气相法CO与亚硝酸甲酯偶联合成草酸二甲酯用Pd/α-Al_2O_3催化剂的研究  

Study on Pd/α-Al_2O_3 Catalyst for Vapor-Phase Coupling Reaction of CO with CH_3ONO to (CH_3OOC)_2

作　　者：赵秀阁[1] 吕兴龙[1] 赵红钢[1] 朱毓群[1] 肖文德[1] 

机构地区：[1]华东理工大学联合化学反应工程研究所,上海200237

出　　处：《催化学报》2004年第2期125-128,共4页

摘　　要：一氧化碳与亚硝酸甲酯 (CH3 ONO)在负载型Pd/α Al2 O3 催化剂上合成草酸二甲酯 (DMO)的反应 ,其催化剂活性与载体的性质及所添加的助剂密切相关 .载体的双峰孔分布是影响催化剂活性的关键因素 ;在双峰孔的基础上 ,载体的比表面积、孔径及孔体积的增大使催化剂活性升高 ;助剂的添加可有效地提高Pd的分散度 ,减小Pd的粒径 ,从而使CH3 ONO转化率从 5 7 1%升高到 84 7% ,DMO时空收率可达到 898g/ (L·h) .助剂添加后 ,活性组分Pd的含量可以从 1%降至 0 3% ,而DMO时空收率仍可达到 74 5 g/ (L·h) .The Pd/α-Al 2O 3 catalyst for vapor-phase coupling reaction of CO with CH 3ONO to (CH 3OOC) 2 was prepared. The influence of support, promoter and Pd loading on the catalyst on the reaction behavior was studied. The XRD analysis confirmed that the α-Al 2O 3 support is well-crystallized. The BET result showed that the double pore structure of the support remarkably affects the catalyst activity. For the support with double pore structure, the CH 3ONO conversion increased with the increase of specific surface area, pore size and pore volume of the support. The dispersity of palladium is higher on Pd-M/α-Al 2O 3 catalyst than on Pd/α-Al 2O 3 catalyst. The results revealed that Pd-M/α-Al 2O 3 catalyst exhibits much higher activity ( X(CH 3ONO)=84.7%) than Pd/α-Al 2O 3 catalyst ( X(CH 3ONO)=57.1%), and higher space time yield of (CH 3OOC) 2 (898 g/(L·h)). Meanwhile, the addition of promoter M can decrease the Pd loading from 1% to 0.3%.

关 键 词：亚硝酸甲酯 一氧化碳 偶联合成 草酸二甲酯 钯 氧化铝 负载型催化剂 助剂 气相法 

分 类 号：O643.3[理学—物理化学]