新型MgO限域NiCo合金碳基催化剂用于苯胺与脂肪醇的N-烷基化反应  

Novel MgO confined NiCo alloy incorporating carbon catalyst prepared for N-alkylation of arylamines with fatty alcohols

作　　者：石靖 李伟作 SHI Jing;LI Wei-Zuo(School of Petrochemical Engineering,Changzhou University,Changzhou 213000,Jiangsu,China)

机构地区：[1]常州大学石油化工学院,江苏常州213164

出　　处：《黑龙江大学工程学报》2023年第2期12-18,共7页Journal of Engineering of Heilongjiang University

基　　金：国家自然科学基金项目(22201024);江苏省自然科学基金项目(BK20220617)。

摘　　要：寻找一种成本效益高且可扩展的策略来制备高效的合金催化剂,用于N-烷基化反应仍然是一个挑战。通过自模板化策略,采用Ni-Co-Mg三金属MOFs(命名为Ni-Co-Mg@H_(2)dhbdc)作为前驱体,一步热解合成了香蕉状形貌固溶体限域NiCo合金的碳基新型纳米催化剂(命名为NiCo/MgO-C)。将此催化剂应用于苯胺与脂肪醇的N-烷基化反应,由于其独特的结构(如NiCo纳米颗粒的小尺寸,电子密度的增强传输)和NiCo合金特性,表现出卓越的性能,与双金属MOFs衍生催化剂(如Ni/MgO-C和Co/MgO-C)相比更优越。在热解过程中,发现Ni-Co-Mg@H 2dhbdc前体能够提高NiO-MgO或CoO-MgO固溶体中NiO或CoO物种的还原程度。因此,这种Ni-Co-Mg@H_(2)dhbdc MOFs模板化的策略是一种简单且可控的方法,用于合成负载型固溶体纳米合金催化剂应用于多相催化反应。Finding a cost-effective and scalable strategy to create highly efficient alloy catalysts for N-alkylation reactions is still challenging.In this work,we have synthesized an unique catalyst named NiCo/MgO-C through a self-templating strategy by using Ni-Co-Mg tri-metallic MOFs called Ni-Co-Mg@H 2 dhbdc.It was a solid-solution confined NiCo alloy catalyst with banana-like morphology containing carbon.This catalyst showed superior performance due to its unique structure(such as small size of NiCo nanoparticles,enhanced transfer of electron density)and NiCo alloy properties upon applied in N-alkylation of arylamines with alcohol reaction in comparison with bimetallic MOFs-derived catalysts such as Ni/MgO-C and Co/MgO-C.It was found that the tri-metallic Ni-Co-Mg@H 2 dhbdc precursor enhance the reduction of NiO/CoO species confined in NiO-CoO-MgO solid-solution during the pyrolysis process.Hence,it is believed that this tri-metallic MOFs-templated strategy provided an easy and controllable way to synthesize solid-solution supported nanoalloy catalysts for heterogeneous catalytic reactions.

关 键 词：金属有机框架 N-烷基化反应 碳基傕化剂 

分 类 号：TQ426.61[化学工程]