Single-Site Palladium(II) Catalyst for Oxidative Heck Reaction: Catalytic Performance and Kinetic Investigations

被引:60
|
作者
Duan, Hui [1 ]
Li, Menghuan [1 ]
Zhang, Guanghui [2 ,3 ]
Gallagher, James R. [3 ]
Huang, Zhiliang [2 ,3 ]
Sun, Yu [2 ]
Luo, Zhong [1 ]
Chen, Hongzhong [1 ]
Miller, Jeffrey T. [3 ]
Zou, Ruqiang [4 ]
Lei, Aiwen [2 ]
Zhao, Yanli [1 ,5 ]
机构
[1] Nanyang Technol Univ, Div Chem & Biol Chem, Sch Phys & Math Sci, Singapore 637371, Singapore
[2] Wuhan Univ, Coll Chem & Mol Sci, Wuhan 430072, Hubei, Peoples R China
[3] Argonne Natl Lab, Chem Sci & Engn Div, Argonne, IL 60439 USA
[4] Peking Univ, Dept Mat Sci & Engn, Coll Engn, Beijing 100871, Peoples R China
[5] Nanyang Technol Univ, Sch Mat Sci & Engn, Singapore 639798, Singapore
来源
ACS CATALYSIS | 2015年 / 5卷 / 06期
基金
新加坡国家研究基金会;
关键词
C-H olefination; cross-coupling reactions; oxidative Heck reaction; periodic mesoporous organosilica; single-site Pd(II) catalyst; METAL-ORGANIC FRAMEWORK; PERIODIC MESOPOROUS ORGANOSILICA; C-H OLEFINATION; AEROBIC DEHYDROGENATION; HETEROGENEOUS CATALYST; NANOPARTICLES; SILICA; FUNCTIONALIZATION; LIGAND; ACTIVATION;
D O I
10.1021/acscatal.5b00569
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
The development of organometallic single-site catalysts (SSCs) has inspired the designs of new heterogeneous catalysts with high efficiency. Nevertheless, the application of SSCs in certain modem organic reactions, such as C-C bond formation reactions, has still been less investigated. In this study, a single-site Pd(II) catalyst was developed, where 2,2'-bipyridine-grafted periodic mesoporous organosilica (PMO) was employed as the support of a Pd(II) complex. The overall performance of the single-site Pd(II) catalyst in the oxidative Heck reaction was then investigated. The investigation results show that the catalyst displays over 99% selectivity for the product formation with high reaction yield. Kinetic profiles further confirm its high catalytic efficiency, showing that the rate constant is nearly 40 times higher than that for the free Pd(II) salt. X-ray absorption spectroscopy reveals that the catalyst has remarkable lifetime and recyclability.
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页码:3752 / 3759
页数:8
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