摘要
采用微波辅助分步浸渍溶剂热法,以ZSM-5分子筛为载体,合成了结构新颖的氨基酸型异双核配合物催化剂CuPdTS/ZSM-5(TS为L-亮氨酸缩水杨醛配体)。采用FT-IR、ICP—AES、1HNMR、XRD、N2吸附-脱附等手段对CuPdTS/ZSM-5进行表征,并将该催化剂用于催化苯酚氧化羰基化合成碳酸二苯酯(DPC)反应,考察了助催化剂Cu用量、反应时间和反应温度对DPC产率和选择性的影响。通过表征确定了CuPdTS配合物的结构,也确认CuPdTS已负载于ZSM-5分子筛上。当Cu(OAc)2用量0.03g、反应时间8h、反应温度100℃时,CuPdTS/ZSM-5催化苯酚氧化羰基化反应的碳酸二苯酯收率可达18.3%,选择性为47.4%。
A novel catalyst of ZSM-5 supported heterodinuclear Pd( U )-Cu( 1I ) complex with Schiff base of salicylaldehyde-L-leucine ( CuPdTS/ZSM-5 ) was prepared by microwave-assisted solvothermal method of fractional steps. The structure and related properties of the CuPdTS/ZSM-5 were characterized and determined by means of FT-IR, 1H NMR, ICP-AES, XRD, N2 adsorption-desorption. The catalytic performance of the CuPdTS/ZSM-5 and the effects of co-catalyst amount, reaction time, reaction temperature on the DPC yield and selectivity in the oxidative carbonylation of phenol to diphenyl carbonate (DPC) were studied. The characterized results revealed the structure of complex CuPdTS and proved that the CuPdTS was supported on ZSM-5 zeolite. The DPC yield and selectivity reached 18. 3% and 47. 4%, respectively, under the appropriate reaction conditions of Cu(OAc)2 amount 0.03 g, reaction time 8 h and reaction temperature 100 ℃.
出处
《石油学报(石油加工)》
EI
CAS
CSCD
北大核心
2014年第2期224-230,共7页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金(21106030)
河北省自然科学基金(B2010000016)
河北省教育厅科学研究计划项目(2009428)资助