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环己烷直接氧化制丁二酸酐催化剂结构与催化性能研究
Direct catalytic oxidation of cyclohexane to butanedioic anhydride over composite nanocatalysts
【摘要】 以气态环己烷催化氧化脱氢制丁二酸酐为目标反应,采用溶胶-凝胶法制备以TiO2-Al2O3为复合载体的系列纳米催化剂,借助DTA-TG、FT-IR、TEM和XRD等测试手段对载体及其催化剂进行表征,并进行活性评价。结果表明,复合载体中TiO2基本上没有破坏γ-Al2O3的骨架结构,载体中的Al2O3和载体上V2O5的添加均能改变TiO2的晶型转型温度。Al O与Ti—O相互作用后形成Al—O…Ti—O。在晶型转变的同时,可以实现V5+向V4+的转变,添加P2O5后,可以改变V5+/V4+。晶格氧是实现目标反应的供氧中心,V5+和V4+是其脱氢中心,当两种活性中心匹配时,可获得较高的转化率和选择性。
【Abstract】 Composite catalysts were obtained by sol-gel method using nanosized-TiO2 supported on Al2O3 and V2O5 as the main active components.Butanedioic anhydride was synthesized by selective catalytic oxidation of gaseous cyclohexane over the catalysts.The supports and the nanocatalysts were characterized by DTA-TG,FT-IR,TEM and XRD.The results indicated that the cage structure of γ-Al2O3 were basically not affected by TiO2 in the composite support;the crystallographic texture transformation temperature of TiO2 could be changed by Al2O3-TiO2 interaction in the composite support and V2O5 on the composite support.Al—O…Ti—O bond formed due to interaction of AlO and Ti—O.V(Ⅴ) was transferred to V(Ⅳ) with the crystallographic texture transformation and V(Ⅴ)/V(Ⅳ) ratio was changed with doping of P2O5.Crystal lattice oxygen was the oxygen supply for the target reaction.V(Ⅴ) and V(Ⅳ) were dehydrogenization centers.Higher cyclohexane conversion and selectivity to butanedioic anhydride could be attained under appropriate matching of oxygen supply and dehydrogenization centers.
【Key words】 sol-gel method; gaseous cyclohexane oxidation; butanedioic anhydride; catalytic activity; surface structure;
- 【文献出处】 工业催化 ,Industrial Catalysis , 编辑部邮箱 ,2007年06期
- 【分类号】O643.36
- 【被引频次】5
- 【下载频次】127