Promiscuous stabilisation behaviour of silicic acid by cationic macromolecules: the case of phosphonium-grafted dicationic ethylene oxide bolaamphiphiles

Demadis, Konstantinos D.; Tsistraki, Anna; Popa, Adriana; Ilia, Gheorghe; Visa, Aurelia

doi:10.1039/c1ra00448d

Cited by 15 publications

(8 citation statements)

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“…Inhibition of condensation at the later time points resulted in a decrease of silanol units in the system. A similar effect was observed in the presence of poly(ethylene glycol) [ 35 ], poly(1-vinylpyrrolidone) [ 36 ], and poly(1-vinylimidazole) [ 37 ]. These polymers form hydrogen bonds with silanol units which stabilize non-ionized –Si-OH groups, thus decreasing the condensation rate.…”

Section: Resultssupporting

confidence: 61%

Polymeric Amines and Ampholytes Derived from Poly(acryloyl chloride): Synthesis, Influence on Silicic Acid Condensation and Interaction with Nucleic Acid

et al. 2017

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Polymeric amines are intensively studied due to various valuable properties. This study describes the synthesis of new polymeric amines and ampholytes by the reaction of poly(acryloyl chloride) with trimethylene-based polyamines containing one secondary and several (1-3) tertiary amine groups. The polymers contain polyamine side chains and carboxylic groups when the polyamine was in deficiency. These polymers differ in structure of side groups, but they are identical in polymerization degree and polydispersity, which facilitates the study of composition-properties relationships. The structure of the obtained polymers was confirmed with 13 C nuclear magnetic resonance infrared spectroscopy, and acid-base properties were studied with potentiometry titration. Placement of the amine groups in the side chains influences their acid-base properties: protonation of the amine group exerts a larger impact on the amine in the same side chain than on the amines in the neighboring side chains. The obtained polymers are prone to aggregation in aqueous solutions tending to insolubility at definite pH values in the case of polyampholytes. Silicic acid condensation in the presence of new polymers results in soluble composite nanoparticles and composite materials which consist of ordered submicrometer particles according to dynamic light scattering and electron microscopy. Polymeric amines, ampholytes, and composite nanoparticles are capable of interacting with oligonucleotides, giving rise to complexes that hold promise for gene delivery applications.

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Section: Resultssupporting

confidence: 61%

Polymeric Amines and Ampholytes Derived from Poly(acryloyl chloride): Synthesis, Influence on Silicic Acid Condensation and Interaction with Nucleic Acid

et al. 2017

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“…The extent of silica stabilization (P5S3 at ∼ 100 ppm stabilizes molybdate‐reactive silica at 150–180 ppm above the additive‐free control) over 8 hours is similar to that of other polymeric additives, which are often in the 150–200 ppm range, although some additives, such as first‐generation polyaminoamide STARBURST® dendrimers achieved this stabilization level at a significantly lower concentration of 40 ppm . The lack of stabilizing capacity of P5S3 for time periods beyond 24 hours, however, is in contrast to our previous investigations involving cationic systems, such as polyaminoamide (PAMAM) dendrimers, polyethyleneimine, polyallylamine hydrochloride, cationically‐modified inulin, poly(acrylamide‐co‐diallyldimethylammonium chloride), combinations of cationic/anionic assemblies, zwitterionic chitosan‐based macromolecules, phosphonium‐based backbones . In all these cases, significant molybdate‐reactive silica stabilization is noted that depends on a plethora of factors such as polymer architecture (nature of chemical moieties, chain length), charge density, pH, etc.…”

Section: Resultssupporting

confidence: 42%

“…Vice versa , polycationic organic compounds were found to retard the condensation of silicic acid when added at low concentration (up to around 100 ppm) to supersaturated solutions of silicic acid (500 ppm, ∼ 8 m m ). Examples of these condensation‐retarding compounds are poly(vinylimidazole), polyaminoamide dendrimers, poly(acrylamide‐co‐diallyldimethylammonium chloride), polyallylamine hydrochloride, polyethyleneimine, cationically‐modified inulin, combinations of cationic/anionic assemblies, zwitterionic chitosan‐based macromolecules, and phosphonium‐grafted polyethylene glycol backbones . Furthermore, uncharged polymers such as polyethylene glycol or polyvinylpyrrolidone exerted a similar effect.…”

Section: Introductionmentioning

confidence: 99%

Pleiotropic Role of Recombinant Silaffin‐Like Cationic Polypeptide P5S3: Peptide‐Induced Silicic Acid Stabilization, Silica Formation and Inhibition of Silica Dissolution

Spinthaki

Zerfaß²,

Paulsen

et al. 2016

ChemistrySelect

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Silica-mineralizing organisms such as diatoms manage several aspects of silica chemistry when polymerizing monomeric silicic acid into amorphous silica. Silicic acid is undersaturated in the diatoms' habitats and mechanisms of enrichment and prevention of uncontrolled mineralization are not well understood. Diatom-biosilica is associated with organic compounds, including polycationic, post-translationally modified peptides termed silaffins, which induce the condensation of silicic acid under supersaturated conditions. Here, we report the pleiotropic action of the designed silaffin-like peptide P5S3, which (i) stabilizes 4-8x silicic acid (in supersaturated conditions of 8.3 mm), (ii) decelerates silica hydrolysis in non-saturated conditions (1 mm) and (iii) enhances silica precipitation at 15-30x supersaturation (30 mm), forming a composite precipitate. Abundant cationic amino acids in P5S3 can interact with silica, though blocking experiments with selected anions also indicate a role of non-electrostatic (e. g. amide-silica) interactions. This shows how silaffin-like peptides could potentially contribute to both keeping silica soluble, and forming peptide-silica precipitates.

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“…131,137,173,174 For instance, inhibition of Si(OH) 4 condensation is observed for a wide range of polymeric cations and amines. The reason for this contradiction is possibly due to the different procedures employed for measurement of monomeric silicic acid concentration.…”

Section: 135137mentioning

confidence: 99%

“…24,61,62,[65][66][67][68][69][70][71][75][76][77]98,99,[106][107][108]111,112,114,117,121,124,134,135,137,139,143,149,153,155,157 These variants exist in the case of relatively low silicon content in the system, when all PSA nanoparticles can nd chains of organic polymer. Further increase in the silicic acid content results in formation of insoluble non-uniform products 64,83 because of cross-linking by means of silicic acid which was condensed independent of the polymer control.…”

Section: Polymer : Si Ratiomentioning

confidence: 99%

Silicic acid condensation under the influence of water-soluble polymers: from biology to new materials

et al. 2017

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Silicon is among the most abundant elements on the Earth. It occurs in many minerals and plays an important role in several biochemical processes. Some living organisms use silicon dioxide as a substrate for building elements of their bodies. Unicellular diatom algae build frustules from silicon dioxide. The skeleton of siliceous sponges is a silicaprotein composite. Similarly, rice hulls which protect seeds, contain silica as an important component. The living organisms assimilate silicon from the environment in the form of silicic acid. However, the biochemical mechanisms involved in the transformation of silicic acid to solid siliceous materials are still poorly understood.Evidently, condensation of silicic acid in the living organisms proceeds under control of biopolymers and it is important to know how various types of polymers influence the condensation. Bio-inspired chemistry involving the interaction between polymeric silicic acid and functional polymers results in interesting composite materials, including nanoparticles and bulk materials. This review contains a brief description of the mechanism of silicic acid condensation in aqueous medium and also includes a discussion on various precursors of silicic acid. The main focus of the review is on the influence of polymers bearing nitrogen and oxygen-containing functional groups on silicic acid condensation starting from monomer to three-dimensional polymer. Influence of molecular weight of the organic polymer on the condensation and structure of the resulting product is also elaborated. The biological importance of the obtained data and strategies for novel applications of the synthesized composite materials are described in the concluding section of the review. The biomimetic condensation processes open up new vistas for development of novel materials and applications in the biomedical and process industries.

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Promiscuous stabilisation behaviour of silicic acid by cationic macromolecules: the case of phosphonium-grafted dicationic ethylene oxide bolaamphiphiles

Cited by 15 publications

References 50 publications

Polymeric Amines and Ampholytes Derived from Poly(acryloyl chloride): Synthesis, Influence on Silicic Acid Condensation and Interaction with Nucleic Acid

Polymeric Amines and Ampholytes Derived from Poly(acryloyl chloride): Synthesis, Influence on Silicic Acid Condensation and Interaction with Nucleic Acid

Pleiotropic Role of Recombinant Silaffin‐Like Cationic Polypeptide P5S3: Peptide‐Induced Silicic Acid Stabilization, Silica Formation and Inhibition of Silica Dissolution

Silicic acid condensation under the influence of water-soluble polymers: from biology to new materials

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