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Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials

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

Deadline for manuscript submissions: closed (15 August 2020) | Viewed by 46021

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Dr. Andrei Rotaru

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Guest Editor

1. Department of Biology and Environmental Engineering, University of Craiova, Str. A.I. Cuza, Nr. 13, 200585 Craiova, Romania
2. Institute of Physical Chemistry "Ilie Murgulescu", Romanian Academy, Department of Chemical Thermodynamics, Splaiul Independentei, Nr. 202, 060021 Bucharest, Romania
Interests: physical chemistry of materials, thermophysical properties of solids, thermal analysis and calorimetry, kinetics & thermodynamics of heterogeneous processes; diffusional properties; dynamic processes in relaxors; structure-properties relation in electroceramics; thin films of soft molecular compounds

Dr. Maria Dinescu

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Guest Editor

National Institute for Laser, Plasma & Radiation Physics, Atomistilor 409, 077125 Magurele, Romania
Interests: pulsed laser deposition; oxide thin films; heterostructures; matrix assisted pulsed laser evaporation; laser induced forward transfer
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Special Issue Information

Dear Colleagues,

Molecular and soft materials have received great attention due to their novel applications as minute functional materials, often for large-scale manufacturing and in the high-tech industries. Compounds such as liquid crystals, organic fuel cells, organic transistors, coloring indicators, polymeric coatings, cation-containing biologically active inorganic complexes and organometallic materials, composite nanomaterials, fine-coated metals, core–shell nanostructures, catalysts, active bio(macro)molecules, etc., are interesting and valuable candidates. Most of these applications are meaningful in their deposited or dispersed forms, on substrates or over surfaces.

Besides these applications, the fabrication and characterization of surfaces, interfaces, coatings, thin films, nanostructures, functionalized surfaces and composites with a high specific area are key steps in materials science and engineering. Both physical and chemical deposition techniques are employed for coatings and thin films, while usually different wet-chemistry steps and pyrolysis/combustion methods are used in the synthesis of composite materials and functional porous media.

The present Special Issue entitled “Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials”, will gather and publish original articles and review papers regarding the synthesis, functionalization, characterization and application of surfaces, interfaces, coatings and nanostructures of molecular and soft materials with outstanding properties, on the following topics:

General aspects of surfaces and interfaces
Physical and chemical deposition techniques
Thin films and coatings by various deposition techniques
Transfer of soft materials structures by advanced techniques
Imagistics and thermal characterization of flat surfaces
Molecular materials and soft materials
Inorganic complexes, organic compounds and polymers
Composites of porous systems with soft materials
Functionalization of surfaces and fabrication of composite materials with a high specific area
Characterization of porous media and applications
Advanced molecular materials attached to nanotubes and as functional nanomaterials
Nanostructures of soft molecular materials
Nanocomposites and intercalated minute materials
Coated and encapsulated particles, and carbonaceous materials
Long-range structuring and self-assembly of molecular materials
Physical chemistry of colloidal systems and applications
Bio(macro)molecular films and surfaces
Interactions of bio(macro)molecules with surfaces and skin medical remediation

Assoc. Prof. Dr. Andrei Rotaru
Prof. Dr. Maria Dinescu
Guest Editors

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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

Surfaces and interfaces
Thin films and coatings
Soft materials and molecular materials
Chemical deposition techniques
Physical deposition and transfer techniques
MAPLE (matrix-assisted pulsed laser evaporation)
LIFT (laser-induced forward transfer)
Porous materials and composites
Nanomaterials, nanotubes, nanostructures
Colloids and bio(macro)molecules

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Published Papers (11 papers)

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Research

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14 pages, 6464 KiB

Open AccessArticle

The Effect of Moisture on the Adhesion Energy and Nanostructure of Asphalt-Aggregate Interface System Using Molecular Dynamics Simulation

by Wentian Cui, Wenke Huang, Zhicheng Xiao, Jiawen Xie, Bei Hu, Xu Cai and Kuanghuai Wu

Molecules 2020, 25(18), 4165; https://doi.org/10.3390/molecules25184165 - 11 Sep 2020

Cited by 21 | Viewed by 3074

Abstract

In this work, the influences of moisture intruded into the asphalt-aggregate interface have been investigated at the atomistic scale. The molecular interactions of asphalt with limestone and granite were studied using molecular dynamics (MD) simulations and the mineral surface components of limestone and granite were detected using the hyperspectral image technique. Relative concentration and radial distribution function (RDF) were employed for the characterization of asphalt component aggregations on aggregates surface. Adhesion work and debonding energy were also evaluated to investigate interface energy variations in asphalt-aggregate systems. MD results showed that the presence of interfacial moisture modified asphalt nanostructure and affected the aggregation state and distribution characteristics of asphalt components near aggregate surface. The study also demonstrated that the external moisture that intruded into the interface of the asphalt-aggregate system can decrease the concentration distribution of the asphalt components with powerful polarity on aggregate surface, reduce the adhesion works of the asphalt-aggregate interface, and decline the water damage resistance of asphalt mixture. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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14 pages, 3200 KiB

Open AccessArticle

Stearic Acid/Layered Double Hydroxides Composite Thin Films Deposited by Combined Laser Techniques

by Ruxandra Birjega, Andreea Matei, Valentina Marascu, Angela Vlad, Maria Daniela Ionita, Maria Dinescu, Rodica Zăvoianu and Mihai Cosmin Corobea

Molecules 2020, 25(18), 4097; https://doi.org/10.3390/molecules25184097 - 8 Sep 2020

Cited by 3 | Viewed by 2772

Abstract

We report on the investigation of stearic acid-layered double hydroxide (LDH) composite films, with controlled wettability capabilities, deposited by a combined pulsed laser deposition (PLD)-matrix-assisted pulsed laser evaporation (MAPLE) system. Two pulsed lasers working in IR or UV were used for experiments, allowing the use of proper deposition parameters (wavelength, laser fluence, repetition rate) for each organic and inorganic component material. We have studied the time stability and wettability properties of the films and we have seen that the morphology of the surface has a low effect on the wettability of the surfaces. The obtained composite films consist in stearic acid aggregates in LDH structure, exhibiting a shift to hydrophobicity after 36 months of storage. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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11 pages, 3397 KiB

Open AccessArticle

Adsorption Capacity of Vitamin B₁₂ and Creatinine on Highly-Mesoporous Activated Carbons Obtained from Lignocellulosic Raw Materials

by Tudor Lupaşcu, Oleg Petuhov, Nina Ţîmbaliuc, Silvia Cibotaru and Andrei Rotaru

Molecules 2020, 25(13), 3095; https://doi.org/10.3390/molecules25133095 - 7 Jul 2020

Cited by 16 | Viewed by 3397

Abstract

Enterosorbents are widely-used materials for human body detoxification, which function by immobilizing and eliminating endogenous and exogenous toxins. Here, activated carbons, obtained from the lignocellulosic raw vegetal materials of indigenous provenance, have been studied. Walnut shell and wood from local species of nuts and apple-trees were carbonized, and further activated at high temperatures with water vapors in a rotary kiln. A second activation was carried out, in a fluidized bed reactor, but for shorter times. The textural properties of the samples were determined from the adsorption isotherms of nitrogen at 77 K, allowing the obtaining of highly mesoporous materials, while the adsorption capacity permitted an essential rise of six to seven times in the maximal adsorption values of the metabolites, which was determined by the reactivation process. A kinetic study of vitamin B₁₂ and creatinine immobilization was performed, the optimal immobilization time for the apple-tree wood reactivated carbons being 2 times longer than for those originating from walnut shells. An additional investigation was also performed in specific conditions that simulate the real environment of immobilization: the temperature of a febrile human body (at the temperature T = 38 °C) and the characteristic acidity of the urinary tract and stomach (at the pH of 5.68 and 2.53, respectively). The activated carbonic adsorbents studied here, together with the results of the immobilization studies, show that these procedures can conduct a good incorporation of some endogenous metabolic products, such as vitamin B₁₂ and creatinine, therefore presenting a good opportunity for their use as forthcoming commercial enterosorbents. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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16 pages, 692 KiB

Open AccessArticle

Response of Pseudokirchneriella subcapitata in Free and Alginate Immobilized Cells to Heavy Metals Toxicity

by Zaki M. Al-Hasawi, Mohammad I. Abdel-Hamid, Adel W. Almutairi and Hussein E. Touliabah

Molecules 2020, 25(12), 2847; https://doi.org/10.3390/molecules25122847 - 19 Jun 2020

Cited by 23 | Viewed by 3459

Abstract

Effects of 12 heavy metals on growth of free and alginate-immobilized cells of the alga Pseudokirchneriella subcapitata were investigated. The tested metals ions include Al, As, Cd, Co, Cr, Cu, Hg, Se, Ni, Pb, Sr, and Zn. Toxicity values (EC₅₀) were calculated by graphical interpolation from dose-response curves. The highest to the lowest toxic metals are in the order Cd > Co > Hg > Cu > Ni > Zn > Cr > Al > Se > As > Pb > Sr. The lowest metal concentration (mg L⁻¹) inhibiting 50% (EC₅₀) of algal growth of free and immobilized (values in parentheses) algal cells were, 0.018 (0.09) for Cd, 0.03 (0.06) for Co, 0.039 (0.06) for Hg, 0.048 (0.050) for Cu, 0.055 (0.3) for Ni, 0.08 (0.1) for Zn, 0.2 (0.3) for Cr, 0.75 (1.8) for Al, 1.2 (1.4) for Se, 3.0 (4.0) for As, 3.3 (5.0) for Pb, and 160 (180) for Sr. Free and immobilized cultures showed similar responses to Cu and Se. The free cells were more sensitive than the immobilized ones. Accordingly, the toxicity (EC₅₀) of heavy metals derived only form immobilized algal cells might by questionable. The study suggests that batteries of alginate-immobilized algae can efficiently replace free algae for the bio-removal of heavy metals. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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17 pages, 3205 KiB

Open AccessArticle

Induced Hydrophilicity and In Vitro Preliminary Osteoblast Response of Polyvinylidene Fluoride (PVDF) Coatings Obtained via MAPLE Deposition and Subsequent Thermal Treatment

by Luminita Nicoleta Dumitrescu, Patricia Neacsu, Madalina G. Necula, Anca Bonciu, Valentina Marascu, Anisoara Cimpean, Antoniu Moldovan, Andrei Rotaru, Valentina Dinca and Maria Dinescu

Molecules 2020, 25(3), 582; https://doi.org/10.3390/molecules25030582 - 29 Jan 2020

Cited by 22 | Viewed by 3757

Abstract

Recent advancements in biomedicine have focused on designing novel and stable interfaces that can drive a specific cellular response toward the requirements of medical devices or implants. Among these, in recent years, electroactive polymers (i.e., polyvinylidene fluoride or PVDF) have caught the attention within the biomedical applications sector, due to their insolubility, stability in biological media, in vitro and in vivo non-toxicity, or even piezoelectric properties. However, the main disadvantage of PVDF-based bio-interfaces is related to the absence of the functional groups on the fluoropolymer and their hydrophobic character leading to a deficiency of cell adhesion and proliferation. This work was aimed at obtaining hydrophilic functional PVDF polymer coatings by using, for the first time, the one-step, matrix-assisted pulsed evaporation (MAPLE) method, testing the need of a post-deposition thermal treatment and analyzing their preliminary capacity to support MC3T3-E1 pre-osteoblast cell survival. As osteoblast cells are known to prefer rough surfaces, MAPLE deposition parameters were studied for obtaining coatings with roughness of tens to hundreds of nm, while maintaining the chemical properties similar to those of the pristine material. The in vitro studies indicated that all surfaces supported the survival of viable osteoblasts with active metabolisms, similar to the “control” sample, with no major differences regarding the thermally treated materials; this eliminates the need to use a secondary step for obtaining hydrophilic PVDF coatings. The physical-chemical characteristics of the thin films, along with the in vitro analyses, suggest that MAPLE is an adequate technique for fabricating PVDF thin films for further bio-applications. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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13 pages, 2126 KiB

Open AccessArticle

Poly (Vinyl Butyral-Co-Vinyl Alcohol-Co-Vinyl Acetate) Coating Performance on Copper Corrosion in Saline Environment

by Adriana Samide, Claudia Merisanu, Bogdan Tutunaru and Gabriela Eugenia Iacobescu

Molecules 2020, 25(3), 439; https://doi.org/10.3390/molecules25030439 - 21 Jan 2020

Cited by 11 | Viewed by 3894

Abstract

Poly (vinyl butyral-co-vinyl alcohol-co-vinyl acetate) named further PVBA was investigated as a protective coating for copper corrosion in 0.9% NaCl solution using electrochemical measurements such as, electrochemical impedance spectroscopy (EIS) and potentiodynamic polarization associated with atomic force microscopy (AFM). The PVBA coating on the copper surface (Cu-PVBA) was modeled in methanol containing PVBA. Its inhibitory properties against corrosion was comparatively discussed with those of the copper sample treated in methanol without polymer (Cu-Me) and of untreated sample (standard copper). A protective performance of PVBA coating of 80% was computed from electrochemical measurements, for copper corrosion in NaCl solution. Moreover, AFM images designed a specific surface morphology of coated surface with PVBA, clearly highlighting a polymer film adsorbed on the copper surface, which presents certain deterioration after corrosion, but the metal surface was not significantly affected compared to those of untreated samples or treated in methanol, in the absence of PVBA. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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21 pages, 7822 KiB

Open AccessArticle

Difference Analysis of Gas Molecules Diffusion Behavior in Natural Ester and Mineral Oil Based on Molecular Dynamic Simulation

by Wenyu Ye, Jian Hao, Yufeng Chen, Mengzhao Zhu, Zhen Pan and Fei Hou

Molecules 2019, 24(24), 4463; https://doi.org/10.3390/molecules24244463 - 5 Dec 2019

Cited by 31 | Viewed by 4244

Abstract

Natural ester, as a new environmentally green insulating oil, has been widely used in transformer. In an oil-immersed transformer, the normal aging, thermal failure, and discharge failure could easily lead to the decomposition of the oil-paper insulation system and produce different kinds of gases. Studying gas dissolution in natural ester and mineral oil could provide assistance in applying criteria to make a diagnosis of different kinds of faults in the transformer. In this paper, the molecular dynamics method was used to investigate the diffusion behavior of seven fault characteristic gases (including H₂, CO, CH₄, C₂H₂, CO₂, C₂H₄, C₂H₆) in natural ester and mineral oil. The simulation parameters of free volume, interaction energy, mean square displacement, and diffusion coefficient were compared between the natural ester and mineral oil. Meanwhile, the influence of temperature on the diffusion of gas molecules in two kinds of oils was also analyzed. Results showed that the free volume, the interaction energy, and the relative molecular mass of gas molecules were the factors influenced by the diffusion of gas molecules in natural ester and mineral oil. The order of the diffusion coefficients of gas molecules in natural ester was as follows: H₂ > CH₄ > CO > C₂H₂ > C₂H₄ > CO₂ > C₂H₆ and that in mineral oil was as follows: H₂ > CH₄ > CO> C₂H₂ > C₂ H₄ > C₂H₆ > CO₂. By comparing the diffusion behavior of gas molecules in natural ester and mineral oil, it was found that the smaller free volume and higher interaction energy of gas molecules in natural ester were the major reasons for the gas molecules to be more difficult to diffuse in natural ester. The rising temperature could enhance the free volume and reduce the interaction energy between gas molecules and oil. The diffusion coefficient of gas molecules increased exponentially with the follow of temperature. However, the temperature didn’t affect the ordering of diffusion coefficient, free volume, and interaction energy of gas molecules in natural ester and mineral oil. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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11 pages, 2772 KiB

Open AccessArticle

Management of Exciton for Highly-Efficient Hybrid White Organic Light-Emitting Diodes with a Non-Doped Blue Emissive Layer

by Wei Luo, Xing Chen, Shuang-Qiao Sun, Yi-Jie Zhang, Tong-Tong Wang, Liang-Sheng Liao and Man-Keung Fung

Molecules 2019, 24(22), 4046; https://doi.org/10.3390/molecules24224046 - 8 Nov 2019

Cited by 1 | Viewed by 3611

Abstract

Hybrid white organic light-emitting diodes (WOLEDs) have drawn great attention both for display and solid-state lighting purposes because of the combined advantages of desirable stability of fluorescent dyes and high efficiency of phosphorescent materials. However, in most WOLEDs, obtaining high efficiency often requires complex device structures. Herein, we achieved high-efficiency hybrid WOLEDs using a simple but efficacious structure, which included a non-doped blue emissive layer (EML) to separate the exciton recombination zone from the light emission region. After optimization of the device structure, the WOLEDs showed a maximum power efficiency (PE), current efficiency (CE), and external quantum efficiency (EQE) of 82.3 lm/W, 70.0 cd/A, and 22.2%, respectively. Our results presented here provided a new option for promoting simple-structure hybrid WOLEDs with superior performance. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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13 pages, 4146 KiB

Open AccessArticle

Molecular Dynamics Simulation of Distribution and Diffusion Behaviour of Oil–Water Interfaces

by Chengbin Zhang, Hanhui Dai, Pengfei Lu, Liangyu Wu, Bo Zhou and Cheng Yu

Molecules 2019, 24(10), 1905; https://doi.org/10.3390/molecules24101905 - 17 May 2019

Cited by 23 | Viewed by 4272

Abstract

The distribution and diffusion behaviors of microscopic particles at fluorobenzene–water and pentanol–water interfaces are investigated using molecular dynamics simulation. The influences of Na⁺/Cl⁻ ions and the steric effects of organic molecules are examined. The concentration distributions of different species, the orientations of oil molecules at the interface, and oil–water interface morphology as well as the diffusion behaviors of water molecules are explored and analyzed. The results indicate that a few fluorobenzene molecules move into the water phase influenced by Na⁺/Cl⁻ ions, while the pentanol molecules at the interface prefer orientating their hydrophilic groups toward the water phase due to their large size. The water molecules more easily burst into the pentanol phase with larger molecular spaces. As the concentration of ions in the water phase increases, more water molecules enter into the pentanol molecules, leading to larger interface roughness and interface thickness. In addition, a lower diffusion coefficient for water molecules at the fluorobenzene–water interface are observed when introducing Na⁺/Cl⁻ ions in the water phase, while for the pentanol–water system, the mobility of interfacial water molecules are enhanced with less ions and inhibited with more ions. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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Review

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35 pages, 5230 KiB

Open AccessReview

Molecular Crystallization Inhibitors for Salt Damage Control in Porous Materials: An Overview

by Maria Paola Bracciale, Svetlana Sammut, JoAnn Cassar, Maria Laura Santarelli and Assunta Marrocchi

Molecules 2020, 25(8), 1873; https://doi.org/10.3390/molecules25081873 - 18 Apr 2020

Cited by 20 | Viewed by 7104

Abstract

The use of inhibition chemicals holds the prospect of an efficient strategy to control crystallization in porous materials, thereby potentially contributing to the prevention or mitigation of the salt decay phenomenon in modern as well as historical building materials in a more sustainable manner. In this review, we first provide an essential background on the mechanism of salt crystallization and on the factors influencing this phenomenon; next, we illustrate the mechanism at the basis of the action of crystal growth inhibitors, and critically discuss the major advances in the development of different families of inhibitors, particularly focusing on their influence on salt transport and crystallization within the structure of porous media. Specifically, correlations between the crystallization inhibition processes in porous materials and variables, such as porous substrate composition and properties, contaminant salt type and concentrations, microclimatic conditions, inhibiting solution concentration and properties, and application methods, will be highlighted. Environmental aspects, limitations, and problems associated with some inhibition chemicals are also taken into account. Finally, a survey and a discussion on the most representative experimental techniques and instrumentation available to assess qualitatively and quantitatively the inhibitor effectiveness, as well as recently developed modelling tools are given out. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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26 pages, 3885 KiB

Open AccessReview

Clay Composites for Thermal Energy Storage: A Review

by Denis V. Voronin, Evgenii Ivanov, Pavel Gushchin, Rawil Fakhrullin and Vladimir Vinokurov

Molecules 2020, 25(7), 1504; https://doi.org/10.3390/molecules25071504 - 26 Mar 2020

Cited by 33 | Viewed by 5724

Abstract

The development of novel materials and approaches for effective energy consumption and the employment of renewable energy sources is one of the current trends in modern material science. With this respect, the number of researches is focused on the effective harvesting and storage of solar energy for various applications. Phase change materials (PCMs) are known to be able to store thermal energy of the sunlight due to adsorption and release of latent heat through reversible phase transitions. Therefore, PCMs are promising as functional additives to construction materials and paints for advanced thermoregulation in building and industry. However, bare PCMs have limited practical applications. Organic PCMs like paraffins suffer from material leakage when undergoing in a liquid state while inorganic ones like salt hydrates lack long-term stability after multiple phase transitions. To avoid this, the loading of PCMs in porous matrices are intensively studied along with the thermal properties of the resulted composites. The loading of PCMs in microcontainers of natural porous or layered clay materials appears as a simple and cost-effective method of encapsulation significantly improving the shape and cyclic stability of PCMs. Additionally, the inclusion of functional clay containers into construction materials allows for improving their mechanical and flame-retardant properties. This article summarizes the recent progress in the preparation of composites based on PCM-loaded clay microcontainers along with their future perspectives as functional additives in thermo-regulating materials. Full article

(This article belongs to the Special Issue Surfaces, Interfaces, Coatings and Nanostructures of Molecular and Soft Materials)

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