Thermal activation of methane by vanadium boride cluster cations VBn+ (n=3-6)

被引：24

作者：

Chen, Qiang ^{[1
,2
]}

Zhao, Yan-Xia ^{[1
,2
]}

Jiang, Li-Xue ^{[1
,2
,3
]}

Li, Hai-Fang ^{[1
,2
]}

Chen, Jiao-Jiao ^{[1
,2
,3
]}

Zhang, Ting ^{[1
,2
,3
]}

Liu, Qing-Yu ^{[1
,2
]}

He, Sheng-Gui ^{[1
,2
,3
]}

机构：

[1] Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China

[2] CAS Res Educ Ctr Excellence Mol Sci, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China

[3] Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

PHYSICAL CHEMISTRY CHEMICAL PHYSICS | 2018年 / 20卷 / 07期

基金：

中国国家自然科学基金; 中国博士后科学基金;

关键词：

GAS-PHASE REACTIONS; EFFICIENT ROOM-TEMPERATURE; BOND ACTIVATION; ATOM TRANSFER; CLOSED-SHELL; METAL-IONS; BORON; ANIONS; REACTIVITY; CHEMISTRY;

D O I：

10.1039/c8cp00071a

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：

Investigation on the reactivity of atomic clusters represents an important approach to discover new species to activate and transform methane, the most stable alkane molecule. While a few types of transition metal species have been found to be capable of cleaving the C-H bond of methane, methane activation by the transition metal boride species has not been explored yet. This study reports that vanadium boride cluster cations VBn+ (n = 3-6) can dehydrogenate methane under thermal collision conditions. The mechanistic details of the efficient reactions have been elucidated by quantum chemistry calculations on the VB3+ reaction system. Compared to the non-polar bare B-3 cluster, the B-3 moiety in VB3+ can be polarized by the V+ cation and thus its reactivity toward methane can be much enhanced. This study provides new insights into the rational design of boron-based catalysts for methane activation.

引用

页码：4641 / 4645

页数：5

共 71 条

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