Synthesis and Characterization of Pincer-Molybdenum Precatalysts for CO2 Hydrogenation

被引：31
|
作者：
Zhang, Yuanyuan [1 ,2 ]
Williard, Paul G. [2 ]
Bernskoetter, Wesley H. [1 ,2 ]
机构：
[1] Univ Missouri, Dept Chem, Columbia, MO 65211 USA
[2] Brown Univ, Dept Chem, Providence, RI 02912 USA
来源：
ORGANOMETALLICS | 2016年 / 35卷 / 06期
基金：
美国国家科学基金会;
关键词：
CARBON-DIOXIDE ACTIVATION; DEFINED IRON CATALYST; C-H BOND; FORMIC-ACID; HOMOGENEOUS HYDROGENATION; ALKYL FORMATES; REVERSIBLE HYDROGENATION; PHOSPHINE COMPLEXES; ETHYLENE COMPLEXES; AQUEOUS-SOLUTION;
D O I：
10.1021/acs.organomet.5b00955
中图分类号：
O61 [无机化学];
学科分类号：
070301 ; 081704 ;
摘要：
A family of low-valent molybdenum complexes supported by the pincer ligand (PNP)-P-Me ((PNP)-P-Me = MeN(CH2CH2PPh2)(2)) was prepared and characterized, including ((PNP)-P-Me)Mo(C2H4)(2), which contains an agostic interaction between the metal and the N-methyl substituent. This beta-agostic C-H bond was cleaved by molybdenum and produced a cyclometalated molybdenum formate complex, (kappa(4)-(PNP)-P-Me)-Mo(C2H4)(kappa(2)-O2CH), upon exposure to CO2. This species serves as a promotor of CO, hydrogenation to formate under basic conditions, a rare transformation for group VI metals. The performance of the precatalyst was enhanced with the addition of Lewis acid salts.
引用
收藏
页码：860 / 865
页数：6
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