Selective Activation of the C-H Bond in Methane by Single Platinum Atomic Anions

被引：35

作者：

Liu, Gaoxiang ^{[1
]}

Zhu, Zhaoguo ^{[1
]}

Ciborowski, Sandra M. ^{[1
]}

Ariyarathna, Isuru R. ^{[2
]}

Miliordos, Evangelos ^{[2
]}

Bowen, Kit H. ^{[1
]}

机构：

[1] Johns Hopkins Univ, Dept Chem, Charles & 34Th St, Baltimore, MD 21218 USA

[2] Auburn Univ, Dept Chem & Biochem, Auburn, AL 36849 USA

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 23期

基金：

美国国家科学基金会;

关键词：

ab initio calculation; anion photoelectron spectroscopy; C-H bond activation; methane; platinum; POTENTIAL-ENERGY SURFACE; GAS-PHASE ACTIVATION; GUIDED-ION-BEAM; ROOM-TEMPERATURE; CLUSTER ANIONS; CHARGE-STATE; GOLD; REACTIVITY; CONVERSION; ALKANES;

D O I：

10.1002/anie.201903252

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

Mass spectrometric analysis of the anionic products of interaction between platinum atomic anions, Pt-, and methane, CH4 and CD4, in a collision cell shows the preferred generation of [PtCH4](-) and [PtCD4](-) complexes and a low tendency toward dehydrogenation. [PtCH4](-) is shown to be H-Pt-CH3- by a synergy between anion photoelectron spectroscopy and quantum chemical calculations, implying the rupture of a single C-H bond. The calculated reaction pathway accounts for the observed selective activation of methane by Pt-. This study presents the first example of methane activation by a single atomic anion.

引用

页码：7773 / 7777

页数：5

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