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Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons
The catalytic activity of alloy nanoparticles depends on the particle size and composition ratio of different metals. Alloy nanoparticles composed of Pd, Pt, and Au are widely used as catalysts for oxidation reactions. The catalytic activities of Pt and Au nanoparticles in oxidation reactions are kn...
Autores principales: | , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Association for the Advancement of Science
2017
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5529056/ https://www.ncbi.nlm.nih.gov/pubmed/28782020 http://dx.doi.org/10.1126/sciadv.1700101 |
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author | Takahashi, Masaki Koizumi, Hiromu Chun, Wang-Jae Kori, Makoto Imaoka, Takane Yamamoto, Kimihisa |
author_facet | Takahashi, Masaki Koizumi, Hiromu Chun, Wang-Jae Kori, Makoto Imaoka, Takane Yamamoto, Kimihisa |
author_sort | Takahashi, Masaki |
collection | PubMed |
description | The catalytic activity of alloy nanoparticles depends on the particle size and composition ratio of different metals. Alloy nanoparticles composed of Pd, Pt, and Au are widely used as catalysts for oxidation reactions. The catalytic activities of Pt and Au nanoparticles in oxidation reactions are known to increase as the particle size decreases and to increase on the metal-metal interface of alloy nanoparticles. Therefore, multimetallic nanoclusters (MNCs) around 1 nm in diameter have potential as catalysts for oxidation reactions. However, there have been few reports describing the preparation of uniform alloy nanoclusters. We report the synthesis of finely controlled MNCs (around 1 nm) using a macromolecular template with coordination sites arranged in a gradient of basicity. We reveal that Cu-Pt-Au MNCs supported on graphitized mesoporous carbon show catalytic activity that is 24 times greater than that of a commercially available Pt catalyst for aerobic oxidation of hydrocarbons. In addition, solvent-free aerobic oxidation of hydrocarbons to ketones at room temperature, using small amounts of a radical initiator, was achieved as a heterogeneous catalytic reaction for the first time. |
format | Online Article Text |
id | pubmed-5529056 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | American Association for the Advancement of Science |
record_format | MEDLINE/PubMed |
spelling | pubmed-55290562017-08-04 Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons Takahashi, Masaki Koizumi, Hiromu Chun, Wang-Jae Kori, Makoto Imaoka, Takane Yamamoto, Kimihisa Sci Adv Research Articles The catalytic activity of alloy nanoparticles depends on the particle size and composition ratio of different metals. Alloy nanoparticles composed of Pd, Pt, and Au are widely used as catalysts for oxidation reactions. The catalytic activities of Pt and Au nanoparticles in oxidation reactions are known to increase as the particle size decreases and to increase on the metal-metal interface of alloy nanoparticles. Therefore, multimetallic nanoclusters (MNCs) around 1 nm in diameter have potential as catalysts for oxidation reactions. However, there have been few reports describing the preparation of uniform alloy nanoclusters. We report the synthesis of finely controlled MNCs (around 1 nm) using a macromolecular template with coordination sites arranged in a gradient of basicity. We reveal that Cu-Pt-Au MNCs supported on graphitized mesoporous carbon show catalytic activity that is 24 times greater than that of a commercially available Pt catalyst for aerobic oxidation of hydrocarbons. In addition, solvent-free aerobic oxidation of hydrocarbons to ketones at room temperature, using small amounts of a radical initiator, was achieved as a heterogeneous catalytic reaction for the first time. American Association for the Advancement of Science 2017-07-26 /pmc/articles/PMC5529056/ /pubmed/28782020 http://dx.doi.org/10.1126/sciadv.1700101 Text en Copyright © 2017 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works. Distributed under a Creative Commons Attribution NonCommercial License 4.0 (CC BY-NC). http://creativecommons.org/licenses/by-nc/4.0/ This is an open-access article distributed under the terms of the Creative Commons Attribution-NonCommercial license (http://creativecommons.org/licenses/by-nc/4.0/) , which permits use, distribution, and reproduction in any medium, so long as the resultant use is not for commercial advantage and provided the original work is properly cited. |
spellingShingle | Research Articles Takahashi, Masaki Koizumi, Hiromu Chun, Wang-Jae Kori, Makoto Imaoka, Takane Yamamoto, Kimihisa Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title | Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title_full | Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title_fullStr | Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title_full_unstemmed | Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title_short | Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
title_sort | finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons |
topic | Research Articles |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5529056/ https://www.ncbi.nlm.nih.gov/pubmed/28782020 http://dx.doi.org/10.1126/sciadv.1700101 |
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