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Chemistry
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Programmable and Stimulus-Responsive Supramolecular Assemblies
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Programmable and Stimulus-Responsive Supramolecular Assemblies

A special issue of Chemistry (ISSN 2624-8549). This special issue belongs to the section "Supramolecular Chemistry".

Deadline for manuscript submissions: closed (31 October 2023) | Viewed by 9029

Special Issue Editors

Prof. Dr. Craig Rice

E-Mail Website
Guest Editor
Department of Chemical Sciences, University of Huddersfield, Huddersfield HD1 3DH, UK
Interests: poly-dentate aromatic ligands; functional supramolecular complexes; re-programmable molecular systems; ditopic cryptate-containing sensors
Dr. Lei Li

E-Mail Website
Guest Editor Assistant
Department of Chemistry, Western Kentucky University, Bowling Green, KY 42104, USA
Interests: organic synthesis; polymer chemistry; fluorescent sensing; stimuli-responsive materials; self-healing polymers
Special Issues, Collections and Topics in MDPI journals

Special Issue Information

Dear Colleagues,

Supramolecular assemblies are assembled from two or more molecules through various noncovalent and reversible bonding modes, such as hydrogen bonding, metal–ligand bonding, cationic–anionic electrostatic interactions, hydrophobic–hydrophilic interactions, aromatic interactions, and charge-transfer interactions. The correct use of these interactions allows the chemist to control a disordered system of pre-existing compounds and form an organized structure as a result of specific pre-programmed interactions among the initial components. This results in structurally complex architectures that are not only intrinsically interesting, but are also inherently pleasing, as molecular order can be formed from chemical chaos.

One of the most important fundamentals of self-assembly is the inherent information contained within the pre-existing components. This information is expressed during the self-assembly process and controls the resultant supramolecular architecture. As a result, these pre-existing components are considered as pre-programmed and minor changes in this chemical information and can have a dramatic effect on the self-assembly process and the resultant architecture.

Another area of self-assembly control is the use of an external stimulus, which gives an added layer of influence, allowing manipulation of the size, shape, and molecular composition of the resultant assemblies. Formation of supramolecular systems that can be affected by electric fields, pH, temperature, and ionic strength is an emerging and important area of study.

This Special Issue of Chemistry is intended to present the recent advances in programmable and stimulus-responsive supramolecular assemblies. Authors are encouraged to submit various types of articles that address this theme in this Special Issue. Topics include, but are not limited to, the following:

(1) Metallosupramolecular self-assembly;

(2) Stimuli-responsive supramolecular polymers;

(3) Host–guest complexes;

(4) Hydrogen-bonded guided self-assembly;

(5) Self-assembly of organic materials;

(6) Design, synthesis, and characterization.

Please note that invited manuscripts are not guaranteed final acceptance and all submitted manuscripts will undergo vigorous external evaluation.

Prof. Dr. Craig Rice
Guest Editor

Dr. Lei Li
Guest Editor Assistant

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. Chemistry 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 1800 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

  • self-assembly
  • supramolecular assembly
  • programmable molecules
  • stimulus-responsive assemblies
  • supramolecular assembly
  • host–guest chemistry
  • crystal enginering

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Published Papers (3 papers)

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Research

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13 pages, 3781 KiB  
Article
Tweaking of Peripheral Moieties in Catalytic Amyloid for Modulating Hydrogel Strength and Hydrolase Activity
by Soumya Patra, Nimisha A. Mavlankar, Lakshminarayan Ramesan, Ashmeet Singh and Asish Pal
Chemistry 2023, 5(2), 1190-1202; https://doi.org/10.3390/chemistry5020080 - 10 May 2023
Cited by 2 | Viewed by 2447
Abstract
The de novo design and synthesis of peptide-based biocatalysts that can mimic the activity of natural enzymes is an exciting field with unique opportunities and challenges. In a natural enzyme, the active site is composed of an assembly of different amino acid residues, [...] Read more.
The de novo design and synthesis of peptide-based biocatalysts that can mimic the activity of natural enzymes is an exciting field with unique opportunities and challenges. In a natural enzyme, the active site is composed of an assembly of different amino acid residues, often coordinated with a metal ion. A metalloenzyme’s catalytic activity results from the dynamic and concerted interplay of various interactions among the residues and metal ions. Aiming to mimic such enzymes, simple peptide fragments, drawing structural inspiration from natural enzymes, can be utilized as a model. In our effort to mimic a metal-containing hydrolase, we designed peptide amphiphiles (PA) 1 and 2 with a terminal histidine having amide and acid functionalities, respectively, at its C-terminal, imparting differential ability to coordinate with Zn and Cu ions. The PAs demonstrate remarkable self-assembly behavior forming excellent nanofibers. Upon coordination with metal ions, depending on the coordination site the nanofibers become rigidified or weakened. Rheological studies revealed excellent mechanical properties of the hydrogels formed by the PAs and the PA–metal co-assemblies. Using such co-assemblies, we mimic hydrolase activity against a p-nitrophenyl acetate (p-NPA) substrate. Michaelis–Menten’s enzyme kinetic parameters indicated superior catalytic activity of 2 with Zn amongst all the assemblies. Full article
(This article belongs to the Special Issue Programmable and Stimulus-Responsive Supramolecular Assemblies)
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12 pages, 3309 KiB  
Article
Stimuli-Responsive Designer Supramolecular Polymer Gel
by M. Douzapau, Srayoshi Roy Chowdhury, Surajit Singh, Olamilekan Joseph Ibukun and Debasish Haldar
Chemistry 2023, 5(1), 691-702; https://doi.org/10.3390/chemistry5010048 - 22 Mar 2023
Cited by 3 | Viewed by 2585
Abstract
This paper reports a stimuli-responsive designer supramolecular polymer gel in dimethylsulphoxide (DMSO)/water (1:2) based on a dipeptide amphiphile and β-cyclodextrin (β-CD) The dipeptide amphiphile contains caproic acid at the N terminus and methyl ester at the C terminus. From X-ray single crystal diffraction, [...] Read more.
This paper reports a stimuli-responsive designer supramolecular polymer gel in dimethylsulphoxide (DMSO)/water (1:2) based on a dipeptide amphiphile and β-cyclodextrin (β-CD) The dipeptide amphiphile contains caproic acid at the N terminus and methyl ester at the C terminus. From X-ray single crystal diffraction, the amphiphile adopts a kink-like conformation. The amphiphile self-assembled to form a parallel sheet-like structure stabilized by multiple intermolecular hydrogen bonds. Moreover, the parallel sheet-like structure is also stabilized by edge-to-edge π–π stacking interactions. In higher-order packing, it forms a corrugated sheet-like structure stabilized by hydrophobic interactions. The dipeptide amphiphile interacts with β-cyclodextrin and forms gel through supramolecular polymer formation in (DMSO)/water (1:2) by a simple heating-cooling cycle. The sol-to-gel transformation is because of a host–guest complex between compound 1 and β-CD and the formation of supramolecular polymer accompanied by microstructure changes from nanofibers to microrods. The gel is temperature responsive with a Tgel of 70 °C. The supramolecular polymer gel is also responsive to stimuli such aspicric acid and HCl. The extensive spectroscopic studies show that the aromatic hydrophobic side chain of compound 1 forms a host–guest complex with β-CD. These results will be helpful for the design of advanced programable eco-friendly functional materials. Full article
(This article belongs to the Special Issue Programmable and Stimulus-Responsive Supramolecular Assemblies)
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Review

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19 pages, 5039 KiB  
Review
Lewis Acidic Zinc(II) Complexes of Tetradentate Ligands as Building Blocks for Responsive Assembled Supramolecular Structures
by Ivan Pietro Oliveri and Santo Di Bella
Chemistry 2023, 5(1), 119-137; https://doi.org/10.3390/chemistry5010010 - 13 Jan 2023
Cited by 11 | Viewed by 3138
Abstract
This review presents representative examples illustrating how the Lewis acidic character of the Zn(II) metal center in Zn(salen)-type complexes, as well as in complexes of other tetradentate ligands, and the nature of the medium govern their supramolecular aggregation, leading to the formation of [...] Read more.
This review presents representative examples illustrating how the Lewis acidic character of the Zn(II) metal center in Zn(salen)-type complexes, as well as in complexes of other tetradentate ligands, and the nature of the medium govern their supramolecular aggregation, leading to the formation of a variety of supramolecular structures, either in solution or in the solid state. Stabilization of these Lewis acidic complexes is almost always reached through an axial coordination of a Lewis base, leading to a penta-coordinated square-pyramidal geometry around the metal center. The coverage is not exhaustive, mainly focused on their crystallographic structures, but also on their aggregation and sensing properties in solution, and on their self-assembled and responsive nanostructures, summarizing their salient aspects. The axial ligands can easily be displaced, either in solution or in the solid state, with suitable Lewis bases, thus being responsive supramolecular structures useful for sensing. This contribution represents the first attempt to relate some common features of the chemistry of different families of Zn(II) complexes of tetradentate ligands to their intrinsic Lewis acidic character. Full article
(This article belongs to the Special Issue Programmable and Stimulus-Responsive Supramolecular Assemblies)
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