Cargando…

Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions

A family of microporous and robust Ln(iii)-based metal–organic frameworks (1-Ln, Ln = Sm, Eu, Gd, Tb, Dy, Ho, Er, Yb) have been obtained using 4,4′,4′′-nitrilotribenzoic acid (H(3)NTB) in NMP–HCl solvent. Both single-crystal and powder X-ray diffraction analyses demonstrate that 1-Ln are isostructur...

Descripción completa

Detalles Bibliográficos
Autores principales: Si, Xuezhen, Pan, Xuze, Xue, Jintang, Yao, Qingxia, Huang, Xianqiang, Duan, Wenzeng, Qiu, Yi, Su, Jie, Cao, Minglei, Li, Jun
Formato: Online Artículo Texto
Lenguaje:English
Publicado: The Royal Society of Chemistry 2022
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9682443/
https://www.ncbi.nlm.nih.gov/pubmed/36505724
http://dx.doi.org/10.1039/d2ra06545b
_version_ 1784834852836605952
author Si, Xuezhen
Pan, Xuze
Xue, Jintang
Yao, Qingxia
Huang, Xianqiang
Duan, Wenzeng
Qiu, Yi
Su, Jie
Cao, Minglei
Li, Jun
author_facet Si, Xuezhen
Pan, Xuze
Xue, Jintang
Yao, Qingxia
Huang, Xianqiang
Duan, Wenzeng
Qiu, Yi
Su, Jie
Cao, Minglei
Li, Jun
author_sort Si, Xuezhen
collection PubMed
description A family of microporous and robust Ln(iii)-based metal–organic frameworks (1-Ln, Ln = Sm, Eu, Gd, Tb, Dy, Ho, Er, Yb) have been obtained using 4,4′,4′′-nitrilotribenzoic acid (H(3)NTB) in NMP–HCl solvent. Both single-crystal and powder X-ray diffraction analyses demonstrate that 1-Ln are isostructural and possess 3D frameworks with permanent porosity for Ar and CO(2) adsorption. Strikingly, the incorporation of both Lewis acidic lanthanide ions and the basic triphenylamine group into 1-Ln makes them efficient acid–base catalysts for both cycloaddition of epoxides with CO(2) and one-pot cascade deacetalization–Knoevenagel reactions. The systematic catalytic studies show that 1-Tb and 1-Yb possess the best catalytic activities for both reactions, indicating the catalytic activities of these Ln-MOFs are strongly dependent on metal Lewis acid sites embedded in the frameworks.
format Online
Article
Text
id pubmed-9682443
institution National Center for Biotechnology Information
language English
publishDate 2022
publisher The Royal Society of Chemistry
record_format MEDLINE/PubMed
spelling pubmed-96824432022-12-08 Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions Si, Xuezhen Pan, Xuze Xue, Jintang Yao, Qingxia Huang, Xianqiang Duan, Wenzeng Qiu, Yi Su, Jie Cao, Minglei Li, Jun RSC Adv Chemistry A family of microporous and robust Ln(iii)-based metal–organic frameworks (1-Ln, Ln = Sm, Eu, Gd, Tb, Dy, Ho, Er, Yb) have been obtained using 4,4′,4′′-nitrilotribenzoic acid (H(3)NTB) in NMP–HCl solvent. Both single-crystal and powder X-ray diffraction analyses demonstrate that 1-Ln are isostructural and possess 3D frameworks with permanent porosity for Ar and CO(2) adsorption. Strikingly, the incorporation of both Lewis acidic lanthanide ions and the basic triphenylamine group into 1-Ln makes them efficient acid–base catalysts for both cycloaddition of epoxides with CO(2) and one-pot cascade deacetalization–Knoevenagel reactions. The systematic catalytic studies show that 1-Tb and 1-Yb possess the best catalytic activities for both reactions, indicating the catalytic activities of these Ln-MOFs are strongly dependent on metal Lewis acid sites embedded in the frameworks. The Royal Society of Chemistry 2022-11-23 /pmc/articles/PMC9682443/ /pubmed/36505724 http://dx.doi.org/10.1039/d2ra06545b Text en This journal is © The Royal Society of Chemistry https://creativecommons.org/licenses/by-nc/3.0/
spellingShingle Chemistry
Si, Xuezhen
Pan, Xuze
Xue, Jintang
Yao, Qingxia
Huang, Xianqiang
Duan, Wenzeng
Qiu, Yi
Su, Jie
Cao, Minglei
Li, Jun
Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title_full Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title_fullStr Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title_full_unstemmed Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title_short Robust acid–base Ln-MOFs: searching for efficient catalysts in cycloaddition of CO(2) with epoxides and cascade deacetalization–Knoevenagel reactions
title_sort robust acid–base ln-mofs: searching for efficient catalysts in cycloaddition of co(2) with epoxides and cascade deacetalization–knoevenagel reactions
topic Chemistry
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9682443/
https://www.ncbi.nlm.nih.gov/pubmed/36505724
http://dx.doi.org/10.1039/d2ra06545b
work_keys_str_mv AT sixuezhen robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT panxuze robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT xuejintang robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT yaoqingxia robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT huangxianqiang robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT duanwenzeng robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT qiuyi robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT sujie robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT caominglei robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions
AT lijun robustacidbaselnmofssearchingforefficientcatalystsincycloadditionofco2withepoxidesandcascadedeacetalizationknoevenagelreactions