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氮硼双掺杂石墨烯负载磷化镍催化剂的表征及其加氢反应机理 被引量:3

Characterization and Hydrogenation Reaction Mechanism of Nickel Phosphide Catalyst Supported on Graphene Doped With Nitrogen and Boron
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摘要 采用水热法制备氮硼双掺杂还原氧化石墨烯(N_(4)B_(1)-rGO)载体,当磷化镍负载质量分数为20%时,分别以Al_(2)O_(3)、rGO、N-rGO和N_(4)B_(1)-rGO为载体,通过浸渍-热分解法制备20%Ni_(2)P/Al_(2)O_(3)、20%Ni_(2)P/rGO、20%Ni_(2)P/N-rGO和20%Ni_(2)P/N_(4)B_(1)-rGO催化剂。采用N 2吸附-脱附、FT-IR、XRD、SEM、TGA等手段对载体及催化剂进行表征,并以苯酚选择性加氢制备环己酮为反应体系评价4种催化剂的反应性能。结果表明:在反应温度160℃、反应压力0.5 MPa、反应时间4 h、催化剂用量0.3 g的条件下,20%Ni_(2)P/N_(4)B_(1)-rGO催化剂进行苯酚选择性加氢反应性能较好,苯酚转化率为72.36%,环己酮选择性达到61.06%;20%Ni_(2)P/N_(4)B_(1)-rGO催化剂具有介孔结构、较大的比表面积和良好的热稳定性,以及优异的催化活性和选择性,归因于Ni_(2)P在载体表面有较好的分散度和N_(4)B_(1)-rGO与Ni_(2)P间良好的协同作用。 The carrier of nitrogen-and boron-doped reduced graphene oxide(N_(4)B_(1)-rGO)was prepared by hydrothermal method.Using the impregnation-thermal decomposition method,the catalysts of 20%Ni_(2)P/Al_(2)O_(3),20%Ni_(2)P/rGO,20%Ni_(2)P/N-rGO and 20%Ni_(2)P/N_(4)B_(1)-rGO were prepared with Al_(2)O_(3),rGO,N-rGO and N_(4)B_(1)-rGO as carrier at the mass fraction of 20%for nickel phosphide.The carriers and catalysts were characterized by N 2 adsorption-desorption,FT-IR,XRD,SEM and TGA.Besides,the reaction performance of the four catalysts was evaluated based on the reaction system of the selective hydrogenation of phenol to cyclohexanone.The results show that 20%Ni_(2)P/N_(4)B_(1)-rGO catalyst has good reaction property of selective hydrogenation of phenol under the conditions of reaction temperature of 160℃,reaction pressure of 0.5 MPa,reaction time of 4 h and catalyst amount of 0.3 g,the conversion rate of phenol is 72.36%,and the selectivity of cyclohexanone is up to 61.06%.20%Ni_(2)P/N_(4)B_(1)-rGO catalyst has mesoporous structure,large specific surface area,good thermal stability,and excellent catalytic activity and selectivity,which is attributed to the good dispersion of Ni_(2)P on the carrier surface and good synergy between N_(4)B_(1)-rGO and Ni_(2)P.
作者 徐海升 郜鹏程 薛媚月 范峥 XU Haisheng;GAO Pengcheng;XUE Meiyue;FAN Zheng(College of Chemistry and Chemical Engineering,Xi′an Shiyou University,Xi′an 710065,China;Shaanxi Engineering Research Center of Low-Carbon Energy Materials and Green Processes,Xi′an 710065,China;Xi′an Key Laboratory of Low-Carbon Utilization for High-Carbon Resources,Xi′an 710065,China)
出处 《石油学报(石油加工)》 EI CAS CSCD 北大核心 2023年第3期517-524,共8页 Acta Petrolei Sinica(Petroleum Processing Section)
基金 陕西省自然科学基础研究计划项目(2023-JC-YB-118) 西安石油大学研究生创新与实践能力培养立项项目(YCS21211022,YCS22111008)资助。
关键词 氮硼双掺杂 还原氧化石墨烯 苯酚 环己酮 反应机理 nitrogen-boron doping reduced graphene oxide phenol cyclohexanone reaction mechanism
作者简介 通讯联系人:徐海升,男,副教授,博士,从事能源化工方向功能催化材料的研究,E-mail:xhs74@xsyu.edu.cn。
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