载体和担载酸对乙烯直接氧化合成乙酸反应的影响  

Effect of Support and Acidity of Catalyst on Direct Oxidation of Ethylene to Acetic Acid

作　　者：张建鲁[1] 王新平[1] 蔡天锡[1] 程谟杰[2] 包信和[2] 

机构地区：[1]大连理工大学精细化工国家重点实验室,辽宁大连116012 [2]中国科学院大连化学物理研究所催化基础国家重点实验室,辽宁大连116023

出　　处：《催化学报》2002年第3期203-206,共4页

摘　　要：在固定床流动反应器上研究了Pd 酸 /载体体系催化乙烯直接氧化合成乙酸的反应 ,并对载体相同但担载酸强度不同的催化剂的催化活性进行了比较 .结果表明 ,担载酸的强度明显影响催化剂的活性 ,酸强度越大其催化活性越高 .用NH3 TPD和异丙醇脱水探针反应表征了二氧化硅、活性碳和酸性白土三种载体担载的Pd H4SiW12 催化剂的酸性 ,并测试了三种催化剂的催化活性 .结果表明 ,载体通过影响担载酸的强度而影响催化剂的活性 ,载体上的强酸中心越多 ,催化剂的活性越高 .测定了二氧化硅、活性碳和酸性白土三种载体担载的Pd H4SiW12 催化剂上Pd的分散度 ,并与其催化活性相关联 .结果表明 。The direct oxidation of ethylene to acetic acid over Pd-acid/support catalysts in a fixed-bed reactor was studied The results showed that when the phospho-tungstic acid ( H3PW12), phospho-molybdic acid (H3PMo12) I phosphoric acid, sulfuric acid, silicotungstic acid (H4SiW12) or its soldium salts were supported on Pd/SiO2, the acid strength influences the catalytic activity strongly, and the catalyst with stronger acid strength has higher activity. The acidity of Pd-H4SiW12 catalysts supported respectively on SiO2, activated carbon (AC), and acid clay (ACy) was characterized by NH3-TPD and i-C3H7OH dehydration. The results showed that the supports affect the catalytic activity through influencing the acid strength. The more the strong acid sites on catalyst, the higher the catalytic activity. When the silica, AC or ACy was used as support, the influence of Pd dispersion determined by hydrogen adsorption on the catalytic activity can not be observed. Therefore, it can be deduced that the decisive factor to the activity of catalysts is the acid strength but not the Pet dispersion.

关 键 词：载体 担载酸 直接氧化 合成 钯 二氧化硅 活性碳 酸性白土 负载型催化剂 乙烯 乙酸 催化活性 

分 类 号：O643.3[理学—物理化学]