NiO-CoO/SiO_2-Al_2O_3催化剂上苯胺和1,6-己二醇气相催化合成1-苯基氮杂环庚烷的研究  

Study on the vapor-phase synthesis of 1-phenylazepane from aniline and 1,6-hexanediol over NiO-CoO/SiO_2-Al_2O_3 catalyst

作　　者：石雷[1] 魏婷[1] 刘兴海[1] 

机构地区：[1]辽宁师范大学化学化工学院,辽宁大连116029

出　　处：《辽宁师范大学学报（自然科学版）》2016年第1期59-63,共5页Journal of Liaoning Normal University:Natural Science Edition

基　　金：辽宁省教育厅高等学校科学研究一般项目(2009A421)

摘　　要：1-苯基氮杂环庚烷在材料化学、药物化学及有机合成等领域有广泛应用.由苯胺和1,6-己二醇气相催化合成1-苯基氮杂环庚烷绿色环保、价格低廉,是理想的合成方法.通过常压气固相反应对用于该反应的NiO-CoO/SiO_2-Al_2O_3催化剂进行了研究,并通过X射线粉末衍射、NH_3程序升温脱附、N_2物理吸附和热重等手段对催化剂进行了表征,以揭示催化剂结构与反应性能的关系.结果表明,当氧化镍和氧化钴担载量分别为0.075和0.025mmol/g、采用程序升温由室温升至800℃、并在该温度下焙烧4h,催化剂具有很高的活性和选择性,1-苯基氮杂环庚烷的收率达到85%.催化剂活性组分高度分散、中强酸中心数少、平均孔径大有利于1-苯基氮杂环庚烷的合成.积碳是催化剂失活的主要原因.1-Phenylazepane is widely used in the fields of material chemistry,pharmaceutical chemistry and organic synthesis,etc.A promising route for producing 1-phenylazepane,from environmental and economic viewpoints,seems to be the vapor phase catalytic synthesis from aniline and 1,6-hexanediol.In this paper,NiO-CoO/SiO_2-Al_2O_3 catalyst was investigated through the gas-solid reaction under atmospheric pressure and characterized by X-ray diffraction（XRD）,temperature programmed desorption of ammonia（NH_3-TPD）,BET physisorption and thermogravimetric analysis（TG）techniques to investigate the relationship between the structure of the catalyst and its catalytic performance.The results indicated that the catalyst showed high activity and selectivity with the yield of 1-phenylazepane up to 85% when the loadings of NiO and CoO were 0.075 and 0.025mmol/g and the catalyst was prepared by temperature-programmed-calcining from RT to 800 ℃ and holding the temperature for 4h.The catalyst with highly dispersed active components,small amount of middlestrong acid sites and large average pore size took advantage of the synthesis of 1-phenylazepane.The deactivation of the catalyst was mainly due to the carbon deposition.

关 键 词：1-苯基氮杂环庚烷 NiO-CoO/SiO2-Al2O3催化剂 苯胺 1 6-己二醇 气相合成 

分 类 号：O643.322[理学—物理化学]