Cargando…

Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction

[Image: see text] The increase in demand for Pd and its low abundance pose a significant threat to its future availability, rendering research into more sustainable Pd-based technologies essential. Herein, we report Pd scavenging mechanically robust hybrid gel beads composed of agarose, a polymer ge...

Descripción completa

Detalles Bibliográficos
Autores principales: Albino, Matteo, Burden, Thomas J., Piras, Carmen C., Whitwood, Adrian C., Fairlamb, Ian J. S., Smith, David K.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9906743/
https://www.ncbi.nlm.nih.gov/pubmed/36778525
http://dx.doi.org/10.1021/acssuschemeng.2c05484
_version_ 1784884039007600640
author Albino, Matteo
Burden, Thomas J.
Piras, Carmen C.
Whitwood, Adrian C.
Fairlamb, Ian J. S.
Smith, David K.
author_facet Albino, Matteo
Burden, Thomas J.
Piras, Carmen C.
Whitwood, Adrian C.
Fairlamb, Ian J. S.
Smith, David K.
author_sort Albino, Matteo
collection PubMed
description [Image: see text] The increase in demand for Pd and its low abundance pose a significant threat to its future availability, rendering research into more sustainable Pd-based technologies essential. Herein, we report Pd scavenging mechanically robust hybrid gel beads composed of agarose, a polymer gelator (PG), and an active low-molecular-weight gelator (LMWG) based on 1,3:2,4-dibenzylidenesorbitol (DBS), DBS-CONHNH(2). The robustness of the PG and the ability of the LMWG to reduce Pd(II) in situ to generate naked Pd(0) nanoparticles (PdNPs) combine within these gel beads to give them potential as practical catalysts for Suzuki–Miyaura cross-coupling reactions. The optimized gel beads demonstrate good reusability, green metrics, and most importantly the ability to sustain stirring, improving reaction times and energy consumption compared to previous examples. In contrast to previous reports, the leaching of palladium from these next-generation beads is almost completely eliminated. Additionally, for the first time, a detailed investigation of these Pd-loaded gel beads explains precisely how the nanoparticles are formed in situ without a stabilizing ligand. Further, detailed catalytic investigations demonstrate that catalysis occurs within the gel beads. Hence, these beads can essentially be considered as robust “nonligated” heterogeneous PdNP catalysts. Given the challenges in developing ligand-free, naked Pd nanoparticles as stable catalysts, these gel beads may have future potential for the development of easily used systems to perform chemical reactions in “kit” form.
format Online
Article
Text
id pubmed-9906743
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-99067432023-02-08 Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction Albino, Matteo Burden, Thomas J. Piras, Carmen C. Whitwood, Adrian C. Fairlamb, Ian J. S. Smith, David K. ACS Sustain Chem Eng [Image: see text] The increase in demand for Pd and its low abundance pose a significant threat to its future availability, rendering research into more sustainable Pd-based technologies essential. Herein, we report Pd scavenging mechanically robust hybrid gel beads composed of agarose, a polymer gelator (PG), and an active low-molecular-weight gelator (LMWG) based on 1,3:2,4-dibenzylidenesorbitol (DBS), DBS-CONHNH(2). The robustness of the PG and the ability of the LMWG to reduce Pd(II) in situ to generate naked Pd(0) nanoparticles (PdNPs) combine within these gel beads to give them potential as practical catalysts for Suzuki–Miyaura cross-coupling reactions. The optimized gel beads demonstrate good reusability, green metrics, and most importantly the ability to sustain stirring, improving reaction times and energy consumption compared to previous examples. In contrast to previous reports, the leaching of palladium from these next-generation beads is almost completely eliminated. Additionally, for the first time, a detailed investigation of these Pd-loaded gel beads explains precisely how the nanoparticles are formed in situ without a stabilizing ligand. Further, detailed catalytic investigations demonstrate that catalysis occurs within the gel beads. Hence, these beads can essentially be considered as robust “nonligated” heterogeneous PdNP catalysts. Given the challenges in developing ligand-free, naked Pd nanoparticles as stable catalysts, these gel beads may have future potential for the development of easily used systems to perform chemical reactions in “kit” form. American Chemical Society 2023-01-24 /pmc/articles/PMC9906743/ /pubmed/36778525 http://dx.doi.org/10.1021/acssuschemeng.2c05484 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/).
spellingShingle Albino, Matteo
Burden, Thomas J.
Piras, Carmen C.
Whitwood, Adrian C.
Fairlamb, Ian J. S.
Smith, David K.
Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title_full Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title_fullStr Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title_full_unstemmed Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title_short Mechanically Robust Hybrid Gel Beads Loaded with “Naked” Palladium Nanoparticles as Efficient, Reusable, and Sustainable Catalysts for the Suzuki–Miyaura Reaction
title_sort mechanically robust hybrid gel beads loaded with “naked” palladium nanoparticles as efficient, reusable, and sustainable catalysts for the suzuki–miyaura reaction
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9906743/
https://www.ncbi.nlm.nih.gov/pubmed/36778525
http://dx.doi.org/10.1021/acssuschemeng.2c05484
work_keys_str_mv AT albinomatteo mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction
AT burdenthomasj mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction
AT pirascarmenc mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction
AT whitwoodadrianc mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction
AT fairlambianjs mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction
AT smithdavidk mechanicallyrobusthybridgelbeadsloadedwithnakedpalladiumnanoparticlesasefficientreusableandsustainablecatalystsforthesuzukimiyaurareaction