摘要
新奇复杂 Pd (C4H2O4 )(C4H8N2 )_(0.5 ) 被溶剂综合了热合成并且由酚的氧化 carbonylation 为 diphenyl (DPC ) 的直接合成用作异构的催化剂。在 Pd ( C4H2O4 )( C4H8N2 )的反应系统,催化活上的_( 0.5 ) /Cu ( OAc )2/ tetrabutylammonium bromide/hydroquinone/ 4A 分子筛,反应温度的效果,时间和公司压力被调查,并且结果表明催化剂能有效地催化酚的氧化 carbonylation 。在象溶剂的 T=90 °C , t=4 h , p ( O2 ) =0.3 MPa , p (公司) =3.9 MPa 和 CH2Cl2 的合适的反应条件下面, diphenyl 的转换数(吨)能到达大约 13.50 ( mol-DPC/mol-Pd ),它比为在一样的反应条件下面的纯 PdCl2 的 TON 高。
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 oure PdCl2 under the same reaction conditions.
基金
Supported by the National Natural Science Foundation of China (20636030), Tlanjin Natural Science Foundation (07JCZDJC 00100).