Rutile TiO2-Supported Pt Nanoparticle Catalysts for the Low-Temperature Oxidation of Ethane to Ethanol

被引：1

作者：

Oda, Akira ^{[1
]}

Kimura, Yuya ^{[1
]}

Ichino, Koyo ^{[1
]}

Yamamoto, Yuta ^{[2
]}

Kumagai, Jun ^{[2
]}

Lee, Gunik ^{[1
]}

Sawabe, Kyoichi ^{[1
]}

Satsuma, Atsushi ^{[1
]}

机构：

[1] Nagoya Univ, Grad Sch Engn, Dept Mat Chem, Nagoya 4648603, Japan

[2] Nagoya Univ, Inst Mat & Syst Sustainabil, Nagoya 4648603, Japan

来源：

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY | 2024年 / 146卷 / 29期

基金：

日本学术振兴会;

关键词：

METAL-SUPPORT INTERACTIONS; SELECTIVE OXIDATION; LOWER ALKANES; DIOXYGEN; METHANE; HYDROGENATION; CONVERSION; RADICALS; SYSTEM; OXYGEN;

D O I：

10.1021/jacs.4c04381

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Structure-function relationships of supported metal nanoparticle catalysts in the CO-assisted oxidation of ethane to ethanol were investigated. A rutile TiO2-supported Pt nanoparticle catalyst exhibited the highest ethanol production rate and selectivity. During the reaction, sequential changes in the geometric/electronic states and the particle size of the Pt nanoparticles were observed. The comparison of the catalytic performances of model catalysts with controlled metal-support interactions revealed that Pt-0 nanoparticles of 2-3 nm with a high fraction of the surface Pt delta+ species are highly active for the oxidation of ethane to ethanol. The coadded CO plays a pivotal role not only in tuning the oxidation state of the surface Pt but also in producing H2O2, which is the true oxidant for the reaction. The supported Pt nanoparticle uses in situ-generated H2O2 to activate ethane, where the C2H5OOH intermediate is formed through a nonradical mechanism and subsequently converted to C2H5OH. This reaction occurs even at 50 degrees C with an apparent activation energy of 32 kJ mol(-1). The present study sheds light on the usefulness of surface-engineered Pt nanoparticles for the low-temperature oxidation of ethane to ethanol.

引用

页码：20122 / 20132

页数：11

共 58 条

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