scholarly journals Concurrent self-regulated autonomous synthesis and functionalization of pH-responsive giant vesicles by a chemical pH oscillator

Soft Matter ◽  
2021 ◽  
Vol 17 (15) ◽  
pp. 4011-4018
Author(s):  
E. Poros-Tarcali ◽  
J. Perez-Mercader

pH oscillatory chemistry-driven generation of polymer vesicles from homogenous medium and their pH-responsive self-assembly in a one-pot reaction network.

2019 ◽  
Author(s):  
Liman Hou ◽  
Marta Dueñas-Diez ◽  
Rohit Srivastava ◽  
Juan Perez-Mercader

<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>


2016 ◽  
Vol 120 (48) ◽  
pp. 27533-27540 ◽  
Author(s):  
Jinglin Shen ◽  
Xia Xin ◽  
Guokui Liu ◽  
Jinyu Pang ◽  
Zhaohua Song ◽  
...  

RSC Advances ◽  
2016 ◽  
Vol 6 (46) ◽  
pp. 40418-40421 ◽  
Author(s):  
Jie Yang ◽  
Zhengtao Li ◽  
Li Shao ◽  
Guocan Yu

A novel host-guest recognition motif between a water-soluble pillar[10]arene and pyrene derivative was established and further applied in the fabrication of a pH-responsive supra-amphiphile.


2021 ◽  
Vol 9 ◽  
Author(s):  
Jinshan Guo ◽  
Eszter Poros-Tarcali ◽  
Juan Pérez-Mercader

Using the radicals generated during pH oscillations, a semibatch pH oscillator is used as the chemical fuel and engine to drive polymerization induced self-assembly (PISA) for the one-pot autonomous synthesis of functional giant vesicles. Vesicles with diameters ranging from sub-micron to ∼5 µm are generated. Radical formation is found to be switched ON/OFF and be autonomously controlled by the pH oscillator itself, inducing a periodic polymerization process. The mechanism underlying these complex processes is studied and compared to conventional (non-oscillatory) initiation by the same redox pair. The pH oscillations along with the continuous increase in salt concentration in the semibatch reactor make the self-assembled objects undergo morphological evolution. This process provides a self-regulated means for the synthesis of soft giant polymersomes and opens the door for new applications of pH oscillators in a variety of contexts, from the exploration of new geochemical scenarios for the origin of life and the autonomous emergence of the necessary free-energy and proton gradients, to the creation of active functional microreactors and programmable release of cargo molecules for pH-responsive materials.


2019 ◽  
Author(s):  
Liman Hou ◽  
Marta Dueñas-Diez ◽  
Rohit Srivastava ◽  
Juan Perez-Mercader

<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>


Molecules ◽  
2021 ◽  
Vol 26 (5) ◽  
pp. 1412
Author(s):  
Eunkyung Ji ◽  
Cian Cummins ◽  
Guillaume Fleury

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.


2015 ◽  
Vol 22 (2) ◽  
pp. 486-490 ◽  
Author(s):  
Joseph P. Byrne ◽  
Miguel Martínez-Calvo ◽  
Robert D. Peacock ◽  
Thorfinnur Gunnlaugsson

RSC Advances ◽  
2015 ◽  
Vol 5 (44) ◽  
pp. 34942-34948 ◽  
Author(s):  
Sayantan Mazumdar ◽  
Aninda J. Bhattacharyya

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.


Sign in / Sign up

Export Citation Format

Share Document