30 Sep 16:35
by Tatiana Tikhonova,
Nataliya Rovnyagina,
Zohar Arnon,
Boris Yakimov,
Yuri Efremov,
Dana Cohen-Gerassi,
Nastasia Kosheleva,
Vladimir Drachev,
Andrey Svistunov,
Peter Timashev,
Lihi Adler-Abramovich,
Evgeny Shirshin,
Michal Halperin-Sternfeld
Thioflavin T dramatically enhances the structural and mechanical properties of the Fmoc-FF hydrogel and drives the self-assembly by interfering the metastable phase of the two-step nucleation process.
Abstract
The self-assembly of peptides is a key direction for fabrication of advanced materials. Novel approaches for fine tuning of macroscopic and microscopic properties of peptide self-assemblies are of a high demand for constructing biomaterials with desired properties. In this work, while studying the kinetics of the Fmoc-Diphenylalanine (Fmoc-FF) dipeptide self-assembly using the Thioflavin T (ThT) dye, we observed that the presence of ThT strongly modifies structural and mechanical properties of the Fmoc-FF hydrogel. Notably, the presence of ThT resulted in a tenfold increase of the gelation time and in the formation of short and dense fibers in the hydrogel. As a result of these morphological alteration higher thermal stability, and most important, tenfold increase of the hydrogel rigidity was achieved. Hence, ThT not only slowed the kinetics of the Fmoc-FF hydrogel formation, but also strongly enhanced its mechanical properties. In this study, we provide a detailed description of the ThT effect on the hydrogel properties and suggest the mechanisms for this phenomenon, paving the way for the novel approach to the control of the peptide hydrogels’ micro- and macroscale properties.
26 Jan 18:37
by Sander Borgmans,
Sven M.J. Rogge,
Juul S. De Vos,
Christian V. Stevens,
Pascal Van Der Voort,
Veronique Van Speybroeck
Structurally characterizing new materials is tremendously challenging, especially when single crystal structures are hardly available which is often the case for covalent organic frameworks. Yet, knowledge of the atomic structure is key to establish structure‐function relations and enable functional material design. Herein a new protocol is proposed to unambiguously predict the structure of poorly crystalline materials through a likelihood ordering based on the X‐ray diffraction (XRD) pattern. Key of the procedure is the broad set of structures generated from a limited number of building blocks and topologies, which is submitted to operando structural characterization. The dynamic averaging in the latter accounts for the operando conditions and inherent temporal character of experimental measurements, yielding unparalleled agreement with experimental powder XRD patterns. The proposed concept can hence unquestionably identify the structure of experimentally synthesized materials, a crucial step to design next generation functional materials.
05 Jan 17:39
by Yuya Okuyama,
Mayu Kidena,
Erina Kato,
Sayaka Kawano,
Koki Ishii,
Kenta Maie,
Kazuki Miura,
Siro Simizu,
Takaaki Sato,
Noritaka Chida
All‐nitrogenated sugars (ANSs), in which all hydroxy groups in a carbohydrate are replaced with amino groups, are anticipated to be privileged structures with useful biological activities. In their Communication (DOI: 10.1002/anie.202015141), Takaaki Sato, Noritaka Chida et al. report synthesis, transformation, and biological tests of ANS derivatives. The key to success is a seven‐step synthesis of ANSs by the sequential Overman rearrangement enabling formal simultaneous substitution of four or five hydroxy groups in monosaccharides with amino groups.
15 Mar 23:21
by Durga Prasad Hari, Joseph C. Abell, Valerio Fasano, and Varinder K. Aggarwal*
Journal of the American Chemical Society
DOI: 10.1021/jacs.0c00813
15 Feb 08:11
by Guangbin Jiang,
Shoucai Wang,
Jun Zhang,
Jianwen Yu,
Ziang Zhang,
Fanghua Ji
Abstract
An efficient protocol for the preparation of indolo[1,2‐a]quinazolines via palladium‐catalyzed decarboxylative annulation of indols with α‐oxocarboxylic acids has been realized by using primary amine as a directing group (DG). This transformation proceeds smoothly with exclusive regioselectivity and represents an one‐pot Domino synthesis of indo‐lo[1,2‐a]quinazolines from α‐oxocarboxylic acids.