摘要
用组合法合成CsMPVAsMoO(M=Cu、Fe、Ni)系列催化剂.采用FT-IR、H2-TPR方法对催化剂进行了表征;在自制固定床反应器中对丙烯进行选择性氧化,探讨了助剂α-Sb2O4含量,不同活化温度对催化剂催化性能的影响.结果表明,Cu2+、Fe3+、Ni2+的引入,有利于提高丙烯酸的收率;加入助剂极大地增大催化剂活性,降低了反应温度,但丙烯酸的收率有所下降.组成为Cs0.1Cu0.2HxPVAs0.2Mo10Oy的催化剂对丙烯具有很好的选择性氧化能力,440℃时,丙烯转化率达86.8%,丙烯酸、丙烯醛、乙酸、丙酮的收率分别可达53.7%、3.2%、10.7%、10.45%;Cs0.1Cu0.2HxPVAs0.2Mo10Oy/17%α-Sb2O4,在360℃时,丙烯转化达率89.02%,丙烯酸、丙烯醛、乙酸、丙酮的收率分别可达37.2%、2.2%、18.2%、2.8%.
In this paper, a series of Cs_(0.1)M_(0.2)H_xPVAs_(0.2)Mo_(10)O_y(M=Cu, Fe, Ni) heteropolycompounds were prepared by impregnation method. The catalysts were characterized by IR, H_2-TPR.Catalytic selective oxidation of propene was carried out in a continuous flow fixed-bed reactor.The effects of addition of promoter α-Sb_2O_4 to Cs_(0.1)M_(0.2)H_xPVAs_(0.2)Mo_(10)O_y(M=Cu, Fe, Ni)and activation temperature on activity and selectivity of the catalysts were studied respectively. The results showed that the addition of Cu^(2+), Fe^(3+), Ni^(2+)is very important for increasing the selectivity of acrylic acid and α-Sb_2O_4 can markedly improve the catalytic activity. Among these catalysts, Cs_(0.1)Cu_(0.2)H_xPVAs_(0.2)Mo_(10)O_y and Cs_(0.1)Cu_(0.2)H_xPVAs_(0.2)Mo_(10)O_y/α-Sb_2O_4(17%) treated in an O_2 stream (10 cm^3 min^(-1)) for 1 h at 320 ℃, the best catalytic performance for selective oxidation of propene can be obtained. At 440 ℃, over the Cs_(0.1)Cu_(0.2)H_xPVAs_(0.2)Mo_(10)O_y catalyst, the yield of acrylic acid, acrolein, aceticacid and acetone can reach 53.7%, 3.2%, 10.7%, 10.45% respectively; At 360 ℃, over the Cs_(0.1)Cu_(0.2)H_xPVAs_(0.2)Mo_(10)O_y/α-Sb_2O_4 (17%)catalyst, the yield of acrylic acid, acrolein, acetic acid and acetone is 37.2%, 2.2%, 18.2%, 2.8% respectively.
出处
《分子催化》
EI
CAS
CSCD
北大核心
2003年第6期444-449,共6页
Journal of Molecular Catalysis(China)
基金
湖南省教育厅科研项目(01C267).
