SCI和EI收录∣中国化工学会会刊

›› 2008, Vol. 16 ›› Issue (3): 354-356.

• • 上一篇    下一篇

Synthesis of Pd(C4H2O4)(C4H8N2)0.5 Complex and the Catalytic Activity for Oxidative Carbonylation of Phenol

程庆彦1, 梁亚男1, 高玲2, 王延吉1   

  1. 1. Key Laboratory of Green Chemical Technology & High Efficient Energy Saving of Hebei Province, Hebei University of Technology, Tianjin 300130, China;
    2. Tianjin Honest Industry Co. Ltd., Tianjin 300382, China
  • 收稿日期:2007-09-20 修回日期:2008-03-30 出版日期:2008-06-28 发布日期:2008-06-28
  • 通讯作者: CHENG Qingyan,E-mail:chengqingyan@hebut.edu.cn
  • 基金资助:
    Supported by the National Natural Science Foundation of China(20636030);Tianjin Natural Science Foundation(07JCZDJC00100)

Synthesis of Pd(C4H2O4)(C4H8N2)0.5 Complex and the Catalytic Activity for Oxidative Carbonylation of Phenol

CHENG Qingyan1, LIANG Yanank1, GAO Ling2, WANG Yanji1   

  1. 1. Key Laboratory of Green Chemical Technology & High Efficient Energy Saving of Hebei Province, Hebei University of Technology, Tianjin 300130, China;
    2. Tianjin Honest Industry Co. Ltd., Tianjin 300382, China
  • Received:2007-09-20 Revised:2008-03-30 Online:2008-06-28 Published:2008-06-28
  • Supported by:
    Supported by the National Natural Science Foundation of China(20636030);Tianjin Natural Science Foundation(07JCZDJC00100)

摘要: A novel complex Pd(C4H2O4)(C4H8N2)0.5 has been synthesized by solvent thermal synthesis and used as a heterogeneous catalyst for direct synthesis of diphenyl carbonate (DPC) by oxidative carbonylation of phenol. In the reaction system of Pd(C4H2O4)(C4H8N2)0.5/Cu(OAc)2/tetrabutylammonium bromide/hydroquinone/4A molecular sieves, the effect of reaction temperature, time and CO pressure on catalytic activity were investigated, and the results revealed that the catalyst could catalyze oxidative carbonylation of phenol effectively. Under suitable reaction conditions of T=90℃, t=4 h, p(O2)=0.3 MPa, p(CO)=3.9 MPa and CH2Cl2 as solvent, the turnover number (TON) of diphenyl carbonate can reach about 13.50 (mol-DPC/mol-Pd), which is higher than the TON for pure PdCl2 under the same reaction conditions.

关键词: diphenyl carbonate, synthesis, heterogeneous catalyst, palladium complex, oxidative carbonylation

Abstract: A novel complex Pd(C4H2O4)(C4H8N2)0.5 has been synthesized by solvent thermal synthesis and used as a heterogeneous catalyst for direct synthesis of diphenyl carbonate (DPC) by oxidative carbonylation of phenol. In the reaction system of Pd(C4H2O4)(C4H8N2)0.5/Cu(OAc)2/tetrabutylammonium bromide/hydroquinone/4A molecular sieves, the effect of reaction temperature, time and CO pressure on catalytic activity were investigated, and the results revealed that the catalyst could catalyze oxidative carbonylation of phenol effectively. Under suitable reaction conditions of T=90℃, t=4 h, p(O2)=0.3 MPa, p(CO)=3.9 MPa and CH2Cl2 as solvent, the turnover number (TON) of diphenyl carbonate can reach about 13.50 (mol-DPC/mol-Pd), which is higher than the TON for pure PdCl2 under the same reaction conditions.

Key words: diphenyl carbonate, synthesis, heterogeneous catalyst, palladium complex, oxidative carbonylation