钴催化糠醛还原胺化反应合成糠胺  

Cobalt-Catalyzed Furfural Reduction of Ammoniation to Synthesis of Furfuramine

作　　者：王佳欢 陈金铸 徐益升[1] WANG Jiahuan;CHEN Jinzhu;XU Yisheng(School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China;College of Chemistry and Materials Science,Jinan University,Guangzhou 511443,China)

机构地区：[1]华东理工大学化工学院,上海200237 [2]暨南大学化学与材料学院,广州511443

出　　处：《华东理工大学学报（自然科学版）》2024年第4期489-496,共8页Journal of East China University of Science and Technology

摘　　要：以聚N-乙烯基咪唑、六水硝酸钴和钛酸四丁酯为原料,通过高温H2还原,制备非贵金属钴基催化剂Co/NC-TiO_(2)-800。采用X射线衍射(XRD)、比表面积(BET)和孔径分析、红外光谱分析(FT-IR)、透射电子显微镜(TEM)和扫描电子显微镜(SEM)等方法对样品进行了测试和表征。以糠醛还原胺化作为模型反应,测试了Co/NC-TiO_(2)-800的热催化活性,并探讨了反应路径。结果表明:以水合肼为氮源、H2为氢源,在温度100℃、H_(2)压力2.0 MPa、反应时间18 h的反应条件下糠胺收率达到99%;Co/NC-TiO_(2)-800在循环回收6次后仍具有较强的催化活性。A non-precious metal catalyst coated with carbon doped nitrogen supported cobalt by titanium oxide(Co/NC-TiO_(2)-800)was prepared by hydrogen reduction at high temperature using poly(N-vinylimidazole),cobalt nitrate hexahydrate,and tetrabutyl titanate as the raw materials.The carbon network catalyst containing metal-nitrogen can effectively generate isolated active substances to catalyze the reduction amination reaction.Titanium oxide is introduced to stabilize cobalt nanoparticles on nitrogen-doped carbon,which enhances the stability of the catalyst.The samples were characterized by X-ray diffractometer(XRD),specific surface and aperture analyzer(BET),infrared spectrum analyzer(FT-IR),transmission electron microscope(TEM)and scanning electron microscope(SEM).The composition and structure of Co/NC-TiO_(2)-800 were analyzed,and the active center and characteristics of Co/NC-TiO_(2)-800 were revealed.The catalytic activity of Co/NC-TiO_(2)-800 was tested using furfural reduction amination as the model reaction,and the reaction path was discussed.In addition,the effects of different nitrogen sources such as hydrazine hydrate,ammonia water and hydroxylamine hydrate on the reactivity were investigated.The results showed that the yield of furfuryl amine reached 99% at 100℃ and a H_(2) pressure of 2.0 MPa for 18 h with hydrazine hydrate as nitrogen source and hydrogen as hydrogen source.After 6 times of recycling,the catalytic activity is still high and has excellent stability.

关 键 词：生物质 糠醛 还原胺化 Co催化剂 含氮化学品 

分 类 号：O643.3[理学—物理化学]