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

石油炼制与化工 ›› 2018, Vol. 49 ›› Issue (6): 56-60.

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

张惠民

国家能源投资集团有限责任公司

收稿日期:2017-11-07 修回日期:2017-12-12 出版日期:2018-06-12 发布日期:2018-06-20
通讯作者: 张惠民 E-mail:10000377@shenhua.cc
基金资助:
低碳烷烃选择氧化高分散隔离活性位催化剂的设计及反应机理研究

EFFECT OF Ni/Mo RATIO ON STRUCTURE OF Ni-Mo NITRIDE AND PROPANE AMMOXIDATION REACTION

Received:2017-11-07 Revised:2017-12-12 Online:2018-06-12 Published:2018-06-20
Supported by:

摘要/Abstract

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Ni2Mo3N或定向合成g-Mo2N和Ni2Mo3N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g-Mo2N或Ni2Mo3N；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%。

关键词: 镍钼配比, 镍钼氮化物, 催化剂, 烷烃, 氨氧化

Abstract: Ni-Mo oxide was prepared by co-precipitation of nickel nitrate and ammonium heptamolybdate. 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 ammoxidation was tested. The experimental results showed that Ni2Mo3N or the mixture of g-Mo2N and Ni2Mo3N can be synthesized by controlling Ni/Mo atomic ratio. These results suggested that the synergetic effect between g-Mo2N and Ni2Mo3N in the mixed Ni-Mo nitrides plays an important role in the process of propane ammoxidation. The mixed Ni-Mo nitride catalyst shows much higher catalytic activity and selectivity for ACN than g-Mo2N or Ni2Mo3N 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.

Key words: Ni/Mo ratio, Ni-Mo nitride, catalyst, alkane, ammoxidation

中图分类号:

张惠民. 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[J]. 石油炼制与化工, 2018, 49(6): 56-60.

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