首页|期刊导航|石油化工|氮氧共掺杂碳载Pt基催化剂选择性加氢制备N-(1,3-二甲基丁基)-N'-苯基对苯二胺

氮氧共掺杂碳载Pt基催化剂选择性加氢制备N-(1,3-二甲基丁基)-N'-苯基对苯二胺OA

N,O co-doped carbon supported Pt-based catalyst for selective hydrogenation to N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine

中文摘要英文摘要

以焦油废渣作为碳源和氮源,采用MgO模板法与H2O2 氧化法制备了N,O共掺杂多孔碳载体(NOPC),然后负载Pt制得催化剂Pt/NOPC.利用SEM、TEM、HRTEM、XRD、拉曼光谱等方法对催化剂进行了表征,并对其用于催化合成N-(1,3-二甲基丁基)-N'-苯基对苯二胺(6PPD)的性能进行了评价.实验结果表明,Pt/NOPC中,N与O在碳基骨架中均匀分布,Pt在载体表面均匀分散.N掺杂降低Pt表面电子密度,削弱羰基吸附,抑制酮加氢副反应;O掺杂引入酸性位点,促进席夫碱生成;介孔结构改善传质保证催化剂稳定性,在120℃、1.5 MPa下Pt/NOPC制备6PPD的收率达99.4%,连续 8 次循环使用后收率仍大于 95%.提供了焦油废渣资源化利用的途径,对于酮胺还原烷基化催化剂的设计及对苯二胺类抗氧剂的高效合成提供了理论基础.

Tar residue was utilized as the carbon and nitrogen sources to prepare an N,O co-doped porous carbon(NOPC)by an MgO-template method combined with H2O2 oxidation,and a Pt/NOPC catalyst was subsequently prepared by loading Pt onto the obtained support.The catalyst was characterized by SEM,TEM,HRTEM,XRD,and Raman spectroscopy,and its catalytic activity for the synthesis of N-(1,3-dimethylbutyl)-N'-phenyl-p-phenylenediamine(6PPD)was evaluated.The experimental results show that N and O are uniformly incorporated into the carbon framework of Pt/NOPC,and Pt is evenly dispersed on the support surface.N doping decreases the surface electron density of Pt,weakens carbonyl adsorption,and suppresses side hydrogenation reactions of ketones,whereas O doping introduces acidic sites that promote Schiff base formation.The mesoporous structure improves mass transfer and ensures catalyst stability.Under 120℃and 1.5 MPa,the yield of 6PPD over Pt/NOPC reaches 99.4%,and remains higher than 95%after eight consecutive cycles.A feasible pathway for the valorization of tar residue is thus provided,and a theoretical basis is established for the design of catalysts for the reductive alkylation of ketones with amines as well as for the efficient synthesis of p-phenylenediamine antioxidants.

李东升;丁军委;于文龙

青岛科技大学 化工学院,山东 青岛 266042青岛科技大学 化工学院,山东 青岛 266042青岛科技大学 化工学院,山东 青岛 266042

化学化工

氮氧共掺杂多孔碳Pt基催化剂选择性加氢废渣资源化利用

N,O co-doped porous carbonPt-based catalystselective hydrogenationwaste residue valorization

《石油化工》 2026 (3)

325-333,9

国家自然科学基金项目(22208182).

10.3969/j.issn.1000-8144.2026.03.002

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