摘要
采用共沉淀法制备了不同Fe/Ni摩尔比(0、0.125、0.25、0.5和0.75)的Al_(2)O_(3)负载型NiFe单、双金属催化剂,并考察了它们在生物糠醛衍生2-羟基四氢吡喃(2-HTHP)还原胺化合成高附加值5-氨基戊醇反应中的催化性能.研究发现当Fe/Ni摩尔比为0.25时表现出最高的5-氨基戊醇收率(在80℃和2 MPa优化条件下达90%).利用N_(2)吸脱附、X射线衍射(XRD)、氢气程序升温还原(H_(2)-TPR)、透射电镜(TEM)等技术对催化剂进行了表征,结果表明适量Fe的掺入可以提高催化剂的分散性和还原性,同时在还原活化催化剂中形成Ni-Fe合金相,继而使相应催化剂表现出更优异的催化活性.通过固定床对比考察了催化剂的稳定性,NiFe(0.25)-Al-O双金属催化剂表现出明显优于NiFe(0)-Al-O单金属催化剂的稳定性,运行120 h前者只有微弱失活而后者显著失活.对比反应后催化剂表征发现,金属Fe的修饰可以有效抑制金属活性颗粒的烧结和流失,从而显著提高其反应稳定性.
Al_(2)O_(3)supported NiFe bimetallic catalysts with different Fe/Ni molar ratios(0,0.125,0.25,0.5 and 0.75)were prepared by co-precipitation method for the reductive amination(RA)of biofurfural-derived 2-hydroxytetrahydropyran(2-HTHP)to synthesis valuable 5-amino-1-pentanol(5-AP)and best catalytic performance was obtained when the Fe/Ni mole ratio is 0.25.The effect of metal Fe modification on the catalyst structure,in combination with the evaluation of the catalytic activity and stability was studied in 2-HTHP reductive amination.The results show that incorporation of appropriated Fe could improve the dispersity and reducibility of the catalyst.Moreover,the formation of Ni-Fe alloy structure showed better catalytic activity and stability on bimetallic catalyst.Through the XRD and TEM analysis of the used catalyst showed that the Ni-Fe alloy structure could effectively inhibit the sintering and leaching of active metal particles,thus significantly improving its stability.
作者
杨坚
李雪梅
张佳
刘海龙
田俊英
夏春谷
黄志威
YANG Jian;LI Xue-mei;ZHANG Jia;LIU Hai-long;TIAN Jun-ying;XIA Chun-gu;HUANG Zhi-wei(State Key Laboratory for Oxo Synthesis and Selective Oxidation,Lanzhou Institute of Chemical Physics,Chinese Academy of Sciences,Lanzhou 730000,China;University of Chinese Academy of Sciences,Beijing 100049,China)
出处
《分子催化》
CAS
CSCD
北大核心
2022年第2期118-128,共11页
Journal of Molecular Catalysis(China)
基金
国家自然科学基金(21872155,21902164)
中国科学院战略性先导科技专项项目(XDA21010700)
中国科学院西部青年学者项目和兰州市城关区科技发展项目(2020JSCX0051)
关键词
NiFe双金属
生物质
还原胺化
氨基醇
构效关系
NiFe bimetal
biomass
reductive amination
amino alcohol
structure-activity relationship
作者简介
杨坚(1991-),男,硕士研究生,主要从事多相催化研究;通讯联系人:黄志威,E-mail:zwhuang@licp.cas.cn.
