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Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers

Five novel disiloxane compounds comprising guanidinium and pyridinium moieties were obtained with high yields and purity. The verified synthetic pathways were then applied for modification of pre-functionalized silica gel, producing materials with the analogous organic side-chains. These halide-cont...

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Autores principales: Tabisz, Łukasz, Tukibayeva, Ainur, Pankiewicz, Radoslaw, Dobielska, Marta, Leska, Boguslawa
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Public Library of Science 2015
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4699886/
https://www.ncbi.nlm.nih.gov/pubmed/26714187
http://dx.doi.org/10.1371/journal.pone.0145680
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author Tabisz, Łukasz
Tukibayeva, Ainur
Pankiewicz, Radoslaw
Dobielska, Marta
Leska, Boguslawa
author_facet Tabisz, Łukasz
Tukibayeva, Ainur
Pankiewicz, Radoslaw
Dobielska, Marta
Leska, Boguslawa
author_sort Tabisz, Łukasz
collection PubMed
description Five novel disiloxane compounds comprising guanidinium and pyridinium moieties were obtained with high yields and purity. The verified synthetic pathways were then applied for modification of pre-functionalized silica gel, producing materials with the analogous organic side-chains. These halide-containing compounds and materials were then compared as to their ion-exchange properties: two disiloxanes proved to be effective in leaching different anions (nitrate, benzoate and ascorbate) from solid to organic phase, and pyridinium-functionalized silica gels showed selectivity towards perchlorate ion, removing it from methanolic solutions with preference to other singly charged anions. The results presented demonstrate that both compounds and materials containing silicon-carbon bonds can be produced using the same methodology, but offer strikingly different application opportunities. Comparison of their properties provides additional insight into the binding mode of different anions and hints at how the transition from a flexible siloxane bridge to immobilization on solid surface influences anion-binding selectivity. Additionally, one of the siloxane dipodands was found to form a crystalline and poorly soluble nitrate salt (1.316 g/L, water), although it was miscible with a wide range of solvents as a hydrochloride. A possible explanation is given with the help of semi-empirical calculations. A simple, time- and cost-efficient automated potentiometric titration methodology was used as a viable analytical tool for studying ion-exchange processes for both compounds and materials, in addition to standard NMR, FT-IR and ESI-MS methods.
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spelling pubmed-46998862016-01-14 Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers Tabisz, Łukasz Tukibayeva, Ainur Pankiewicz, Radoslaw Dobielska, Marta Leska, Boguslawa PLoS One Research Article Five novel disiloxane compounds comprising guanidinium and pyridinium moieties were obtained with high yields and purity. The verified synthetic pathways were then applied for modification of pre-functionalized silica gel, producing materials with the analogous organic side-chains. These halide-containing compounds and materials were then compared as to their ion-exchange properties: two disiloxanes proved to be effective in leaching different anions (nitrate, benzoate and ascorbate) from solid to organic phase, and pyridinium-functionalized silica gels showed selectivity towards perchlorate ion, removing it from methanolic solutions with preference to other singly charged anions. The results presented demonstrate that both compounds and materials containing silicon-carbon bonds can be produced using the same methodology, but offer strikingly different application opportunities. Comparison of their properties provides additional insight into the binding mode of different anions and hints at how the transition from a flexible siloxane bridge to immobilization on solid surface influences anion-binding selectivity. Additionally, one of the siloxane dipodands was found to form a crystalline and poorly soluble nitrate salt (1.316 g/L, water), although it was miscible with a wide range of solvents as a hydrochloride. A possible explanation is given with the help of semi-empirical calculations. A simple, time- and cost-efficient automated potentiometric titration methodology was used as a viable analytical tool for studying ion-exchange processes for both compounds and materials, in addition to standard NMR, FT-IR and ESI-MS methods. Public Library of Science 2015-12-29 /pmc/articles/PMC4699886/ /pubmed/26714187 http://dx.doi.org/10.1371/journal.pone.0145680 Text en © 2015 Tabisz et al http://creativecommons.org/licenses/by/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original author and source are properly credited.
spellingShingle Research Article
Tabisz, Łukasz
Tukibayeva, Ainur
Pankiewicz, Radoslaw
Dobielska, Marta
Leska, Boguslawa
Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title_full Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title_fullStr Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title_full_unstemmed Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title_short Disiloxanes and Functionalized Silica Gels: One Route, Two Complementary Outcomes—Guanidinium and Pyridinium Ion-Exchangers
title_sort disiloxanes and functionalized silica gels: one route, two complementary outcomes—guanidinium and pyridinium ion-exchangers
topic Research Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4699886/
https://www.ncbi.nlm.nih.gov/pubmed/26714187
http://dx.doi.org/10.1371/journal.pone.0145680
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