氮掺杂及表面活性剂辅助Co-N@C催化剂的制备及催化加氢应用  

Preparation and Hydrogenation Catalytic Application of Co-N@C Catalysts by Nitrogen Doping and Surfactant Modification

作　　者：戴玉玉 王千禧 沈纪达 张骏 王亚权[1] 严新焕[2] DAI Yuyu;WANG Qianxi;SHEN Jida;ZHANG Jun;WANG Yaquan;YAN Xinhuan(School of Chemical Engineering and Technology,Tianjin University,Tianjin 300072,China;College of Chemical Engineering,Zhejiang University of Technology,Hangzhou,Zhejiang 310014,China;Zhejiang Alpha Chemical Technology Co.,Ltd.,Jiaxing,Zhejiang 314304,China)

机构地区：[1]天津大学化工学院,天津300072 [2]浙江工业大学化学工程学院,浙江杭州310014 [3]浙江阿尔法化工科技有限公司,浙江嘉兴314304

出　　处：《浙江化工》2024年第11期37-45,共9页Zhejiang Chemical Industry

基　　金：国家重点研发计划(2017YFC0210901);国家自然科学基金项目(52103272);浙江省自然科学基金项目(LQ21E030004)。

摘　　要：设计具有高稳定性和高催化活性的非贵金属纳米催化剂是催化加氢工业化的迫切需求,金属有机框架衍生形成的非贵金属纳米颗粒均匀分散在多孔碳网格中被认为是构筑高稳定性和高活性催化剂非常有效的方法。本文通过金属钴离子和含氮配体/含羧酸配体之间的络合作用,非离子型表面活性剂辅助制备获得钴基金属有机框架(Co MOF)前驱体,进一步高温衍生获得金属纳米颗粒均匀分布的Co-N@C催化剂,研究含氮配体和表面活性剂的用量对Co MOF形貌及相应催化活性的影响。Co-N@C催化剂应用于催化邻氯硝基苯的加氢还原表现出优异的活性和选择性,在80℃、2 MPa H2压力下,反应60 min,转化率为100%,选择性为99.9%。此外,该催化剂对其他含卤素、醛基等硝基苯类化合物亦显示出优异的催化活性和选择性。The design of non-noble metal nanocatalysts with high stability and high catalytic activity is an urgent need for catalytic hydrogenation industrialization,and the uniform dispersion of non-noble metal nanoparticles derived from metal-organic frameworks in porous carbon grids is considered to be a very effective method for constructing catalysts with high stability and high activity.In this paper,cobalt-based metal-based organic framework(Co MOF)precursors were prepared with the assistance of non-ionic surfactants through the complexation between metal cobalt ions and nitrogen-containing ligands/carboxylic acid ligands,and the Co-N@C catalysts with uniform distribution of metal nanoparticles were further derived at high temperatures.The effects of nitrogen-containing ligands and surfactants on the morphology and corresponding catalytic activity of Co MOF were studied.The Co-N@C catalyst exhibited excellent activity and selectivity in catalyzing the hydrogenation reduction of o-chloronitrobenzene,with a reaction time of 60 min,a conversion rate of 100%,and a selectivity of 99.9%at 80°C and 2 MPa H2 pressure.In addition,the catalyst also showed excellent catalytic activity and selectivity for other nitrobenzene compounds containing halogens and aldehydes.

关 键 词：金属有机框架 Co-N@C 邻氯硝基苯 催化加氢 

分 类 号：O643.36[理学—物理化学] TQ246.31[理学—化学]