葡萄糖基水热炭构建Co―N―C催化剂及其硝基苯催化加氢反应性能  

Synthesis of Co―N―C catalysts from a glucose hydrochar and their efficient hydrogenation of nitrobenzene

作　　者：杨雨 卜钰 龙兴霖 周志康 王静[1] 蔡进军[1] YANG Yu;BU Yu;LONG Xing-lin;ZHOU Zhi-kang;WANG Jing;CAI Jin-jun(School of Chemical Engineering,Xiangtan University,Xiangtan 411105,China)

机构地区：[1]湘潭大学化工学院,湖南湘潭411105

出　　处：《新型炭材料（中英文）》2023年第3期555-565,共11页New Carbon Materials

基　　金：国家自然科学基金(21506184);湖南省教育厅优秀青年项目(21B0098);湘潭市科技计划指导项目(CG-ZDJH202120);湘潭大学大学生创新训练计划.

摘　　要：硝基苯选择性加氢反应是生产苯胺的重要方法,其关键在于开发一种具有高效选择性且低成本的绿色催化剂。本文基于葡萄糖水热炭化得到水热炭前驱体,结合尿素和硝酸钴一步高温热解制备了一种高度分散的富含Co纳米颗粒的氮掺杂多孔炭材料,将其作为催化剂用于硝基苯加氢反应。详细研究了热解温度对催化剂结构和催化活性的影响,证实了催化活性主要受催化剂的比表面积、Co掺杂量及其Co-Nx配位效应的影响。结果表明,将含10%Co源制备的前驱体800℃热解得到的催化剂(Co@NCG-800)表现出优异的硝基苯催化加氢性能,在以异丙醇为溶剂、100℃和1 MPa氢压下反应2.5 h时可实现硝基苯的转化,苯胺选择性高达99%。催化剂循环使用6次后的硝基苯转化率和苯胺选择性几乎保持不变。优异的循环稳定性能可归因于多孔炭材料中的氮元素和Co纳米颗粒的强相互作用,同时磁性Co纳米颗粒使得催化剂具有较好的分离特性和重复使用性。A low-cost,green catalyst for nitrobenzene(NB)hydrogenation is needed for aniline production.We report the preparation of highly-dispersed Co particles supported on N-doped carbons by the hydrothermal treatment of glucose,followed by the pyrolysis of a mixture of urea,glucose hydrochar and cobalt nitrate in one-pot.The effect of the pyrolysis temperature on the microstructure of the catalysts was studied.Results indicated that the activity for NB hydrogenation was highly affected by the surface area,Co-loading level and Co-Nx coordination in the catalysts.Co@NCG-800 pyrolyzed at 800℃ with 10%Co in the precursor had extraordinary activity for NB hydrogenation,achieving full conversion and 99%aniline selectivity in isopropanol at 100℃ and 1 MPa H2 pressure for 2.5 h.NB conversion and aniline selectivity over the catalysts remained almost unchanged after six recycles,due to the strong coordination between the N-and Co-species.The reaction system showed not only a high NB activity but also a green and durable catalytic process,with easy operation,easy separation and catalyst reusability.

关 键 词：生物质葡萄糖 水热炭化 Co-N-C催化剂 硝基苯加氢 

分 类 号：X712[环境科学与工程—环境工程]