化工学报2019，Vol.70Issue(12)：4625-4634,10.DOI:10.11949/0438-1157.20190395
Ce在负载Pd催化苯酚氧化羰基化合成碳酸二苯酯反应中的作用
Role of Ce in supported Pd catalyst for oxidative carbonylation of phenol to diphenyl carbonate
摘要
Abstract
A Pd-Ce-O/SiO2 catalyst with Ce as auxiliary was prepared by microemulsion method for oxidative carbonylation of phenol to synthesize diphenyl carbonate (DPC). The activity evaluation results showed that the catalyst performance increased with the increase of the amount of Ce. When the Ce/Pd molar ratio was 10/1, the phenol conversion rate was 64.4%, and the diphenyl carbonate selectivity was 83.4%. The XRD results showed that part of Ce4+entered into PdO crystal lattice, therefore the electrons of deactivated Pd could easily be transferred to Ce. So the Pd-Ce-O/SiO2 catalyst could be easily regenerated and showed better performance. According to the above mentioned results, Pd-O/CeO2 was designed and prepared for oxidative carbonylation of phenol. However, unlike Pd-Ce-O/SiO2, Pd-O/CeO2 showed poor catalytic performance. The phenol conversion and DPC selectivity was only 24.0% and 23.3% respectively. The characterization results showed that PdO was the main species of Pd on the surface of Pd-Ce-O/SiO2, but there was more PdO2 on Pd-O/CeO2. Because Pd(Ⅱ) is the active site for oxidative carbonyation, Pd-O/CeO2 exhibited inferior activity to Pd-Ce-O/SiO2. In addition, in Pd-O/CeO2 catalyst, the surface Pd content was lower than that of other catalyst because of the strong interaction between Pd species and CeO2. That??s one of the reasons for the poor activity of Pd-O/CeO2.关键词
碳酸二苯酯/氧化羰基化/多相反应/催化剂/载体/二氧化铈Key words
diphenyl carbonate/ oxidative carbonlyation/ heterogeneous reaction/ catalyst/ support/ ceria分类
数理科学引用本文复制引用
王志苗,张洪起,周立超,李芳,薛伟,王延吉..Ce在负载Pd催化苯酚氧化羰基化合成碳酸二苯酯反应中的作用[J].化工学报,2019,70(12):4625-4634,10.基金项目
国家自然科学基金项目(21776057) （21776057）
天津市自然科学基金项目(17JCYBJC20100, 18JCYBJC21500) （17JCYBJC20100, 18JCYBJC21500）
河北省留学人员科技活动择优资助项目(CL201605) （CL201605）
