Direct Conversion of Methane with Carbon Dioxide Mediated by RhVO3- Cluster Anions

被引：20
作者：
Yang, Yuan [1 ,3 ,4 ,5 ]
Yang, Bin [2 ,3 ,4 ,5 ]
Zhao, Yan-Xia [1 ,3 ,4 ,5 ]
Jiang, Li-Xue [1 ,4 ,5 ]
Li, Zi-Yu [1 ,4 ,5 ]
Ren, Yi [1 ,3 ,4 ,5 ]
Xu, Hong-Guang [2 ,4 ,5 ]
Zheng, Wei-Jun [2 ,3 ,4 ,5 ]
He, Sheng-Gui [1 ,3 ,4 ,5 ]
机构：
[1] Chinese Acad Sci, Inst Chem, State Key Lab Struct Chem Unstable & Stable Speci, Beijing 100190, Peoples R China
[2] Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100049, Peoples R China
[3] Univ Chinese Acad Sci, Beijing 100190, Peoples R China
[4] Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China
[5] CAS Res Educ Ctr Excellence Mol Sci, Beijing 100190, Peoples R China
来源：
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2019年 / 58卷 / 48期
基金：
中国国家自然科学基金;
关键词：
carbon dioxide; catalytic reactions; mass spectrometry; methane; quantum chemistry calculations; C-H BOND; GAS-PHASE OXIDATION; ACETIC-ACID; ROOM-TEMPERATURE; TRANSITION-METAL; ACTIVATION; CO2; CH4; RHODIUM; REACTIVITY;
D O I：
10.1002/anie.201911195
中图分类号：
O6 [化学];
学科分类号：
0703 ;
摘要：
Direct conversion of methane with carbon dioxide to value-added chemicals is attractive but extremely challenging because of the thermodynamic stability and kinetic inertness of both molecules. Herein, the first dinuclear cluster species, RhVO3-, has been designed to mediate the co-conversion of CH4 and CO2 to oxygenated products, CH3OH and CH2O, in the temperature range of 393-600K. The resulting cluster ions RhVO3CO- after CH3OH formation can further desorb the [CO] unit to regenerate the RhVO3- cluster, leading to the successful establishment of a catalytic cycle for methanol production from CH4 and CO2 (CH4+CO2 -> CH3OH+CO). The exceptional activity of Rh-V dinuclear oxide cluster (RhVO3-) identified herein provides a new mechanism for co-conversion of two very stable molecules CH4 and CO2.
引用
收藏
页码：17287 / 17292
页数：6
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