Finely controlled multimetallic nanocluster catalysts for solvent-free aerobic oxidation of hydrocarbons

被引:94
|
作者
Takahashi, Masaki [1 ,2 ,3 ]
Koizumi, Hiromu [2 ]
Chun, Wang-Jae [3 ,4 ]
Kori, Makoto [2 ]
Imaoka, Takane [2 ,3 ,5 ]
Yamamoto, Kimihisa [2 ,3 ]
机构
[1] Univ Yamanashi, Interdisciplinary Grad Sch Med & Engn, 4-4-37 Takeda, Kofu, Yamanashi 4008510, Japan
[2] Tokyo Inst Technol, Inst Innovat Res, Lab Chem & Life Sci, Yokohama, Kanagawa 2268503, Japan
[3] Exploratory Res Adv Technol Japan Sci & Technol A, Kawaguchi, Saitama 3320012, Japan
[4] Int Christian Univ, Grad Sch Arts & Sci, Mitaka, Tokyo 1818585, Japan
[5] Precursory Res Embryon Sci & Technol Japan Sci &, Kawaguchi, Saitama 3320012, Japan
来源
SCIENCE ADVANCES | 2017年 / 3卷 / 07期
基金
日本科学技术振兴机构; 日本学术振兴会;
关键词
LIQUID-PHASE OXIDATION; MOLECULAR-OXYGEN; PLATINUM CLUSTERS; CO OXIDATION; NANOPARTICLES; DENDRIMER; TOLUENE; INTERFACE; ALDEHYDES; VALENCE;
D O I
10.1126/sciadv.1700101
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 themetal-metal interface of alloy nanoparticles. Therefore, multimetallic nanoclusters (MNCs) around 1 nmin 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.
引用
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页数:8
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