CsCuHPVAs MoO杂多化合物对异丁烯选择性氧化反应的催化性能  

Catalytic Performance of CsCuHPVAsMoO Heteropolycompounds for Selective Oxidation of Isobutene

作　　者：蔡铁军[1] 余长林[1] 邓谦[1] 彭振山[1] 龙云飞[1] 蒋绍亮[1] 

机构地区：[1]湖南科技大学化学化工系,湖南湘潭411201

出　　处：《催化学报》2003年第12期951-956,共6页

基　　金：湖南省教育厅科研项目 ( 0 3C5 15 )

摘　　要：用组合法合成了CsCuHPVAsMoO系列杂多化合物催化剂 ,并采用FT IR ,H2 TPR ,NH3 TPD和TG DTA等方法对催化剂进行了表征 .在自制固定床反应器中对异丁烯进行选择性氧化 ,考察了Cs,Cu和As含量、催化剂焙烧温度及反应条件对催化剂催化性能的影响 .结果表明 ,Cs的引入有利于提高催化剂的选择性 ;Cu和As的引入在提高催化剂活性的同时 ,也提高了催化剂的选择性 ;当焙烧温度为 340℃时 ,催化剂的活性和选择性最高 .组成为Cs0 1 Cu0 2 HxPVAs0 2 Mo1 0 Oy 的催化剂对异丁烯具有很强的选择性氧化能力 ,在最佳反应条件下 ,甲基丙烯酸、甲基丙烯醛和乙酸的收率分别可达 5 2 84 % ,1 2 0 5 %和1 8 2 1 % .A series of CsCuHPVAsMoO heteropolycompound catalysts were prepared by combination. The catalysts were characterized by FT IR, H 2 TPR, NH 3 TPD and TG DTA. The selective oxidation of isobutene was carried out in a continuous flow fixed bed reactor. The effects of the contents of Cs, Cu and As and the calcination temperature of the catalysts on the activity and the selectivity of the catalysts were studied. The results showed that the addition of Cs is very important for increasing the catalyst selectivity and the addition of Cu and As markedly improve the activity and the selectivity of the catalysts. Among the catalysts, Cs 0.1 Cu 0.2 H x PVAs 0.2 Mo 10 O y calcined at 340 ℃ exhibits the best catalytic performance in selective oxidation of isobutene. Under the optimum reaction conditions of n ( i C = 4) ∶ n (O 2) ∶ n (N 2) =1 0∶4 17∶1 83, SV=540 h -1 and θ =340 ℃, the yield of methacrylic acid, methacrolein and acetic acid can reach 52 84%, 12 05% and 18 21% respectively, suggesting that Cs 0.1 Cu 0.2 H x PVAs 0.2 Mo 10 O y is a promising catalyst.

关 键 词：铯 铜 磷 钒 砷 钼 复合氧化物 杂多化合物 异丁烯 选择性氧化 甲基丙烯酸 甲基丙烯醛 乙酸 

分 类 号：O643.3[理学—物理化学]