Living supramolecular polymerization

Mukhopadhyay, Rahul; Ajayaghosh, Ayyappanpillai

doi:10.1126/science.aac7422

Cited by 177 publications

(115 citation statements)

References 12 publications

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“…In this regard, gels made up of Bodipy-based fluorescent ET donor (16)-acceptor (17) molecules containing aldehyde moieties and acyl hydrazine (18) have been reported to have a combination of both the ET and self-healing ability ( Figure 7). 56 Cross-reactivity of acyl-hydrazine and aldehyde moieties has been regarded as the basis behind this dynamic covalent chemistry leading to sol-gel transition as well as repairing of the mechanically damaged gel film.…”

Section: Bodipy-derived Supramolecular Gelatorsmentioning

confidence: 99%

“…46,47 For instance, self-assembly of block copolymers with multi-color fluorophores is considered to be an emerging strategy to construct multifunctional structures with a high degree of spatial control. 7,18 In particular, crystallization-driven self-assembly of block copolymers is a useful synthetic tool to prepare complex nanoscale architectures. For example, Bodipy functionalized block copolymers containing crystallizable polyferrocenyldimethylsilane (PFS) block was used in the crystallizationdriven self-assembly to form segmented cylindrical micelles.…”

Section: Self-assembly Of Bodipy-linked Polymersmentioning

confidence: 99%

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Self-Assembly of Bodipy-Derived Extended π-Systems

Cherumukkil

Vedhanarayanan

Das

et al. 2017

Bulletin of the Chemical Society of Japan

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Self-assembly is a viable approach to create soft functional materials with architectural diversity and property variations. Among the large number of different chromophores used, borondipyrromethene (Bodipy) dyes find a unique space because of their promising photophysical properties such as high molar absorptivity, fluorescent quantum yield and excellent photostability along with the associated synthetic ease. Recently, research on Bodipy dyes has experienced a surge of activities in view of favorable self-assembling properties. In this review, recent developments in self-assembled Bodipy dyes and their significance in various applications are discussed.

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Section: Bodipy-derived Supramolecular Gelatorsmentioning

confidence: 99%

Section: Self-assembly Of Bodipy-linked Polymersmentioning

confidence: 99%

Self-Assembly of Bodipy-Derived Extended π-Systems

Cherumukkil

Vedhanarayanan

Das

et al. 2017

Bulletin of the Chemical Society of Japan

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“…10,[420][421][422] Alternatively, the manipulation of self-assembly pathways was very recently achieved via the rational design of selfassembling small molecular weight building blocks by three different groups. [423][424][425] Sugiyasu, Takeuchi and coworkers have been able to show that seed-induced growth in combination with a competing off-pathway aggregation leads to a "living" supramolecular polymerization of a Zn(II)-porphyrin dye ZnP4 in apolar methylcyclohexan (MCH). 36,426 The competing off-pathway porphyrin J-aggregates with a nanoparticle morphology are formed through isodesmic growth, and act as a kinetic trap that consumes monomers from solution (Fig.…”

Section: Living Supramolecular Polymerizationmentioning

confidence: 99%

Controlling supramolecular polymerization through multicomponent self‐assembly

Besenius

2016

J. Polym. Sci. Part A: Polym. Chem.

127

102

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The self-assembly into supramolecular polymers is a process driven by reversible non-covalent interactions between monomers, and gives access to materials applications incorporating mechanical, biological, optical or electronic functionalities. Compared to the achievements in precision polymer synthesis via living and controlled covalent polymerization processes, supramolecular chemists have only just learned how to developed strategies that allow similar control over polymer length, (co)monomer sequence and morphology (random, alternating or blocked ordering). This highlight article discusses the unique opportunities that arise when coassembling multicomponent supramolecular polymers, and focusses on four strategies in order to control the polymer architecture, size, stability and its stimuli-responsive properties: (1) endcapping of supramolecular polymers, (2) biomimetic templated polymerization, (3) controlled selectivity and reactivity in supramolecular copolymerization, and (4) living supramolecular polymerization. In contrast to the traditional focus on equilibrium systems, our emphasis is also on the manipulation of selfassembly kinetics of synthetic supramolecular systems. V C 2016

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“…The non-covalent nature of SPs brings the additional feature of reversibility of the polymerization process. [28][29][30][31][32][33][34] Furthermore, it enables the formation of polymers with a high DNA grafting density. 25, 26 Herein we describe the hierarchical organization of DNA-grafted SPs.…”

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confidence: 99%

From Ribbons to Networks: Hierarchical Organization of DNA-Grafted Supramolecular Polymers

2015

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DNA-grafted supramolecular polymers (SPs) allow the programmed organization of DNA in a highly regular, one-dimensional array. Oligonucleotides are arranged along the edges of pyrene-based helical polymers. Addition of complementary oligonucleotides triggers the assembly of individual nanoribbons resulting in the formation of extended supramolecular networks. Network formation is enabled by cooperative coaxial stacking interactions of terminal GC base pairs. The process is accompanied by structural changes in the pyrene polymer core that can be followed spectroscopically. Network formation is reversible and disassembly into individual ribbons is realized either via thermal denaturation or by addition of a DNA separator strand.The creation of functional nanoscale structures represents a major goal of today's nanotechnology. DNA-based materials are of primary interest for the construction of functional platforms. [1][2][3][4] Proper choice of the nucleotide sequence provides control over aromatic stacking and hydrogen bonding interactions, 5-7 thus enabling the assembly of systems with a high degree of complexity. [8][9][10][11] Approaches towards the preparation of functional DNA materials include the designed DNA self-assembly, 12-15 the grafting of oligonucleotides onto metal nanoparticles (NPs) 16 and other surfaces, [17][18][19] as well as polymers. [20][21][22][23] The latter class, DNA-grafted polymers, has been pioneered by Nguyen and Mirkin and gained increasing attention over the last years. 24,25 We have recently introduced DNA-grafted supramolecular polymers (SPs). 26 These self-assembled structures appear as one-dimensional (1D) ribbons, consisting of an oligopyrenotide core 27 with arrays of singlestranded oligonucleotides appended onto its edges. The non-covalent nature of SPs brings the additional feature of reversibility of the polymerization process. [28][29][30][31][32][33][34] Furthermore, it enables the formation of polymers with a high DNA grafting density. 25,26 Herein we describe the hierarchical organization of DNA-grafted SPs. It is shown that individual ribbons assemble into extended networks through a highly cooperative mesh of DNA blunt end stacking interactions.Chimeric oligomers Py-a, Py-b and Py-c (Scheme 1) are all composed of a heptapyrenotide part and an appended oligonucleotide.They were prepared via solid-phase synthesis, purified by RP-HPLC and characterized by MS (SI). The two complementary oligonucleotides 1a (separator strand) and 1b (connector strand) have the same nucleobase sequence as the respective corresponding chimeric oligomers Py-a and Py-b; 1c is complementary to the oligonucleotide part of Py-c. DNA-grafted SPs are typically performed by slow annealing. Thus, a 2 μM solution of Py-a in aqueous buffer (10 mM sodium phosphate, pH=7.0 and 250 mM sodium chloride) is cooled from 95° to 20°C using a gradient of 0.1°C/min. Stacking interactions between pyrenes drive the self-assembly of polymeric ribbons. The polymerization process leads to the development ...

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Living supramolecular polymerization

Abstract: Greater control is achieved over the chain growth and properties of dynamic materials

Cited by 177 publications

References 12 publications

Self-Assembly of Bodipy-Derived Extended π-Systems

Self-Assembly of Bodipy-Derived Extended π-Systems

Controlling supramolecular polymerization through multicomponent self‐assembly

From Ribbons to Networks: Hierarchical Organization of DNA-Grafted Supramolecular Polymers

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