發(fā)布時(shí)間：2019-03-31 16:39

【摘要】：針對(duì)丙烷和液體石蠟選擇性氧化制備脂肪酸的催化劑篩選與制備關(guān)鍵技術(shù)問題,本文以草酸鈮、碲酸、鉬酸銨、偏釩酸銨、硝酸鎳和ZSM-5為原料制備了多金屬氧化物基催化劑MoVTeNbO、Mo VTe Nb Ni O,V2O5/ZSM-5系列催化劑,分別用于催化丙烷氧化轉(zhuǎn)化制取丙烯酸和催化液體石蠟氧化轉(zhuǎn)化制取脂肪酸。用SEM、EDX、XRD、XPS、Raman、H2-TPR、NH3-TPD和FT-IR對(duì)催化劑進(jìn)行了表征和功能特性研究,研究結(jié)果表明:(1)制備MoVTeNbO催化劑制備的最佳條件為:漿液法,元素比Mo:V:Nb:Te=1:0.3:0.12:0.23,焙燒溫度600℃,惰性氣氛下制取的催化劑具有高含量的活性相和最佳的丙烯酸產(chǎn)率。MoVTeNbO氧化轉(zhuǎn)化丙烷的最佳條件:40目催化劑為0.4g,通入的混合反應(yīng)氣烷氧比為2:3,反應(yīng)溫度為400℃時(shí)丙烯酸產(chǎn)率最高,達(dá)到了16.1%,其中丙烷轉(zhuǎn)化率為50.1%,丙烯酸選擇性為33.2%。(2)對(duì)MoVTeNbO的改性研究發(fā)現(xiàn)Te元素在MoVTeNbO催化氧化丙烷過程中主要起丙烯酸的選擇作用;Mo1V0.3Te0.23Nb0.12Ni0.008O對(duì)丙烷氧化轉(zhuǎn)化丙烯酸的性能優(yōu)于其它Ni含量摻雜的催化劑,丙烯酸產(chǎn)率為17.9%。其中丙烷轉(zhuǎn)化率為51.9%,丙烯酸選擇性為34.5%。(3)MoVNbO在液體石蠟的氧化轉(zhuǎn)化過程中只起催化作用,V元素為MoVNbO的主要催化元素。ZMS-5為載體,采用共沉淀法制備V2O5/ZSM-5催化劑可用于液體石蠟催化氧化轉(zhuǎn)化脂肪酸。當(dāng)反應(yīng)溫度為150℃,反應(yīng)時(shí)間為8 h,催化劑用量為0.1g時(shí),在純氧氣氛下氧化產(chǎn)物酸值為17.33mg(KOH)/g、皂化值為33.52mg(KOH)/g。
[Abstract]:In this paper, niobium oxalate, tellurate, ammonium molybdate and metavanadate were selected as catalysts for selective oxidation of propane and liquid paraffin to prepare fatty acids. Polymetallic oxide-based catalysts MoVTeNbO,Mo VTeNb Ni-O and V _ 2O _ 5 / ZSM _ 5 series catalysts were prepared from nickel nitrate and ZSM-5. The catalysts were used for catalytic conversion of propane to acrylic acid and oxidation conversion of liquid paraffin to fatty acids, respectively. The catalysts were characterized and characterized by SEM,EDX,XRD,XPS,Raman,H2-TPR,NH3-TPD and FT-IR. The results showed that: (1) the optimum conditions for preparing MoVTeNbO catalysts were: slurry method; The calcination temperature of the element is 600 鈩，

本文編號(hào)：2451085