Supported palladium nanoparticles on hybrid mesoporous silica:: Structure/activity-relationship in the aerobic alcohol oxidation using supercritical carbon dioxide

被引：58

作者：

Hou, Zhenshan ^{[1
]}

Theyssen, Nils ^{[1
]}

Brinkmann, Axel ^{[1
]}

Klementiev, Konstantin V. ^{[2
,3
]}

Gruenert, Wolfgang ^{[2
]}

Buehl, Michael ^{[1
]}

Schmidt, Wolfgang ^{[1
]}

Spliethoff, Bernd ^{[1
]}

Tesche, Bernd ^{[1
]}

Weidenthaler, Claudia ^{[1
]}

Leitner, Walter ^{[1
,4
]}

机构：

[1] Max Planck Inst Kohlenforsch, D-45470 Mulheim, Germany

[2] Ruhr Univ Bochum, Lehrstuhl Tech Chem, D-44801 Bochum, Germany

[3] DESY, HASYLAB, D-22607 Hamburg, Germany

[4] Rhein Westfal TH Aachen, Lehrstuhl Tech Chem & Petrolchem, Inst Tech & Makromol Chem, D-52064 Aachen, Germany

来源：

JOURNAL OF CATALYSIS | 2008年 / 258卷 / 02期

关键词：

palladium; nanoparticles; supercritical carbon dioxide; alcohol oxidation; mesoporous support; hybrid materials;

D O I：

10.1016/j.jcat.2008.07.002

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

The preparation, characterization, and catalytic properties of Pd nanoparticles supported on mesoporous organic-inorganic hybrid materials are described for continuous-flow aerobic oxidation of alcohols using supercritical carbon dioxide (scCO(2)) as a mobile phase. The nanoparticles were generated "bottom-up" from molecular precursors that were precoordinated to the support through suitable anchor units. The most active material allows high single-pass conversions in scCO(2) at temperatures as low as 60 degrees C. This high activity may be associated with the presence of small primary crystallites (approx. 2 nm) that conglomerate to ensembles about 25 nm in size, leading to a larger number of high-indexed planes in small volume units. These findings may provide useful guidelines for further catalyst design on the nanoscale for green oxidation methods. (C) 2008 Elsevier Inc. All rights reserved.

引用

页码：315 / 323

页数：9

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