摘要
针对苯酚氧化羰基化直接催化合成碳酸二苯酯反应,研制出一种新型高效负载型催化剂PdCl2 Cu(OAc)2/HZSM 5,该催化剂适宜的n(Cu)/n(Pd)为14.3。采用XPS探讨了Pd、Cu物种间的协同作用;考察了溶剂对直接催化合成碳酸二苯酯反应的影响,碳酸二苯酯的收率按甲醇、环己烷、碳酸二甲酯、二氯甲烷的顺序增加。而在不同的载体上,碳酸二苯酯的收率则按5A分子筛、MgO、4A分子筛、SiO2、Hβ沸石、γ Al2O3、HZSM 5沸石的顺序增加。
A new supported catalyst PdCl2-Cu(OAc)2/HZSM-5 with high activity was developed for synthesis of diphenyl carbonate through oxidative carbonylation of phenol. The optimum n(Cu)/w(Pd) molar ratio of the catalyst was 14.3 and the PdClz loading was 1.5%. Solvents performed favorable effects on DPC yield with the increasing order of CH3OH, C6H14, DMC, CH2C12. In addition, DMC may take the place of CH2C12 as the solvent for the reaction. The catalyst activity was greatly affected by the supports with the increasing following order of 5A molecular sieve, MgO, 4A molecular sieve, SiO2, Hβ zeolite, y-Al2O3 , HZSM-5. PdCl2/HZSM-5 and Cu(OAc)2/HZSM-5 catalyst was prepared for studying the interaction between Pd and Cu and characterized by XPS.
出处
《石油学报(石油加工)》
EI
CAS
CSCD
北大核心
2004年第3期49-53,共5页
Acta Petrolei Sinica(Petroleum Processing Section)
基金
国家自然科学基金(20176008)
天津市自然科学基金(003801211)资助项目
关键词
苯酚
氧化羰基化
碳酸二苯酯
负载型催化剂
Carbonates
Carbonylation
Catalyst activity
Catalyst supports
Molecular sieves
Phenols
Synthesis (chemical)