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Cationic Chain-Growth Polymerization: Mechanism00:57

Cationic Chain-Growth Polymerization: Mechanism

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The cationic polymerization mechanism consists of three steps: initiation, propagation, and termination. In the initiation step of the polymerization process, the π bond of a monomer gets protonated by the Lewis acid catalyst, which is formed from boron trifluoride and water. The protonation of the π bond generates a carbocation stabilized by the electron‐donating group. In the propagation step, the π bond of the second monomer acts as a nucleophile and attacks the...
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Step-Growth Polymerization: Overview01:03

Step-Growth Polymerization: Overview

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Step-growth or condensation polymerization is a stepwise reaction of bi or multifunctional monomers to form long-chain polymers. As all the monomers are reactive, most of the monomers are consumed at the early stages of the reaction to form small chains of reactive oligomers, which then combine to form long polymer chains in the late stages. Hence, the reaction has to proceed for a long time to achieve high molecular weight polymers.
Many natural and synthetic polymers are produced by...
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Radical Chain-Growth Polymerization: Overview01:10

Radical Chain-Growth Polymerization: Overview

2.9K
Chain-growth or addition polymerization is successive addition reactions of monomers with a polymer chain. In radical chain-growth polymerization, the reaction proceeds via a free-radical intermediate. The free radical is formed from radical initiators, which spontaneously generate free radicals by homolytic fission. Organic peroxides (such as dibenzoyl peroxide, as shown in Figure 1) or azo compounds are popular radical initiators. A low concentration ratio of radical initiator to monomer is...
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Ziegler–Natta Chain-Growth Polymerization: Overview01:17

Ziegler–Natta Chain-Growth Polymerization: Overview

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Ziegler–Natta polymerization is another form of addition or chain‐growth polymerization used for synthesizing linear polymers over branched polymers. The catalyst used for polymerization is the Ziegler–Natta catalyst, named after Karl Ziegler and Giulio Natta, who developed it in 1953. This catalyst is an organometallic complex of titanium tetrachloride and triethyl aluminum, with the active form of the catalyst being an alkyl titanium compound. Using the Ziegler–Natta...
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Molecular Weight of Step-Growth Polymers01:08

Molecular Weight of Step-Growth Polymers

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Step growth polymerization involves bi or multifunctional monomers. Bifunctional monomers react to form linear step growth polymers, whereas multifunctional monomers react to form non-linear or branched polymers.
As the step-growth polymerization involves step-wise condensation of monomers, the molecular weight also builds up eventually. Consequently, high molecular weight polymers are obtained at the late stages of the polymerization, where 99% of monomers have been consumed.
The extent of the...
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Anionic Chain-Growth Polymerization: Mechanism01:04

Anionic Chain-Growth Polymerization: Mechanism

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The mechanism for anionic chain-growth polymerization involves initiation, propagation, and termination steps. In the initiation step, a nucleophilic anion, such as butyl lithium, initiates the polymerization process by attacking the π bond of the vinylic monomer. As a result, a carbanion, stabilized by the electron‐withdrawing group, is generated. The resulting carbanion acts as a Michael donor in the propagation step and attacks the second vinylic monomer, which acts as a Michael...
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Controlling the Size, Shape and Stability of Supramolecular Polymers in Water
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Externally Regulated Specific Molecular Recognition Driven Pathway Selectivity in Supramolecular Polymerization.

Anwesha Chakraborty1, Rabindra Nath Manna2, Ankan Paul2

  • 1School of Applied and Interdisciplinary Sciences Indian Association for the Cultivation of Science, Kolkata, 2A and 2B Raja S. C. Mullick Road, India-, 700032.

Chemistry (Weinheim an Der Bergstrasse, Germany)
|May 12, 2021
PubMed
Summary

This study shows how 4-dimethylaminopyridine (DMAP) controls supramolecular polymerization pathways in naphthalene-diimide derivatives. DMAP addition and cooling rates dictate the formation of different nanostructures, including J-aggregates and 2D materials.

Keywords:
Externally regulated nucleation-elongationHydrogen-bondingKinetic and thermodynamic controlPathway complexitySupramolecular polymerization

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Area of Science:

  • Supramolecular Chemistry
  • Materials Science
  • Organic Chemistry

Background:

  • Naphthalene-diimide derivatives are key building blocks for functional materials.
  • Controlling supramolecular polymerization is crucial for designing nanostructures with specific properties.
  • The role of additives like 4-dimethylaminopyridine (DMAP) in directing self-assembly is not fully understood.

Purpose of the Study:

  • To investigate the effect of DMAP on the supramolecular polymerization of a naphthalene-diimide derivative (NDI-1) bearing a carboxylic acid group.
  • To elucidate how DMAP concentration and cooling rate influence the resulting aggregate morphology and assembly pathway.
  • To understand the mechanism of pathway selectivity in DMAP-regulated self-assembly.

Main Methods:

  • Supramolecular polymerization experiments using NDI-1 in decane with varying amounts of DMAP.
  • Controlled cooling rates (fast and slow) to influence nucleation and growth.
  • Characterization of the resulting aggregates (Agg-1, Agg-2, Agg-2a, Agg-3) using techniques not specified but implied by morphology analysis.
  • Computational modeling to provide insights into the assembly process and internal structure.

Main Results:

  • NDI-1 alone forms ill-defined aggregates (Agg-1) due to undirected H-bonding.
  • One mole equivalent of DMAP induces cooperative polymerization, forming J-aggregated fibrillar nanostructures (Agg-2).
  • Specific conditions (10% DMAP, fast cooling) yield J-aggregates (Agg-2a) via anti-parallel H-bonding.
  • Different conditions (2.5% DMAP, slow cooling) lead to thermodynamically controlled 2D materials (Agg-3) with face-to-face stacking.
  • Varying DMAP concentrations and cooling rates result in mixtures of aggregate types.

Conclusions:

  • DMAP acts as a crucial regulator, enabling pathway selectivity in NDI-1 supramolecular polymerization.
  • The interplay between DMAP concentration and cooling rate offers precise control over nanostructure formation.
  • Computational modeling supports the experimental findings, highlighting the complexity of the self-assembly pathways.