首页> 中文期刊> 《石油炼制与化工》 >镍钼配比对镍钼氮化物结构和丙烷氨氧化反应性能的影响

镍钼配比对镍钼氮化物结构和丙烷氨氧化反应性能的影响

         

摘要

以钼酸铵和硝酸镍为原料,采用共沉淀法合成镍钼金属氧化物,再经过程序升温氮化反应合成镍钼双金属氮化物.利用XRD,Visible-Raman,FTIR,H2-TPR对镍钼氧化物及氮化物晶体结构及氧化还原性进行表征,并考察了丙烷在镍钼氮化物催化剂上的氨氧化反应性能.结果表明:通过控制化学试剂镍钼配比能够定向合成Ni2 Mo3 N或定向合成γ-Mo2 N和Ni2 Mo3 N两相共存的镍钼氮化物;两相共存的镍钼氮化物催化剂能够产生相互协同作用,有利于催化丙烷氨氧化反应,其催化活性和丙烯腈选择性明显优于单一晶相的 γ-Mo2 N或Ni2 Mo3 N;由镍钼摩尔比为3/2的化学试剂制得的镍钼氮化物催化剂表现出最优的催化性能,在773 K时丙烷转化率为75.0%,丙烯腈选择性为38.6%,产率为28.95%.%Ni-Mo oxide was prepared by co-precipitation of nickel nitrate and ammonium heptamolyb-date. Ni-Mo nitride catalysts were synthesized by temperature-programmed nitridation reaction of Ni-Mo oxide in a mixture of H2/N2. The structure and redox properties of the Ni-Mo oxide and corresponding nitride catalysts were characterized by XRD,visible-Raman,FT-IR,and H2-TPR. The catalytic performance for propane ammoxi-dation was tested. The experimental results showed that Ni2 Mo3 N or the mixture of γ-Mo2 N and Ni2 Mo3 N can be synthesized by controlling Ni/Mo atomic ratio. These results suggested that the synergetic effect betweenγ-Mo2 N and Ni2 Mo3 N in the mixed Ni-Mo nitrides plays an important role in the process of propane ammoxida-tion. The mixed Ni-Mo nitride catalyst shows much higher catalytic activity and selectivity for ACN thanγ-Mo2 N or Ni2 Mo3 N alone. The mixed NiMo nitride catalyst with 3/2 of Ni/Mo atomic ratio showed the best catalytic performance for propane ammoxidation. At 773 K,the conversion of propane is 75. 0%,the selectivity and the yield of ACN are 38. 6% and 28. 95%,respectively.

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