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Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone
The synthesis of heterogeneous cooperative catalysts in which two or more catalytically active components are spatially separated within a single material has generated considerable research efforts. The multiple functionalities of catalysts can significantly improve the efficiency of existing organ...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Frontiers Media S.A.
2019
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6367244/ https://www.ncbi.nlm.nih.gov/pubmed/30775365 http://dx.doi.org/10.3389/fchem.2019.00042 |
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author | Cai, Xiaoxiong Xu, Qionghao Tu, Gaomei Fu, Yanghe Zhang, Fumin Zhu, Weidong |
author_facet | Cai, Xiaoxiong Xu, Qionghao Tu, Gaomei Fu, Yanghe Zhang, Fumin Zhu, Weidong |
author_sort | Cai, Xiaoxiong |
collection | PubMed |
description | The synthesis of heterogeneous cooperative catalysts in which two or more catalytically active components are spatially separated within a single material has generated considerable research efforts. The multiple functionalities of catalysts can significantly improve the efficiency of existing organic chemical transformations. Herein, we introduce ruthenium (Ru) nanoparticles (NPs) on the surfaces of a metal–organic framework pre-encapsulated with polyoxometalate silicotungstic acid (SiW) UiO−66 (University of Oslo [UiO]) and prepared a 2.0% Ru/11.7% SiW@UiO−66 porous hybrid using the impregnation method. The close synergistic effect of metal Ru NPs, SiW, and UiO-66 endow 2.0% Ru/11.7% SiW@UiO-66 with increased activity and stability for complete methyl levulinate (ML) conversion and exclusive γ-valerolactone (GVL) selectivity at mild conditions of 80°C and at a H(2) pressure of 0.5 MPa. Effectively, this serves as a model reaction for the upgrading of biomass and outperforms the performances of the constituent parts and that of the physical mixture (SiW + Ru/UiO−66). The highly dispersed Ru NPs act as active centers for hydrogenation, while the SiW molecules possess Brønsted acidic sites that cooperatively promote the subsequent lactonization of MHV to generate GVL, and the UiO−66 crystal accelerates the mass transportation facilitated by its own porous structure with a large surface area. |
format | Online Article Text |
id | pubmed-6367244 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | Frontiers Media S.A. |
record_format | MEDLINE/PubMed |
spelling | pubmed-63672442019-02-15 Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone Cai, Xiaoxiong Xu, Qionghao Tu, Gaomei Fu, Yanghe Zhang, Fumin Zhu, Weidong Front Chem Chemistry The synthesis of heterogeneous cooperative catalysts in which two or more catalytically active components are spatially separated within a single material has generated considerable research efforts. The multiple functionalities of catalysts can significantly improve the efficiency of existing organic chemical transformations. Herein, we introduce ruthenium (Ru) nanoparticles (NPs) on the surfaces of a metal–organic framework pre-encapsulated with polyoxometalate silicotungstic acid (SiW) UiO−66 (University of Oslo [UiO]) and prepared a 2.0% Ru/11.7% SiW@UiO−66 porous hybrid using the impregnation method. The close synergistic effect of metal Ru NPs, SiW, and UiO-66 endow 2.0% Ru/11.7% SiW@UiO-66 with increased activity and stability for complete methyl levulinate (ML) conversion and exclusive γ-valerolactone (GVL) selectivity at mild conditions of 80°C and at a H(2) pressure of 0.5 MPa. Effectively, this serves as a model reaction for the upgrading of biomass and outperforms the performances of the constituent parts and that of the physical mixture (SiW + Ru/UiO−66). The highly dispersed Ru NPs act as active centers for hydrogenation, while the SiW molecules possess Brønsted acidic sites that cooperatively promote the subsequent lactonization of MHV to generate GVL, and the UiO−66 crystal accelerates the mass transportation facilitated by its own porous structure with a large surface area. Frontiers Media S.A. 2019-02-01 /pmc/articles/PMC6367244/ /pubmed/30775365 http://dx.doi.org/10.3389/fchem.2019.00042 Text en Copyright © 2019 Cai, Xu, Tu, Fu, Zhang and Zhu. http://creativecommons.org/licenses/by/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution License (CC BY). The use, distribution or reproduction in other forums is permitted, provided the original author(s) and the copyright owner(s) are credited and that the original publication in this journal is cited, in accordance with accepted academic practice. No use, distribution or reproduction is permitted which does not comply with these terms. |
spellingShingle | Chemistry Cai, Xiaoxiong Xu, Qionghao Tu, Gaomei Fu, Yanghe Zhang, Fumin Zhu, Weidong Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title | Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title_full | Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title_fullStr | Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title_full_unstemmed | Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title_short | Synergistic Catalysis of Ruthenium Nanoparticles and Polyoxometalate Integrated Within Single UiO−66 Microcrystals for Boosting the Efficiency of Methyl Levulinate to γ-Valerolactone |
title_sort | synergistic catalysis of ruthenium nanoparticles and polyoxometalate integrated within single uio−66 microcrystals for boosting the efficiency of methyl levulinate to γ-valerolactone |
topic | Chemistry |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6367244/ https://www.ncbi.nlm.nih.gov/pubmed/30775365 http://dx.doi.org/10.3389/fchem.2019.00042 |
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