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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...

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Autores principales: Takahashi, Masaki, Koizumi, Hiromu, Chun, Wang-Jae, Kori, Makoto, Imaoka, Takane, Yamamoto, Kimihisa
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Association for the Advancement of Science 2017
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.
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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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