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Supramolecular Chemistry and Self-Assembly: Themed Issue in Honor of Professor Itamar Willner on the Occasion of His 70th Birthday

A special issue of Molecules (ISSN 1420-3049).

Deadline for manuscript submissions: closed (31 October 2017) | Viewed by 43772

Special Issue Editors


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Guest Editor
Department of Chemistry, University of South Dakota, Vermillion, SD 57069, USA
Interests: photocatalysis; photo-responsive liquid crystal; time-resolved dynamics; microscopy; charge carrier dynamics

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Guest Editor
Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem, Israel
Interests: scanning electrochemical microscopy and nanoelectrochemsitry; electrodeposition of nanomaterials; sol-gel technology; self-assembled monolayers; thin films and functional coatings; solar-thermal energy conversion; forensic science; supercapacitors; molecular imprinting; electrochemical filtration; antibiofouling and antimicrobial coatings

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Guest Editor
School of Chemistry, the Raymond and Beverly Sackler Faculty of Exact Sciences, Tel Aviv University, Tel Aviv 69978, Israel
Interests: bioelectronics; nanoelectronics; nanomaterials; sensors and biosensors; medical diagnosis

Special Issue Information

Dear Colleagues,

Supramolecular chemistry and self-assembly have long been recognized as major pillars in understanding the organization of chemical and biological components that are beyond molecules. Although the first contributions to supramolecular chemistry were made by well-known scientists, such as Fischer in the 19th century, it took almost another century until the first artificial systems were synthesized by Pedersen, Cram and Lehn. Since then, the concepts of supramolecular chemistry and self-assembly have become the bread and butter of the scientific community dealing with the organization of monolayers, thin films and biologically inspired complex systems. These concepts, which drive the organization and activity of many biological systems, have been studied experimentally and theoretically, and have paved their implementation in numerous applications, ranging from sensing to responsive materials actuators, and many more.

Our journal is pleased to publish a themed issue in honor of Professor Itamar Willner for his outstanding research contributions in the fields of “Supramolecular Chemistry and Self-Assembly”.

Professor Itamar Willner, from the Institute of Chemistry at the Hebrew University, is undoubtedly one of the leading chemists in Israel and around the world. He graduated at the Hebrew University, and carried out his post-doctoral studies at the University of California Berkeley, with Melvin Calvin (who received the Nobel Prize in Chemistry in 1961). He joined the Hebrew University in 1981, where he was appointed Professor in 1986.

Professor Willner is the author or more than 730 publications, with more than 48,000 citations, and an h-index of 117. He serves as the head of the sciences division of the Israeli Academy of Science, and was also nominated to the German National of Academy of Science and the European Academy of Sciences and Arts. He has received a remarkable number of awards, among them the Israel Prize (which is the highest prize awarded by the Israeli Government), the Max- Planck Research Award for International Cooperation, the Israel Chemical Society Award, the Rothschild Prize and the EMET Prize.

His research interests embrace bioelectronics, biomolecule-based nanocircuitry and nanostructures, biomolecule-inorganic nanostructures, DNA machines for biosensing, biomolecule-based computing, biomolecular photonics, molecular switches and motors and functional polymers. Yet, he has contributed significantly to many more areas, such as energy conversion and storage, nanomedicine and nanobiotechnology. In his outstanding research, Professor Willner very successfully combines organic synthesis with the principles of supramolecular chemistry, self-assembly, and a wide variety of biological components spanning from enzymes to antigens and nucleic acids.

Professor Willner had a very large number of graduate and post-doctoral students, many of whom are currently holding academic positions in Israel and around the world.

Prof. Dr. Ranjit T. Koodali
Prof. Dr. Daniel Mandler
Prof. Dr. Fernando Patolsky
Guest Editors

Manuscript Submission Information

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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

  • supramolecular chemistry

  • self-assembly

  • self-organization

  • imprinting

  • sensing

  • Biosystems

  • bioelectronics

  • nanostructures

  • nanomotors

  • thin films

Published Papers (6 papers)

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Research

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10 pages, 2900 KiB  
Article
Coordination-Enhanced Luminescence on Tetra-Phenylethylene-Based Supramolecular Assemblies
by Qian-Qian Yan, Shao-Jun Hu, Guang-Lu Zhang, Ting Zhang, Li-Peng Zhou and Qing-Fu Sun
Molecules 2018, 23(2), 363; https://doi.org/10.3390/molecules23020363 - 09 Feb 2018
Cited by 7 | Viewed by 5375
Abstract
Materials with aggregation-induced emission (AIE) properties have received increased attention recently due to their potential applications in light-emitting devices, chemo/biosensors and biomedical diagnostics. In general, AIE requires the forced aggregation of the AIEgens induced by the poor solvent or close arrangement of AIEgens [...] Read more.
Materials with aggregation-induced emission (AIE) properties have received increased attention recently due to their potential applications in light-emitting devices, chemo/biosensors and biomedical diagnostics. In general, AIE requires the forced aggregation of the AIEgens induced by the poor solvent or close arrangement of AIEgens covalently attached to polymer chains. Here, we report two coordination-enhanced fluorescent supramolecular complexes featuring hierarchically restricted intramolecular motions via the self-assembly of tetraphenylethylene (TPE)-based tetra-dentate (La) and bidentate (Lb) ligands and the cis-Pd(en)(NO3)2 (en = ethylenediamine) unit. While the free ligands are non-emissive in dilute solution and show typical AIE properties in both mixed solvent system and the solid state, the self-assembled complexes maintain their fluorescent nature in the solution state. In particular, the Pd4(La)2 complex shows remarkable 6-fold fluorescent enhancement over La in dilute solution. We anticipate that these kinds of coordination-enhanced emissive supramolecules will find applications in biomedical sensing or labeling. Full article
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1550 KiB  
Article
Design, Synthesis, and Use of Peptides Derived from Human Papillomavirus L1 Protein for the Modification of Gold Electrode Surfaces by Self-Assembled Monolayers
by John Alejandro Lara Carrillo, Ricardo Fierro Medina, Juan Manríquez Rocha, Erika Bustos Bustos, Diego Sebastián Insuasty Cepeda, Javier Eduardo García Castañeda and Zuly Jenny Rivera Monroy
Molecules 2017, 22(11), 1970; https://doi.org/10.3390/molecules22111970 - 14 Nov 2017
Cited by 6 | Viewed by 3980
Abstract
In order to obtain gold electrode surfaces modified with Human Papillomavirus L1 protein (HPV L1)-derived peptides, two sequences, SPINNTKPHEAR and YIK, were chosen. Both have been recognized by means of sera from patients infected with HPV. The molecules, Fc-Ahx-SPINNTKPHEAR, Ac–C–Ahx-(Fc)KSPINNTKPHEAR, Ac–C– [...] Read more.
In order to obtain gold electrode surfaces modified with Human Papillomavirus L1 protein (HPV L1)-derived peptides, two sequences, SPINNTKPHEAR and YIK, were chosen. Both have been recognized by means of sera from patients infected with HPV. The molecules, Fc-Ahx-SPINNTKPHEAR, Ac–C–Ahx-(Fc)KSPINNTKPHEAR, Ac–C–Ahx-SPINNTKPHEAR(Fc)K, C–Ahx–SPINNTKPHEAR, and (YIK)2Ahx–C, were designed, synthesized, and characterized. Our results suggest that peptides derived from the SPINNTKPHEAR sequence, containing ferrocene and cysteine residues, are not stable and not adequate for electrode surface modification. The surface of polycrystalline gold electrodes was modified with the peptides C-Ahx-SPINNTKPHEAR or (YIK)2-Ahx-C through self-assembly. The modified polycrystalline gold electrodes were characterized via infrared spectroscopy and electrochemical measurements. The thermodynamic parameters, surface coverage factor, and medium pH effect were determined for these surfaces. The results indicate that surface modification depends on the peptide sequence (length, amino acid composition, polyvalence, etc.). The influence of antipeptide antibodies on the voltammetric response of the modified electrode was evaluated by comparing results obtained with pre-immune and post-immune serum samples. Full article
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5640 KiB  
Article
Continuous Preparation of Hollow Polymeric Nanocapsules Using Self-Assembly and a Photo-Crosslinking Process of an Amphiphilic Block Copolymer
by Xuan Don Nguyen, Hyeong Jin Jeon, Van Tien Nguyen, Dong Hyeok Park, Taeheon Lee, Hyun-jong Paik, June Huh and Jeung Sang Go
Molecules 2017, 22(11), 1892; https://doi.org/10.3390/molecules22111892 - 03 Nov 2017
Cited by 2 | Viewed by 4334
Abstract
This paper presents a fabrication method of hollow polymeric nanocapsules (HPNCs). The HPNCs were examined to reduce light trapping in an organic light emitting diodes (OLED) device by increasing the refractive index contrast. They were continuously fabricated by the sequential process of self-assembly [...] Read more.
This paper presents a fabrication method of hollow polymeric nanocapsules (HPNCs). The HPNCs were examined to reduce light trapping in an organic light emitting diodes (OLED) device by increasing the refractive index contrast. They were continuously fabricated by the sequential process of self-assembly and photo-crosslinking of an amphiphilic block copolymer of SBR-b-PEGMA, poly(styrene-r-butadiene)-b-poly(poly(ethylene glycol) methyl ether methacrylate) in a flow-focusing microfluidic device. After the photo-crosslinking process, the produced HPNCs have a higher resistance to water and organic solvents, which is applicable to the fabrication process of optical devices. The morphology and hollow structure of the produced nanocapsules were determined by transmission electron microscopy (TEM), scanning electron microscopy (SEM), and atomic force microscopy (AFM). Also, their size control was examined by varying the ratio of inlet flow rates and the morphological difference was studied by changing the polymer concentration. The size was measured by dynamic light scattering (DLS). The refractive index of the layer with and without the HPNCs was measured, and a lower refractive index was obtained in the HPNCs-dispersed layer. In future work, the light extraction efficiency of the HPNCs-dispersed OLED will be examined. Full article
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Review

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38 pages, 12618 KiB  
Review
Quantum-Chemical Insights into the Self-Assembly of Carbon-Based Supramolecular Complexes
by Joaquín Calbo, Juan Carlos Sancho-García, Enrique Ortí and Juan Aragó
Molecules 2018, 23(1), 118; https://doi.org/10.3390/molecules23010118 - 07 Jan 2018
Cited by 9 | Viewed by 5897
Abstract
Understanding how molecular systems self-assemble to form well-organized superstructures governed by noncovalent interactions is essential in the field of supramolecular chemistry. In the nanoscience context, the self-assembly of different carbon-based nanoforms (fullerenes, carbon nanotubes and graphene) with, in general, electron-donor molecular systems, has [...] Read more.
Understanding how molecular systems self-assemble to form well-organized superstructures governed by noncovalent interactions is essential in the field of supramolecular chemistry. In the nanoscience context, the self-assembly of different carbon-based nanoforms (fullerenes, carbon nanotubes and graphene) with, in general, electron-donor molecular systems, has received increasing attention as a means of generating potential candidates for technological applications. In these carbon-based systems, a deep characterization of the supramolecular organization is crucial to establish an intimate relation between supramolecular structure and functionality. Detailed structural information on the self-assembly of these carbon-based nanoforms is however not always accessible from experimental techniques. In this regard, quantum chemistry has demonstrated to be key to gain a deep insight into the supramolecular organization of molecular systems of high interest. In this review, we intend to highlight the fundamental role that quantum-chemical calculations can play to understand the supramolecular self-assembly of carbon-based nanoforms through a limited selection of supramolecular assemblies involving fullerene, fullerene fragments, nanotubes and graphene with several electron-rich π-conjugated systems. Full article
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3587 KiB  
Review
Recent Progress in Nanomaterial-Based Electrochemical Biosensors for Cancer Biomarkers: A Review
by Baozhen Wang, Uichi Akiba and Jun-ichi Anzai
Molecules 2017, 22(7), 1048; https://doi.org/10.3390/molecules22071048 - 24 Jun 2017
Cited by 97 | Viewed by 9470
Abstract
This article reviews recent progress in the development of nanomaterial-based electrochemical biosensors for cancer biomarkers. Because of their high electrical conductivity, high affinity to biomolecules, and high surface area-to-weight ratios, nanomaterials, including metal nanoparticles, carbon nanotubes, and graphene, have been used for fabricating [...] Read more.
This article reviews recent progress in the development of nanomaterial-based electrochemical biosensors for cancer biomarkers. Because of their high electrical conductivity, high affinity to biomolecules, and high surface area-to-weight ratios, nanomaterials, including metal nanoparticles, carbon nanotubes, and graphene, have been used for fabricating electrochemical biosensors. Electrodes are often coated with nanomaterials to increase the effective surface area of the electrodes and immobilize a large number of biomolecules such as enzymes and antibodies. Alternatively, nanomaterials are used as signaling labels for increasing the output signals of cancer biomarker sensors, in which nanomaterials are conjugated with secondary antibodies and redox compounds. According to this strategy, a variety of biosensors have been developed for detecting cancer biomarkers. Recent studies show that using nanomaterials is highly advantageous in preparing high-performance biosensors for detecting lower levels of cancer biomarkers. This review focuses mainly on the protocols for using nanomaterials to construct cancer biomarker sensors and the performance characteristics of the sensors. Recent trends in the development of cancer biomarker sensors are discussed according to the nanomaterials used. Full article
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11873 KiB  
Review
Porous Hydrogen-Bonded Organic Frameworks
by Yi-Fei Han, Ying-Xue Yuan and Hong-Bo Wang
Molecules 2017, 22(2), 266; https://doi.org/10.3390/molecules22020266 - 13 Feb 2017
Cited by 99 | Viewed by 13727
Abstract
Ordered porous solid-state architectures constructed via non-covalent supramolecular self-assembly have attracted increasing interest due to their unique advantages and potential applications. Porous metal-coordination organic frameworks (MOFs) are generated by the assembly of metal coordination centers and organic linkers. Compared to MOFs, porous hydrogen-bonded [...] Read more.
Ordered porous solid-state architectures constructed via non-covalent supramolecular self-assembly have attracted increasing interest due to their unique advantages and potential applications. Porous metal-coordination organic frameworks (MOFs) are generated by the assembly of metal coordination centers and organic linkers. Compared to MOFs, porous hydrogen-bonded organic frameworks (HOFs) are readily purified and recovered via simple recrystallization. However, due to lacking of sufficiently ability to orientate self-aggregation of building motifs in predictable manners, rational design and preparation of porous HOFs are still challenging. Herein, we summarize recent developments about porous HOFs and attempt to gain deeper insights into the design strategies of basic building motifs. Full article
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