Co-N-C催化剂的制备及“一锅法”合成N-亚苄基苯胺

以甲酰胺为氮源和碳源,乙酸钴为钴源,采用预先缩合/高温焙烧两步法制备了一系列Co-N-C催化剂,利用XRD、TEM、N₂吸附-脱附以及XPS等表征了催化剂结构,考察了催化剂用于硝基苯与苯甲醇"一锅法"合成N-亚苄基苯胺的催化性能及其稳定性。结果表明,焙烧温度和掺杂氮元素对Co-N-C催化剂性能影响显著,催化剂Co-N-C/800具有最好的催化性能,0.6 MPa氮气气氛下,温度140℃,反应12 h,硝基苯转化率达99%,N-亚苄基苯胺选择性达99%,催化剂重复使用5次,其活性无明显下降。

Preparation of Co-N-C catalysts and"one-pot method"for synthesis of N-benzyl aniline

A series of Co-N-C catalysts were prepared by a two-step process including pre-condensation and high-temperature calcination, as well as formamide was used as both nitrogen and carbon sources, and cobalt acetate was employed as the source of cobalt. Then the characterizations of XRD, TEM, N₂ adsorption-desorption, and XPS were carried out to investigate the morphology and textural properties of as-prepared Co-N-C catalysts. Moreover, the catalytic activity and reusability of such Co-N-C catalysts were further studied for one-pot synthesis of N-benzyl aniline from nitrobenzene and benzyl alcohol. The results demonstrated that the annealing temperature and nitrogen-doping have remarkable influence on the catalytic activity of Co-N-C catalysts. The Co-N-C/800 catalyst exhibited the best catalytic performance, in which the conversion of nitrobenzene was 99%, and the selectivity of N-benzyl aniline was 99% under 0.6 MPa nitrogen, temperature of 140℃, and reaction time of 12 h. The catalyst was used repeatedly for 5 times, and its activity did not decrease significantly.