Metalated Mesoporous Poly(triphenylphosphine) with Azo Functionality: Efficient Catalysts for CO2 Conversion

被引:124
|
作者
Yang, Zhenzhen [1 ]
Yu, Bo [1 ]
Zhang, Hongye [1 ]
Zhao, Yanfei [1 ]
Chen, Yu [1 ]
Ma, Zhishuang [1 ]
Ji, Guipeng [1 ]
Gao, Xiang [1 ]
Han, Buxing [1 ]
Liu, Zhimin [1 ]
机构
[1] Chinese Acad Sci, Inst Chem, Key Lab Colloid Interface & Thermodynam, Beijing Natl Lab Mol Sci, Beijing 100190, Peoples R China
来源
ACS CATALYSIS | 2016年 / 6卷 / 02期
基金
中国国家自然科学基金;
关键词
porous organic polymer; CO2; conversion; alpha-alkylidene cyclic carbonate; methylation of amine; heterogeneous catalysis; POROUS ORGANIC POLYMERS; CARBON-DIOXIDE; FACILE SYNTHESIS; METHYLATION; AMINES; NANOPARTICLES; DESIGN; TRANSFORMATION; REDUCTION; COMPLEXES;
D O I
10.1021/acscatal.5b02583
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
Mesoporous poly(triphenylphosphine) with azo functionality (poly(PPh3)-azo) is reported, which was synthesized via oxidative polymerization of P(m-NH2Ph)(3) at ambient conditions. This kind of polymer could strongly coordinate with metal ions (e.g., Ru3+) and could reduce Ag+ in situ to metallic form. The resultant metalated poly(PPh3)-azo (e.g., poly(PPh3)-azo-Ag or -Ru) were discovered to be highly efficient catalysts for CO2 transformation. Poly(PPh3)-azo-Ag showed more than 400 times higher site-time-yield (STY) for the carboxylative cyclization of propargylic alcohols with CO2 at room temperature compared with the best heterogeneous catalyst reported. Poly(PPh3)-azo-Ru also exhibited good activity for the methylation of amines with CO2. It was demonstrated that the high performances of the catalysts originated from the cooperative effects between the polymer and the metal species. In addition, both catalysts showed good stability and easy recyclability, thus demonstrating promising potential for practical utilization for the conversion of CO2 into value-added chemicals.
引用
收藏
页码:1268 / 1273
页数:6
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