{2-Phases 2-reactions 1-catalyst} concept for the sustainable performance of coupled reactions

Schmid, Philipp; Jost, G; Grass, Xaver; Touraud, Didier; Diat, Olivier; Pfitzner, Arno; Bauduin, Pierre

doi:10.1039/d1gc04265c

“…[ 1a , 3a ] Since nano‐ion/solute co‐assembly is much stronger than for classical chaotropic ions, such as SCN − or I − , nano‐ions were termed superchaotropic ions [3] in extension to the well‐known Hofmeister series. [10] Nano‐ion co‐assembly has thus opened novel pathways to the formulation of hybrid organic/inorganic materials such as foams [8] and inorganic supramolecular networks [11] as well as catalytic [12] and drug delivery [13] applications.…”

mentioning

confidence: 99%

Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions

Hohenschutz

¹

,

Bauduin

²

,

López

³

et al. 2022

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Nanometer-sized anions (nano-ions) like polyoxometalates and boron clusters exhibit so-called superchaotropic behavior, which describes their strong binding to hydrated non-ionic matter in water. We show here that nano-ions, at millimolar concentrations, dramatically enhance the viscosity and induce gelation of aqueous solutions of non-ionic cellulose ethers (CEs), a class of widely utilized polymers known for their thickening and gel-forming ability. These phenomena arise from an interplay of attractive forces and repulsive electrostatic forces between CE-chains upon nano-ion binding. The attractive forces manifest themselves as aggregation of CE-chains into a physically crosslinked polymer network (gel). In turn, the electrostatic repulsions hamper the viscosity increase and gelation. Superchaotropic nano-ion binding emerges as a novel and general physical crosslinking motif for CE-solutions and exceeds by far the conventional thickening effects of classical salts and ionic surfactants.

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“…Accordingly, the superchaotropic properties of POMs cannot only be used for biological membrane transport, but they are transferable to artificial membranes and phase-transfer processes in general, as recently independently demonstrated for catalysis and dissolution. [13,74,75] To better mimic biological membranes, which contain negatively charged components and cholesterol, equivalent transport experiments were performed in anionic liposomes [19,20] with the prototypal POM carriers, [PVW 11 ] 4and [SiMoW 11 ] 4-. These experiments showed that, despite the apparent Coulombic repulsion, both POMs retained their carrier capabilities (Figure S8 and Table S5, Supporting Information), with only slightly reduced net efficiencies.…”

Section: Resultsmentioning

confidence: 99%

“…Accordingly, the superchaotropic properties of POMs cannot only be used for biological membrane transport, but they are transferable to artificial membranes and phase‐transfer processes in general, as recently independently demonstrated for catalysis and dissolution. [ 13,74,75 ]…”

Section: Resultsmentioning

confidence: 99%

All‐Inorganic Polyoxometalates Act as Superchaotropic Membrane Carriers

Barba‐Bon,

Gumerova,

Tanuhadi

et al. 2023

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Polyoxometalates (POMs) are known antitumoral, antibacterial, antiviral, and anticancer agents and considered as next‐generation metallodrugs. Herein, we report a new biological functionality in neutral physiological media, where selected mixed‐metal POMs are sufficiently stable and able to affect membrane transport of impermeable, hydrophilic, and cationic peptides (heptaarginine, heptalysine, protamine, and polyarginine). The uptake is observed in both, model membranes as well as cells, and attributed to the superchaotropic properties of the polyoxoanions. In view of the structural diversity of POMs these findings pave the way towards their biomedical application in drug delivery or for cell‐biological uptake studies with biological effector molecules or staining agents.This article is protected by copyright. All rights reserved

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“…[1a, 3a] Since nano-ion/solute co-assembly is much stronger than for classical chaotropic ions, such as SCN À or I À , nano-ions were termed superchaotropic ions [3] in extension to the well-known Hofmeister series. [10] Nano-ion co-assembly has thus opened novel pathways to the formulation of hybrid organic/inorganic materials such as foams [8] and inorganic supramolecular networks [11] as well as catalytic [12] and drug delivery [13] applications.…”

mentioning

confidence: 99%

Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions

Hohenschutz

¹

,

Bauduin

²

,

López

³

et al. 2022

Self Cite

View full text Add to dashboard Cite

Nanometer-sized anions (nano-ions) like polyoxometalates and boron clusters exhibit so-called superchaotropic behavior, which describes their strong binding to hydrated non-ionic matter in water. We show here that nano-ions, at millimolar concentrations, dramatically enhance the viscosity and induce gelation of aqueous solutions of non-ionic cellulose ethers (CEs), a class of widely utilized polymers known for their thickening and gel-forming ability. These phenomena arise from an interplay of attractive forces and repulsive electrostatic forces between CE-chains upon nano-ion binding. The attractive forces manifest themselves as aggregation of CE-chains into a physically crosslinked polymer network (gel). In turn, the electrostatic repulsions hamper the viscosity increase and gelation. Superchaotropic nano-ion binding emerges as a novel and general physical crosslinking motif for CE-solutions and exceeds by far the conventional thickening effects of classical salts and ionic surfactants.

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{2-Phases 2-reactions 1-catalyst} concept for the sustainable performance of coupled reactions

Abstract: In the recent years, photoredox chemistry has been intensively investigated due to its sustainability and low energy-cost. Here, we propose a physicochemical concept – called {2-phases 2-reactions 1-catalyst} – to...

Cited by 6 publications

References 88 publications

Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions

Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions

All‐Inorganic Polyoxometalates Act as Superchaotropic Membrane Carriers

Superchaotropic Nano‐ion Binding as a Gelation Motif in Cellulose Ether Solutions

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