Cargando…
Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects
Design of metallosupramolecular materials encompassing more than one kind of supramolecular interaction can become deceptive, but it is necessary to better understand the concept of the controlled formation of supramolecular systems. Herein, we show the structural diversity of the bis-compartmental...
Autores principales: | , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
|
Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10593740/ https://www.ncbi.nlm.nih.gov/pubmed/37872235 http://dx.doi.org/10.1038/s41598-023-45109-z |
_version_ | 1785124495517810688 |
---|---|
author | Marcinkowski, Dawid Kubicki, Maciej Consiglio, Giuseppe Hnatejko, Zbigniew Majcher-Fitas, Anna M. Podgajny, Robert Patroniak, Violetta Gorczyński, Adam |
author_facet | Marcinkowski, Dawid Kubicki, Maciej Consiglio, Giuseppe Hnatejko, Zbigniew Majcher-Fitas, Anna M. Podgajny, Robert Patroniak, Violetta Gorczyński, Adam |
author_sort | Marcinkowski, Dawid |
collection | PubMed |
description | Design of metallosupramolecular materials encompassing more than one kind of supramolecular interaction can become deceptive, but it is necessary to better understand the concept of the controlled formation of supramolecular systems. Herein, we show the structural diversity of the bis-compartmental phenoxo-benzimidazole ligand H(3)L(1) upon self-assembly with variety of d-block metal ions, accounting for factors such as: counterions, pH, solvent and reaction conditions. Solid-state and solution studies show that the parent ligand can accommodate different forms, related to (de)protonation and proton-transfer, resulting in the formation of mono-, bi- or tetrametallic architectures, which was also confirmed with control studies on the new mono-compartmental phenoxo-benzimidazole H(2)L(2) ligand analogue. For the chosen architectures, structural variables such as porous character, magnetic behaviour or luminescence studies were studied to demonstrate how the form of H(3)L(1) ligand affects the final form of the supramolecular architecture and observed properties. Such complex structural variations within the benzimidazole-phenoxo-type ligand have been demonstrated for the first time and this proof-of-concept can be used to integrate these principles in more sophisticated architectures in the future, combining both the benzimidazole and phenoxide subunits. Ultimately, those principles could be utilized for targeted manipulation of properties through molecular tectonics and crystal engineering aspects. |
format | Online Article Text |
id | pubmed-10593740 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-105937402023-10-25 Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects Marcinkowski, Dawid Kubicki, Maciej Consiglio, Giuseppe Hnatejko, Zbigniew Majcher-Fitas, Anna M. Podgajny, Robert Patroniak, Violetta Gorczyński, Adam Sci Rep Article Design of metallosupramolecular materials encompassing more than one kind of supramolecular interaction can become deceptive, but it is necessary to better understand the concept of the controlled formation of supramolecular systems. Herein, we show the structural diversity of the bis-compartmental phenoxo-benzimidazole ligand H(3)L(1) upon self-assembly with variety of d-block metal ions, accounting for factors such as: counterions, pH, solvent and reaction conditions. Solid-state and solution studies show that the parent ligand can accommodate different forms, related to (de)protonation and proton-transfer, resulting in the formation of mono-, bi- or tetrametallic architectures, which was also confirmed with control studies on the new mono-compartmental phenoxo-benzimidazole H(2)L(2) ligand analogue. For the chosen architectures, structural variables such as porous character, magnetic behaviour or luminescence studies were studied to demonstrate how the form of H(3)L(1) ligand affects the final form of the supramolecular architecture and observed properties. Such complex structural variations within the benzimidazole-phenoxo-type ligand have been demonstrated for the first time and this proof-of-concept can be used to integrate these principles in more sophisticated architectures in the future, combining both the benzimidazole and phenoxide subunits. Ultimately, those principles could be utilized for targeted manipulation of properties through molecular tectonics and crystal engineering aspects. Nature Publishing Group UK 2023-10-23 /pmc/articles/PMC10593740/ /pubmed/37872235 http://dx.doi.org/10.1038/s41598-023-45109-z Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article's Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article's Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) . |
spellingShingle | Article Marcinkowski, Dawid Kubicki, Maciej Consiglio, Giuseppe Hnatejko, Zbigniew Majcher-Fitas, Anna M. Podgajny, Robert Patroniak, Violetta Gorczyński, Adam Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title | Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title_full | Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title_fullStr | Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title_full_unstemmed | Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title_short | Unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
title_sort | unexpected structural complexity of d-block metallosupramolecular architectures within the benzimidazole-phenoxo ligand scaffold for crystal engineering aspects |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10593740/ https://www.ncbi.nlm.nih.gov/pubmed/37872235 http://dx.doi.org/10.1038/s41598-023-45109-z |
work_keys_str_mv | AT marcinkowskidawid unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT kubickimaciej unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT consigliogiuseppe unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT hnatejkozbigniew unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT majcherfitasannam unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT podgajnyrobert unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT patroniakvioletta unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects AT gorczynskiadam unexpectedstructuralcomplexityofdblockmetallosupramoleculararchitectureswithinthebenzimidazolephenoxoligandscaffoldforcrystalengineeringaspects |