocks properties, the mutual and cooperative interactions, as well as the initial spatial configuration (and environment conditions) play a fundamental role in the construction of efficient nanostructured materials with desired functional properties. The insertion of functional endgroups (such as polymers, peptides or DNA) within the nanostructured units has enormously increased the complexity of morphologies and functions that can be designed in the fabrication of bio-inspired materials capable of mimicking biological activity. However, unwanted or uncontrollable effects originating from unexpected thermodynamic perturbations or complex cooperative interactions interfere at the molecular level with the designed assembly process. Correction and harmonization of unwanted processes is one of the major challenges of the next decades and requires a deeper knowledge and understanding of the key factors that drive the formation of nanomaterials. Self-assembly of nanomaterials still remains a central topic of current research located at the interface between material science and engineering, biotechnology and nanomedicine, and it will continue to stimulate the renewed interest of biologist, physicists and materials engineers by combining the principles of molecular self-assembly with the concept of supramolecular chemistry. Full article
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