One-Pot Mechanosynthesis with Three Levels of Molecular Self-Assembly: Coordination Bonds, Hydrogen Bonds and Host–Guest Inclusion

2009 ◽  
Vol 15 (46) ◽  
pp. 12644-12652 ◽  
Author(s):  
Tomislav FrisÌŒcÌŒić ◽  
Ernest MesÌŒtrović ◽  
Dijana SÌŒkalec SÌŒamec ◽  
Branko Kaitner ◽  
László Fábián
Keyword(s):  
Hydrogen Bonds ◽  
Self Assembly ◽  
One Pot ◽  
Coordination Bonds

Flow Chemistry Controls Both Self-Assembly and the Entrapped Oscillatory Cargo in Belousov-Zhabotinsky Driven Polymerization-Induced Self-Assembly

2019 ◽  
Author(s):  
Liman Hou ◽  
Marta Dueñas-Diez ◽  
Rohit Srivastava ◽  
Juan Perez-Mercader
Keyword(s):  
Self Assembly ◽  
Flow Chemistry ◽  
Batch Reactors ◽  
Equilibrium Conditions ◽  
One Pot ◽  
Bz Reaction ◽  
Polymer Vesicles ◽  
Simultaneous Control ◽  
Novel Method ◽  
Continuously Stirred Tank Reactor

<p></p><p>Belousov-Zhabotinsky (B-Z) reaction driven polymerization-induced self-assembly (PISA), or B-Z PISA, is a novel method for the autonomous one-pot synthesis of polymer vesicles from a macroCTA (macro chain transfer agent) and monomer solution (“soup”) containing the above and the BZ reaction components. In it, the polymerization is driven (and controlled) by periodically generated radicals generated in the oscillations of the B-Z reaction. These are inhibitor/activator radicals for the polymerization. Until now B-Z PISA has only been carried out in batch reactors. In this manuscript we present the results of running the system using a continuously stirred tank reactor (CSTR) configuration which offers some interesting advantages.Indeed, by controlling the CSTR parameters we achieve reproducible and simultaneous control of the PISA process and of the properties of the oscillatory cargo encapsulated in the resulting vesicles. Furthermore, the use of flow chemistry enables a more precise morphology control and chemical cargo tuning. Finally, in the context of biomimetic applications a CSTR operation mimics more closely the open non-equilibrium conditions of living systems and their surrounding environments.</p><p></p>

scholarly journals Precise Synthesis and Thin Film Self-Assembly of PLLA-b-PS Bottlebrush Block Copolymers

Molecules ◽  
2021 ◽  
Vol 26 (5) ◽  
pp. 1412
Author(s):  
Eunkyung Ji ◽  
Cian Cummins ◽  
Guillaume Fleury
Keyword(s):  
Thin Film ◽  
Block Copolymers ◽  
Self Assembly ◽  
Ring Opening ◽  
Periodic Structures ◽  
One Pot ◽  
Ordered Structures ◽  
Carbonyl Chloride ◽  
Thin Film Patterning ◽  
Nanoporous Templates

The ability of bottlebrush block copolymers (BBCPs) to self-assemble into ordered large periodic structures could greatly expand the scope of photonic and membrane technologies. In this paper, we describe a two-step synthesis of poly(l-lactide)-b-polystyrene (PLLA-b-PS) BBCPs and their rapid thin-film self-assembly. PLLA chains were grown from exo-5-norbornene-2-methanol via ring-opening polymerization (ROP) of l-lactide to produce norbornene-terminated PLLA. Norbonene-terminated PS was prepared using anionic polymerization followed by a termination reaction with exo-5-norbornene-2-carbonyl chloride. PLLA-b-PS BBCPs were prepared from these two norbornenyl macromonomers by a one-pot sequential ring opening metathesis polymerization (ROMP). PLLA-b-PS BBCPs thin-films exhibited cylindrical and lamellar morphologies depending on the relative block volume fractions, with domain sizes of 46–58 nm and periodicities of 70–102 nm. Additionally, nanoporous templates were produced by the selective etching of PLLA blocks from ordered structures. The findings described in this work provide further insight into the controlled synthesis of BBCPs leading to various possible morphologies for applications requiring large periodicities. Moreover, the rapid thin film patterning strategy demonstrated (>5 min) highlights the advantages of using PLLA-b-PS BBCP materials beyond their linear BCP analogues in terms of both dimensions achievable and reduced processing time.

scholarly journals Taming nitroformate through encapsulation with nitrogen-rich hydrogen-bonded organic frameworks

2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Jichuan Zhang ◽  
Yongan Feng ◽  
Richard J. Staples ◽  
Jiaheng Zhang ◽  
Jean’ne M. Shreeve
Keyword(s):  
Thermal Stability ◽  
Hydrogen Bonds ◽  
Self Assembly ◽  
Energetic Materials ◽  
Decomposition Temperature ◽  
High Oxygen Content ◽  
The Poor ◽  
Simple Preparation ◽  
First Time ◽  
Hydrogen Bonded

AbstractOwing to its simple preparation and high oxygen content, nitroformate [−C(NO2)3, NF] is an extremely attractive oxidant component for propellants and explosives. However, the poor thermostability of NF-based derivatives has been an unconquerable barrier for more than 150 years, thus hindering its application. In this study, the first example of a nitrogen-rich hydrogen-bonded organic framework (HOF-NF) is designed and constructed through self-assembly in energetic materials, in which NF anions are trapped in pores of the resulting framework via the dual force of ionic and hydrogen bonds from the strengthened framework. These factors lead to the decomposition temperature of the resulting HOF-NF moiety being 200 °C, which exceeds the challenge of thermal stability over 180 °C for the first time among NF-based compounds. A large number of NF-based compounds with high stabilities and excellent properties can be designed and synthesized on the basis of this work.

Chiroptical Probing of Lanthanide-Directed Self-Assembly Formation Using btp Ligands Formed in One-Pot Diazo-Transfer/Deprotection Click Reaction from Chiral Amines

2015 ◽  
Vol 22 (2) ◽  
pp. 486-490 ◽  
Author(s):  
Joseph P. Byrne ◽  
Miguel Martínez-Calvo ◽  
Robert D. Peacock ◽  
Thorfinnur Gunnlaugsson
Keyword(s):  
Self Assembly ◽  
Click Reaction ◽  
Chiral Amines ◽  
One Pot

One-pot synthesis of a TiO2–CdS nano-heterostructure assembly with enhanced photocatalytic activity

RSC Advances ◽  
2015 ◽  
Vol 5 (44) ◽  
pp. 34942-34948 ◽  
Author(s):  
Sayantan Mazumdar ◽  
Aninda J. Bhattacharyya
Keyword(s):  
Titanium Dioxide ◽  
Photocatalytic Activity ◽  
Cadmium Sulfide ◽  
Self Assembly ◽  
Cost Effective ◽  
One Pot ◽  
One Pot Synthesis ◽  
Cost Effective Method

An unprecedented morphology of a titanium dioxide (TiO2) and cadmium sulfide (CdS) self-assembly obtained using a ‘truly’ one-pot and highly cost effective method with a multi-gram scale yield is reported here.

Thermally bandwidth-controllable reflective liquid crystal film from rupture and self-assembly of hydrogen bonds

2016 ◽  
Vol 43 (12) ◽  
pp. 1732-1738 ◽  
Author(s):  
Feifei Wang ◽  
Ping Song ◽  
Huai Yang ◽  
Xibin Shao
Keyword(s):  
Liquid Crystal ◽  
Hydrogen Bonds ◽  
Self Assembly ◽  
Crystal Film

scholarly journals One-pot synthesis of (1RS,21SR)-diethyl 2-[23-amino-22-ethoxycarbonyl-8,11,14-trioxa-25-azatetracyclo[19.3.1.02,7.015,20]pentacosa-2,4,6,15(20),16,18,22-heptaen-25-yl]but-2-endioate

2018 ◽  
Vol 74 (9) ◽  
pp. 1281-1284
Author(s):  
Thi Thanh Van Tran ◽  
Tuan Anh Le ◽  
Hong Hieu Truong ◽  
Thi Nhung Dao ◽  
Anatoly T. Soldatenkov ◽  
...  
Keyword(s):  
Hydrogen Bonds ◽  
Molecular Conformation ◽  
Michael Reaction ◽  
Biological Activities ◽  
Boat Conformation ◽  
One Pot ◽  
Computer Prediction ◽  
Compound C ◽  
Intramolecular Hydrogen ◽  
The Michael Reaction

The title compound, C30H34N2O9 (4), is a product of the Michael reaction of azacrown ether with dimethyl acetylenedicarboxylate modified by an addition of NH3 (aq.) at 298 K. The aza-14-crown-4-ether ring adopts a bowl conformation. The dihedral angle between the planes of the benzene rings fused to the aza-14-crown-4-ether moiety is 8.65 (5)°. The tetrahydropyridine ring has a boat conformation. The molecular conformation is supported by one N—H...O and two C—H...O intramolecular hydrogen bonds. Both heterocyclic and amino N atoms have essentially planar configurations (sums of the bond angles are 359.35 and 358.00°). Compound 4 crystallizes as a racemate consisting of enantiomeric pairs of the 1R,21S diastereomer. In the crystal, molecules of 4 are connected by N—H...O hydrogen bonds, forming chains along [100]. According to the PASS program (computer prediction of biological activities), compound 4 may exhibit antiallergic (72% probability) and antiasthmatic (67%) activity, as well as be a membrane permeability inhibitor (65%).

scholarly journals Dynamic porous property in a new heterometallic supramolecular compound

2014 ◽  
Vol 70 (a1) ◽  
pp. C1474-C1474
Author(s):  
Patrice Kenfack ◽  
Emmanuel Wenger ◽  
Slimane Dahaoui ◽  
John Lambi ◽  
Pierrick Durand ◽  
...  
Keyword(s):  
Hydrogen Bonds ◽  
Self Assembly ◽  
Water Clusters ◽  
Chair Conformation ◽  
Unit Cell ◽  
Supramolecular Compounds ◽  
Multifunctional Compounds ◽  
Potential Applications ◽  
One Step ◽  
Mean Vector

Supramolecular compounds have attracted considerable interest to chemists, physicists and materials scientists due to their fascinating structures and potential applications as porosity [1-3] but one of the most appealing aims today, is to build multifunctional compounds. We are interested to rationalize the synthesis of porous heterometallic compounds by self- assembly via hydrogen bonds. In this communication, we present a stacked 2D Catena-{Co(amp)3Cr(ox)3.6H2O} (amp = 2-picolylamine, ox=oxalate). It is built by layers in which both (Co(amp)3+ (D) and Cr(ox)3- ( A)) ionic units are linked in a repeating DADADA...pattern along both the a and c axis with four and two hydrogen bonds respectively. These layers host very well resolved dodecameric discrete ring water clusters (R12) built by six independent molecules located around the centrosymmetric Wyckoff position's of the P21/n space group in which the compound crystallizes. The clusters are ranged along the [001] direction, occupy 807.6 Å3 (23.9%) of the unit cell and have a chair conformation via 10 hydrogen bonds. The dehydration process of the compound occurs in one step around 77oC and the dehydrated compound remains crystalline although all framework atoms move by 2.25 Å along a mean vector (dm= 2.21 i + 0.17 j + 0.37 k) during the process. The unit cell is then reduced by 12.34 % along a, 12.22% along b and 2. 03% along c reducing V by 22.03%. By exposure to air, the regeneration of the compound needs 90 min, following the first kinetic Avrami's model.

scholarly journals DESIGN AND SYNTHESIS OF MOLECULAR TWEEZER BASED ON 3-HYDROXYFLAVONE FOR THE DETECTION OF ATP

2017 ◽  
pp. 67-70
Author(s):  
O. Bugera ◽  
A. Netrebchuk ◽  
V. Pivovarenko
Keyword(s):  
Amino Acid ◽  
Hydrogen Bonds ◽  
Atmospheric Oxygen ◽  
High Sensitivity ◽  
Fluorescence Probes ◽  
Amino Acid Derivative ◽  
One Pot ◽  
Design And Synthesis ◽  
Sensitivity And Selectivity ◽  
Molecular Tweezer

Adenosine 5'-triphosphate (ATP) is known as a universal energy source and signaling mediator in numerous biological processes. Among the methods for its determination, molecular fluorescence probes occupy leading positions due to high sensitivity and selectivity. Recently we have shown that 31 of 33 tested flavones and quinolones of various structures give fluorescence response and can be effectively applied as the probes in aqueous solutions for detection of ATP in 1–50,000 μM range of its concentrations. To increase response parameters of a probe in respect to ATP we have synthesized N,N'-(butane-1,4-diyl)bis(2-((2-(4-(dimethylamino)phenyl)-3-hydroxy-4-oxo-4H-chromene-6-yl)oxy)acetamide, the molecular tweezer composed of two flavonol units connected by active linker. On our idea, being equipped by two planar platforms, the tweezershould demonstrate increased affinity and selectivity to ATP in a result of increased number of hydrogen bonds and increased stacking interactions. Having two NH-amide groups the amino acid linker will form hydrogen bonds with the phosphates of ATP, increasing the portion of probe-ATP complex population in the reporting conformation.In the four-step synthesis of this molecular device, starting from methyl 2-(3-acetyl-4-hydroxyphenoxy)acetate and N,N-dimethylaminobenzaldehyde, the conditions for the reaction of one-pot chalcone formation and its oxidative heterocyclization in the presence of an organic base were found, which resulted in the isolation of a target flavonol-amino acid derivative with high yields. We suggest that atmospheric oxygen was an oxidizer in this process. The obtained derivative was converted intotarget compound by dual condensation with 1,4-butane diamine.

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