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

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• 作者：Zhenzhen Yang ; Bo Yu ; Hongye Zhang ; Yanfei Zhao ; Yu Chen ; Zhishuang Ma ; Guipeng Ji ; Xiang Gao ; Buxing Han ; Zhimin Liu
• 刊名：ACS Catalysis
• 出版年：2016
• 出版时间：February 5, 2016
• 年：2016
• 卷：6
• 期：2
• 页码：1268-1273
• 全文大小：368K
• ISSN：2155-5435

文摘

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.