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作 者:丁军委[1] 陈哲 钟缘 李慧 DING Junwei;CHEN Zhe;ZHONG Yuan;LI Hui(College of Chemical Engineering,Qingdao University of Science and Technology,Qingdao 266042,China)
出 处:《青岛科技大学学报(自然科学版)》2021年第1期20-27,共8页Journal of Qingdao University of Science and Technology:Natural Science Edition
基 金:山东省重点研发计划项目(2019GSF109055)。
摘 要:以芳香胺类生产过程中的釜残焦油作为碳源及氮源,采用纳米氧化镁模板法制备了氮掺杂纳米多孔碳材料,并以其做为载体制备了高分散的Pt基催化剂。采用N2低温物理吸附-脱附、SEM、TEM以及XPS等技术手段对制备的多孔碳及碳载Pt催化剂进行表征。研究了上述碳载Pt基催化剂在硝基C酸加氢反应中的催化性能。研究发现:通过改变纳米氧化镁前驱体的类型以及前驱体与碳源的配比,可以对纳米多孔碳材料比表面积和孔结构进行定向调变,且随着载体孔径增加,催化剂的稳定性随之提高。碳载体中N的引入改善了催化剂的选择性,使得硝基C酸加氢脱氯的副反应得到有效抑制。催化剂重复使用15次后,反应底物硝基C酸转化率仍能保持在99.2%,产物CLT酸选择性稳定在99%以上。The N-doped porous carbon nanomaterials(NPCNMs)based on residual tar from aromatic amine production as carbon source and nitrogen source,were prepared by template method using nanometer magnesium oxide,and the Pt-based catalyst with high dispersion was successfully prepared by using NPCNMs as carrier.The NPCNMs@Pt-based catalysts were characterized by N2 physical adsorption-desorption,SEM,TEM and XPS to explore the performance of the NPCNMs@Pt-based catalysts in nitroc acid hydrogenation.It was found that by changing the type of nanometer magnesium oxide precursor and the ratio of precursor to carbon source,the specific surface area and pore structure of the NPCNMs could be adjusted in a directional way.In addition,the stability of the NPCNMs@Pt-based catalysts could be improved with the increase of the carrier aperture.The introduction of N element in the carbon carrier improves the selectivity of the catalyst,which effectively inhibits the side reaction of nitroc acid hydrodechlorination.After the catalyst was reused for 15 times,the conversion rate of nitroc acid remained at 99.2%and the selectivity of CLT acid remained above 99%.
关 键 词:氮掺杂多孔碳 氧化镁模板 铂基催化剂 5-氨基-2-氯甲苯-4-磺酸
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