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Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga

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

Deadline for manuscript submissions: closed (30 April 2022) | Viewed by 34914

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Dr. Gaulthier Rydzek

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ICGM, CNRS, ENSCM, University of Montpellier, Montpellier, France
Interests: polyelectrolyte complexes; self-assembly; block copolymer; thin films; electro-deposition; electrosynthesis
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Prof. Dr. Qingmin Ji

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Herbert Gleiter Institute of Nanoscience, Nanjing University of Science and technology (PRC), Nanjing, China
Interests: mesoporous nanomaterials for catalysis and energy storage

Prof. Dr. Fabien Grasset

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CNRS, ISCR UMR 6226, University of Rennes 1, 263 Avenue du Général Leclerc, 35042 Rennes, France
Interests: nanoparticle and nanocomposite synthesis; processing and characterization; sol–gel; microemulsion; zinc oxide; magnetic iron oxides; functional SiO₂; thin film; energy; biomedical
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Dr. Amir Pakdel

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Department of Mechanical, Manufacturing and Biomedical Engineering, Trinity College Dublin, The University of Dublin, D02 PN40 Dublin, Ireland
Interests: 1D/2D nanomaterials; composites; surfaces and interfaces; energy and environment; thermoelectrics; batteries
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Special Issue Information

Dear Colleagues,

Molecules is very pleased to host a Special Issue honoring Prof. Katsuhiko Ariga for his outstanding achievements in advancing nanomaterials design and nanoarchitectonics for basic science and applied functional materials.

Complementing his curiosity with hard work, Prof. Ariga has always valued thinking differently and demonstrating unexpected concepts. His boundless creative and highly collaborative approach to science have led Prof. Ariga to publish over 700 publications to date, in turn leading to more than 40,000 citations, numerous books and patents, as well as a worldwide reputation as a preeminent scholar.

After obtaining his PhD degree from Tokyo Institute of Technology in 1990, Prof. Ariga worked at the University of Texas at Austin, at Japan’s JST, and at Nara Institute of Technology. Since 2004, he has led the Supermolecules Group at the National Institute for Materials Science (NIMS) and served as a principal investigator of the World Premier International (WPI) Research Centre for Materials Nanoarchitectonics (MANA). In 2017, he was also appointed as a professor of The University of Tokyo.

Prof. Ariga’s many accomplishments include the design and development of supramolecular assemblies enabling functional materials with target properties such as as stimuli-responsive colloids, enhanced catalysts, taylored sensors, electro-active interfaces, nanostructured biomaterials, and molecular machines. In recent years, Prof. Ariga has made a decisive contribution to the emergence of nanoarchitectonics, a technology enabling nanocreation and programmed nano-organization of highly functional materials based on nanosized structural units such as groups of atoms or molecules.

Molecules is inviting papers covering innovative scientific/technical developments, reviews, case studies, and analytical/assessment articles from all relevant disciplines of nanomaterials design and nanoarchitectonics of functional materials.

Prof. Dr. Gaulthier Rydzek
Prof. Dr. Qingmin Ji
Prof. Dr. Fabien Grasset
Prof. Dr. Amir Pakdel
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. 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

Nanoarchitectonics
Supramolecular assemblies
Biomaterials
Stimuli-responsive materials
Nanostructured materials
Materials and interfaces for energy conversion and storage

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Published Papers (8 papers)

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Research

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19 pages, 3715 KiB

Open AccessArticle

Optimization of Nanohybrid Biosensors Based on Electro-Crosslinked Tannic Acid Capped Nanoparticles/Enzyme

by Rémy Savin, Christian Blanck, Nour-Ouda Benzaamia and Fouzia Boulmedais

Molecules 2022, 27(10), 3309; https://doi.org/10.3390/molecules27103309 - 21 May 2022

Cited by 5 | Viewed by 1755

Abstract

Enzymes/Nanoparticles (NPs) bioconjugates are massively used nowadays to develop thin films for optical and electrochemical biosensors. Nevertheless, their full characterization as a thin coating onto electrodes remains little discussed, in particular the influence of NPs size and enzyme/NPs ratio used in the electrodeposition solution. In this study, GOx (160 kDa) and HRP (44 kDa) were used in association with tannic acid capped gold NPs (a series with sizes from 7 to 40 nm) to electrodeposit biosensor coatings, sensitive towards glucose and H₂O₂, respectively. The electrodeposition process was based on a mussel-inspired electro-crosslinking between gallol moieties of tannic acid (at the surface of NPs) and amine moieties of the enzymes. On one hand, the sensitivity of the GOx/NPs coatings depends strongly on the NP size and the enzyme/NPs molar ratio of the electrodeposition solution. An optimal sensitivity was obtained by electrodeposition of 11 nm NPs at a GOx/NPs molar ratio close to the theoretical value of the enzyme monolayer. On the other hand, a modest influence of the NPs size was found on the sensitivity in the case of the electrodeposited HRP/NPs coatings, reaching a plateau at the HRP/NPs molar ratio close to the value of the theoretical enzyme monolayer. In both cases, the enzyme/NPs molar ratio played a role in the sensitivity. To fully understand the parameters driving the biosensor sensitivity, a comprehensive evaluation of the colloidal state of the bioconjugates is proposed here. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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18 pages, 6318 KiB

Open AccessFeature PaperArticle

Molecular Transport within Polymer Brushes: A FRET View at Aqueous Interfaces

by Quinn A. Besford, Simon Schubotz, Soosang Chae, Ayşe B. Özdabak Sert, Alessia C. G. Weiss, Günter K. Auernhammer, Petra Uhlmann, José Paulo S. Farinha and Andreas Fery

Molecules 2022, 27(9), 3043; https://doi.org/10.3390/molecules27093043 - 9 May 2022

Cited by 7 | Viewed by 2636

Abstract

Molecular permeability through polymer brush chains is implicated in surface lubrication, wettability, and solute capture and release. Probing molecular transport through polymer brushes can reveal information on the polymer nanostructure, with a permeability that is dependent on chain conformation and grafting density. Herein, we introduce a brush system to study the molecular transport of fluorophores from an aqueous droplet into the external “dry” polymer brush with the vapour phase above. The brushes consist of a random copolymer of N-isopropylacrylamide and a Förster resonance energy transfer (FRET) donor-labelled monomer, forming ultrathin brush architectures of about 35 nm in solvated height. Aqueous droplets containing a separate FRET acceptor are placed onto the surfaces, with FRET monitored spatially around the 3-phase contact line. FRET is used to monitor the transport from the droplet to the outside brush, and the changing internal distributions with time as the droplets prepare to recede. This reveals information on the dynamics and distances involved in the molecular transport of the FRET acceptor towards and away from the droplet contact line, which are strongly dependent on the relative humidity of the system. We anticipate our system to be extremely useful for studying lubrication dynamics and surface droplet wettability processes. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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12 pages, 2856 KiB

Open AccessArticle

Oligomer Sensor Nanoarchitectonics for “Turn-On” Fluorescence Detection of Cholesterol at the Nanomolar Level

by Vedant Joshi, Sameer Hussain, Sachin Dua, Nishtha Arora, Sajjad Husain Mir, Gaulthier Rydzek and Thangaraj Senthilkumar

Molecules 2022, 27(9), 2856; https://doi.org/10.3390/molecules27092856 - 30 Apr 2022

Cited by 7 | Viewed by 2074

Abstract

Sensitive and rapid monitoring of cholesterol levels in the human body are highly desirable as they are directly related to the diagnosis of cardiovascular diseases. By using the nanoarchitectonic approach, a novel fluorescent conjugated oligofluorene (OFP-CD) functionalized with β-cyclodextrin (β-CD) was assembled for “Turn-On” fluorescence sensing of cholesterol. The appended β-CD units in OFP-CD enabled the forming of host-guest complexes with dabsyl chloride moieties in water, resulting in fluorescence quenching of the oligofluorene through intermolecular energy transfer. In the presence of cholesterol molecules, a more favorable host-guest complex with stoichiometry 1 cholesterol: 2 β-CD units was formed, replacing dabsyl chloride in β-CD’s cavities. This process resulted in fluorescence recovery of OFP-CD, owing to disruption of energy transfer. The potential of this nanoarchitectonic system for “Turn-On” sensing of cholesterol was extensively studied by fluorescence spectroscopy. The high selectivity of the sensor for cholesterol was demonstrated using biologically relevant interfering compounds, such as carbohydrates, amino acids, metal ions, and anions. The detection limit (LOD value) was as low as 68 nM, affirming the high sensitivity of the current system. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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16 pages, 2682 KiB

Open AccessArticle

Ultrastable Conjugated Microporous Polymers Containing Benzobisthiadiazole and Pyrene Building Blocks for Energy Storage Applications

by Mohamed Gamal Mohamed, Tharwat Hassan Mansoure, Maha Mohamed Samy, Yasuno Takashi, Ahmed A. K. Mohammed, Tansir Ahamad, Saad M. Alshehri, Jeonghun Kim, Babasaheb M. Matsagar, Kevin C.-W. Wu and Shiao-Wei Kuo

Molecules 2022, 27(6), 2025; https://doi.org/10.3390/molecules27062025 - 21 Mar 2022

Cited by 40 | Viewed by 4311

Abstract

In recent years, conjugated microporous polymers (CMPs) have become important precursors for environmental and energy applications, compared with inorganic electrode materials, due to their ease of preparation, facile charge storage process, π-conjugated structures, relatively high thermal and chemical stability, abundance in nature, and high surface areas. Therefore, in this study, we designed and prepared new benzobisthiadiazole (BBT)-linked CMPs (BBT–CMPs) using a simple Sonogashira couplings reaction by reaction of 4,8-dibromobenzo(1,2-c;4,5-c′)bis(1,2,5)thiadiazole (BBT–Br₂) with ethynyl derivatives of triphenylamine (TPA-T), pyrene (Py-T), and tetraphenylethene (TPE-T), respectively, to afford TPA–BBT–CMP, Py–BBT–CMP, and TPE–BBT–CMP. The chemical structure and properties of BBT–CMPs such as surface areas, pore size, surface morphologies, and thermal stability using different measurements were discussed in detail. Among the studied BBT–CMPs, we revealed that TPE–BBT–CMP displayed high degradation temperature, up to 340 °C, with high char yield and regular, aggregated sphere based on thermogravimetric analysis (TGA) and scanning electron microscopy (SEM), respectively. Furthermore, the Py–BBT–CMP as organic electrode showed an outstanding specific capacitance of 228 F g⁻¹ and superior capacitance stability of 93.2% (over 2000 cycles). Based on theoretical results, an important role of BBT–CMPs, due to their electronic structure, was revealed to be enhancing the charge storage. Furthermore, all three CMP polymers featured a high conjugation system, leading to improved electron conduction and small bandgaps. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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19 pages, 3669 KiB

Open AccessArticle

Zirconium-Based Metal Organic Frameworks for the Capture of Carbon Dioxide and Ethanol Vapour. A Comparative Study

by Meryem Saidi, Phuoc Hoang Ho, Pankaj Yadav, Fabrice Salles, Clarence Charnay, Luc Girard, Leila Boukli-Hacene and Philippe Trens

Molecules 2021, 26(24), 7620; https://doi.org/10.3390/molecules26247620 - 15 Dec 2021

Cited by 10 | Viewed by 4310

Abstract

This paper reports on the comparison of three zirconium-based metal organic frameworks (MOFs) for the capture of carbon dioxide and ethanol vapour at ambient conditions. In terms of efficiency, two parameters were evaluated by experimental and modeling means, namely the nature of the ligands and the size of the cavities. We demonstrated that amongst three Zr-based MOFs, MIP-202 has the highest affinity for CO₂ (−50 kJ·mol⁻¹ at low coverage against around −20 kJ·mol⁻¹ for MOF-801 and Muc Zr MOF), which could be related to the presence of amino functions borne by its aspartic acid ligands as well as the presence of extra-framework anions. On the other side, regardless of the ligand size, these three materials were able to adsorb similar amounts of carbon dioxide at 1 atm (between 2 and 2.5 µmol·m⁻² at 298 K). These experimental findings were consistent with modeling studies, despite chemisorption effects, which could not be taken into consideration by classical Monte Carlo simulations. Ethanol adsorption confirmed these results, higher enthalpies being found at low coverage for the three materials because of stronger van der Waals interactions. Two distinct sorption processes were proposed in the case of MIP-202 to explain the shape of the enthalpic profiles. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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32 pages, 8833 KiB

Open AccessReview

Weak Polyelectrolytes as Nanoarchitectonic Design Tools for Functional Materials: A Review of Recent Achievements

by Noelia M. Sanchez-Ballester, Flavien Sciortino, Sajjad Husain Mir and Gaulthier Rydzek

Molecules 2022, 27(10), 3263; https://doi.org/10.3390/molecules27103263 - 19 May 2022

Cited by 11 | Viewed by 3121

Abstract

The ionization degree, charge density, and conformation of weak polyelectrolytes can be adjusted through adjusting the pH and ionic strength stimuli. Such polymers thus offer a range of reversible interactions, including electrostatic complexation, H-bonding, and hydrophobic interactions, which position weak polyelectrolytes as key nano-units for the design of dynamic systems with precise structures, compositions, and responses to stimuli. The purpose of this review article is to discuss recent examples of nanoarchitectonic systems and applications that use weak polyelectrolytes as smart components. Surface platforms (electrodeposited films, brushes), multilayers (coatings and capsules), processed polyelectrolyte complexes (gels and membranes), and pharmaceutical vectors from both synthetic or natural-type weak polyelectrolytes are discussed. Finally, the increasing significance of block copolymers with weak polyion blocks is discussed with respect to the design of nanovectors by micellization and film/membrane nanopatterning via phase separation. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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35 pages, 10855 KiB

Open AccessReview

Progress in Molecular Nanoarchitectonics and Materials Nanoarchitectonics

by Katsuhiko Ariga

Molecules 2021, 26(6), 1621; https://doi.org/10.3390/molecules26061621 - 15 Mar 2021

Cited by 21 | Viewed by 3149

Abstract

Although various synthetic methodologies including organic synthesis, polymer chemistry, and materials science are the main contributors to the production of functional materials, the importance of regulation of nanoscale structures for better performance has become clear with recent science and technology developments. Therefore, a new research paradigm to produce functional material systems from nanoscale units has to be created as an advancement of nanoscale science. This task is assigned to an emerging concept, nanoarchitectonics, which aims to produce functional materials and functional structures from nanoscale unit components. This can be done through combining nanotechnology with the other research fields such as organic chemistry, supramolecular chemistry, materials science, and bio-related science. In this review article, the basic-level of nanoarchitectonics is first presented with atom/molecular-level structure formations and conversions from molecular units to functional materials. Then, two typical application-oriented nanoarchitectonics efforts in energy-oriented applications and bio-related applications are discussed. Finally, future directions of the molecular and materials nanoarchitectonics concepts for advancement of functional nanomaterials are briefly discussed. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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25 pages, 2906 KiB

Open AccessReview

Organic Electrochemical Transistors (OECTs) Toward Flexible and Wearable Bioelectronics

by Ariana Villarroel Marquez, Niall McEvoy and Amir Pakdel

Molecules 2020, 25(22), 5288; https://doi.org/10.3390/molecules25225288 - 13 Nov 2020

Cited by 35 | Viewed by 10600

Abstract

Organic electronics have emerged as a fascinating area of research and technology in the past two decades and are anticipated to replace classic inorganic semiconductors in many applications. Research on organic light-emitting diodes, organic photovoltaics, and organic thin-film transistors is already in an advanced stage, and the derived devices are commercially available. A more recent case is the organic electrochemical transistors (OECTs), whose core component is a conductive polymer in contact with ions and solvent molecules of an electrolyte, thus allowing it to simultaneously regulate electron and ion transport. OECTs are very effective in ion-to-electron transduction and sensor signal amplification. The use of synthetically tunable, biocompatible, and depositable organic materials in OECTs makes them specially interesting for biological applications and printable devices. In this review, we provide an overview of the history of OECTs, their physical characterization, and their operation mechanism. We analyze OECT performance improvements obtained by geometry design and active material selection (i.e., conductive polymers and small molecules) and conclude with their broad range of applications from biological sensors to wearable devices. Full article

(This article belongs to the Special Issue Advances in Nanomaterials Design and Nanoarchitectonics of Functional Materials: A Themed Issue Honoring Professor Katsuhiko Ariga)

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