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Growing Polymer Vesicles Generated by Polymerization Induced Self-Assembly Coupled With a Living Chemical Reactor.

ABSTRACT: Chemical oscillatory reactions have attracted intensive attention due to their autonomous, continuous, and periodic features. Herein, the radicals generated in Belousov-Zhabotinsky (BZ) oscillator was used to initiate RAFT (reversible addition-fragmentation chain transfer) polymerization of 2-methoxyethyl acrylate (MEA) extending from hydrophilic poly(ethylene glycol) chain transfer agent (PEG-CTA) to give amphiphilic block copolymer, which self-assembled into collective objects with a size ranging from sub-micron to micron. Small-to-giant polymer vesicles could be generated using the above-mentioned BZ-PISA technology, the encapsulation of active BZ recipe into the vesicles also endorses the vesicles with growing features with potential for drug delivery and biomedical applications.

SUBMITTER: Lu Z

PROVIDER: S-EPMC7490293 | biostudies-literature | 2020

REPOSITORIES: biostudies-literature

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Growing Polymer Vesicles Generated by Polymerization Induced Self-Assembly Coupled With a Living Chemical Reactor.

Lu Zhihui Z Guo Jinshan J

Frontiers in bioengineering and biotechnology 20200901

Chemical oscillatory reactions have attracted intensive attention due to their autonomous, continuous, and periodic features. Herein, the radicals generated in Belousov-Zhabotinsky (BZ) oscillator was used to initiate RAFT (reversible addition-fragmentation chain transfer) polymerization of 2-methoxyethyl acrylate (MEA) extending from hydrophilic poly(ethylene glycol) chain transfer agent (PEG-CTA) to give amphiphilic block copolymer, which self-assembled into collective objects with a size rang ...[more]

PMID: 32984286

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Project description:The RNA world is one of the principal hypotheses to explain the emergence of living systems on the prebiotic Earth. It posits that RNA oligonucleotides acted as both carriers of information as well as catalytic molecules, promoting their own replication. However, it does not explain the origin of the catalytic RNA molecules. How could the transition from a pre-RNA to an RNA world occur? A starting point to answer this question is to analyze the dynamics in sequence space on the lowest level, where mononucleotide and short oligonucleotides come together and collectively evolve into larger molecules. To this end, we study the sequence-dependent self-assembly of polymers from a random initial pool of short building blocks via templated ligation. Templated ligation requires two strands that are hybridized adjacently on a third strand. The thermodynamic stability of such a configuration crucially depends on the sequence context and, therefore, significantly influences the ligation probability. However, the sequence context also has a kinetic effect, since non-complementary nucleotide pairs in the vicinity of the ligation site stall the ligation reaction. These sequence-dependent thermodynamic and kinetic effects are explicitly included in our stochastic model. Using this model, we investigate the system-level dynamics inside a non-equilibrium 'RNA reactor' enabling a fast chemical activation of the termini of interacting oligomers. Moreover, the RNA reactor subjects the oligomer pool to periodic temperature changes inducing the reshuffling of the system. The binding stability of strands typically grows with the number of complementary nucleotides forming the hybridization site. While shorter strands unbind spontaneously during the cold phase, larger complexes only disassemble during the temperature peaks. Inside the RNA reactor, strand growth is balanced by cleavage via hydrolysis, such that the oligomer pool eventually reaches a non-equilibrium stationary state characterized by its length and sequence distribution. How do motif-dependent energy and stalling parameters affect the sequence composition of the pool of long strands? As a critical factor for self-enhancing sequence selection, we identify kinetic stalling due to non-complementary base pairs at the ligation site. Kinetic stalling enables cascades of self-amplification that result in a strong reduction of occupied states in sequence space. Moreover, we discuss the significance of the symmetry breaking for the transition from a pre-RNA to an RNA world.

Dataset Information

Growing Polymer Vesicles Generated by Polymerization Induced Self-Assembly Coupled With a Living Chemical Reactor.

Publications

Growing Polymer Vesicles Generated by Polymerization Induced Self-Assembly Coupled With a Living Chemical Reactor.

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