Co-N-C催化对甲基苯甲醇氨氧化合成对甲基苯腈

Synthesis of p-methylbenzonitrile by catalytic ammoxidation of p-methylbenzyl alcohol over Co-N-C

以不同金属Co、Mn、Fe、Ni的醋酸盐为金属活性组分,1,10-邻菲啰啉为氮源,Vulcan XC72R型碳粉为载体,通过浸渍法负载后在不同温度下焙烧得到系列M-N-C催化剂。采用TEM、EDS、XRD、XPS、TG等对催化剂的结构进行表征分析,以对甲基苯甲醇氨氧化一步合成对甲基苯腈为探针反应考察M-N-C催化剂的催化氨氧化性能。结果表明,800℃焙烧的Co-N-C催化剂能够形成Co-N活性中心,具有较好的催化性能。在氧气分压0.5 MPa、反应时间24 h、氨水用量0.7 mL和反应温度130℃时,对甲基苯甲醇转化率94.4%,对甲基苯腈选择性96.4%。

A series of M-N-C catalysts were prepared by impregnation and calcined at different temperature with acetate of Co,Mn,Fe,Ni as active component source,1,10-phenanthroline as nitrogen source,and Vulcan XC72R type carbon powder as carrier.The prepared catalysts were characterized by TEM,EDS,XRD,XPS,TG,and tested in one-step synthesis of p-toluonitrile by ammoxidation of p-methylbenzyl alcohol.The results showes that Co-N-C catalyst calcined at 800℃could form a Co-N active center and had good catalytic performance.When oxygen partial pressure was 0.5 MPa,reaction time was 24 h,the amount of ammonia was 0.7 mL and reaction temperature was 130℃,the conversion of p-methylbenzyl alcohol reached 94.4%,and the selectivity of p-methylbenzonitrile was 96.4%.