Nickel and Nickel–Magnesia Catalysts Active in the Hydrogenation of 1,4-Butanedinitrile
Nickel and Nickel–Magnesia Catalysts Active in the Hydrogenation of 1,4-Butanedinitrile
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DOI：
10.1006/jcat.2000.3084
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发表时间：
2001
影响因子：
7.3
通讯作者：
M. Serra;P. Salagre;Y. Cesteros;F. Medina;J. Sueiras
中科院分区：
文献类型：
--
作者：
M. Serra;P. Salagre;Y. Cesteros;F. Medina;J. Sueiras
摘要：合成了几种NiO - mgo体系，研究了它们作为1,4-丁腈气相加氢的镍催化剂，并与控制形貌的大块NiO进行了比较。采用XRD、BET、TPR、TPD、SEM和H2化学吸附技术对样品进行了表征。Ni - mgo体系比Ni本体催化剂具有更高的活性。在所有反应温度下，活性最高的催化剂是R4CB型催化剂，其颗粒均质，约为1000 A，金属表面积最大，弱结合氢覆盖率最高。碱性氧化镁的存在抑制了缩合反应，因此有利于胺的消除，并防止催化剂失活。对不同产物的选择性不仅取决于催化性能，而且可以通过控制氢/二腈比来改变。R4CB催化剂对4-氨基丁腈的选择性最高，转化率为85%，转化率为100%，空速为13000 h−1，空速为343 K。降低氢/丁腈比可提高反应的选择性。
Abstract Several NiO–MgO systems were synthesized to be studied as nickel catalysts for the hydrogenation of 1,4-butanedinitrile in the gas phase and compared with a bulk NiO of controlled morphology. All samples were characterized by XRD, BET, TPR, TPD, SEM, and H2 chemisorption techniques. The Ni–MgO systems had higher activities than the Ni bulk catalyst. The most active catalyst at all reaction temperatures was type R4CB which had homogeneous particles of about 1000 A, the highest metal surface area, and the highest coverage with weakly bound hydrogen. The presence of basic magnesia suppresses the condensation reactions and consequently favors the elimination of amines, and prevents catalyst deactivation. The selectivity toward the different products not only depends on the catalytic properties but can also be modified by controlling the hydrogen/dinitrile ratio. The highest selectivity to 4-aminobutanenitrile was achieved by catalyst R4CB, with 85% at 100% conversion and working at a space velocity of 13,000 h−1 and 343 K. This selectivity could be increased by lowering the hydrogen/butanedinitrile ratio.