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Ni/N-rGO催化苯酚选择性加氢制备环己酮性能
引用本文:黄国强,徐海升,李善建,郜鹏程. Ni/N-rGO催化苯酚选择性加氢制备环己酮性能[J]. 石油学报(石油加工), 2022, 38(1): 151-157. DOI: 10.3969/j.issn.1001-8719.2022.01.018
作者姓名:黄国强  徐海升  李善建  郜鹏程
作者单位:西安石油大学 化学化工学院,陕西 西安 710065
基金项目:西安石油大学研究生创新与实践能力培养项目(YCS20221009、YCS20212102)基金资助
摘    要:以自制氧化石墨(GO)为原料,尿素为氮源,通过水热法制备了氮掺杂还原氧化石墨烯(N-rGO)载体,采用浸渍法制得不同镍负载量Ni/N-rGO催化剂,采用N2吸附-脱附、XRD、SEM等手段对Ni/N-rGO催化剂进行表征分析,考察催化剂制备条件(活性组分负载量、尿素添加量、H2还原温度)和反应条件(反应温度、反应压力、反应时间)对Ni/N-rGO催化剂催化苯酚选择性加氢制备环己酮的影响。结果表明:在活性组分负载质量分数为20%、尿素/GO质量比为30、H2还原温度为450 ℃的条件下制备的20%Ni/N-rGO催化剂具有较大的比表面积和适宜的孔结构,金属镍分散相对均匀;在反应温度为150 ℃、反应压力为0.4MPa、反应时间为2.0 h、20%Ni/N-rGO催化剂/苯酚质量比为0.35的最佳条件下,苯酚转化率为91.93%,环己酮选择性为61.75%;20%Ni/N-rGO催化剂重复使用5次后催化性能下降较明显,苯酚转化率降至82.17%,环己酮选择性降至50.93%。

关 键 词:氮掺杂石墨烯  催化剂  苯酚  选择性加氢  环己酮  
收稿时间:2020-12-30

Catalytic Performance of Ni/N-rGO in Selective Hydrogenation of Phenol to Cyclohexanone
HUANG Guoqiang,XU Haisheng,LI Shanjian,GAO Pengcheng. Catalytic Performance of Ni/N-rGO in Selective Hydrogenation of Phenol to Cyclohexanone[J]. Acta Petrolei Sinica (Petroleum Processing Section), 2022, 38(1): 151-157. DOI: 10.3969/j.issn.1001-8719.2022.01.018
Authors:HUANG Guoqiang  XU Haisheng  LI Shanjian  GAO Pengcheng
Affiliation:College of Chemistry and Chemical Engineering, Xi’an Shiyou University, Xi’an 710065, China
Abstract:With self-made graphiteoxide (GO) as raw material and urea as nitrogen source, N-doped reducedgraphene oxide (N-rGO) carrier was prepared by hydrothermal method. Catalystswith different nickel loading Ni/N-rGO were prepared by impregnation method.The Ni/N-rGO catalysts were characterized by N2 adsorption-desorptionand XRD, SEM. The effects of catalyst preparation conditions (active componentloading, addition of urea, H2 reduction temperature) and reactionconditions (reaction temperature, reaction pressure, reaction time) oncatalytic performance in the selective hydrogenation of phenol to cyclohexanonecatalyzed by Ni/N-rGO catalysts were investigated. Results show that theconditions of active components loading mass fraction of 20%, urea/GO mass ratio of 30 and H2 reductiontemperature of 450 ℃,this 20%Ni/N-rGO catalyst has large specific surface area and suitable porestructure, and the metal nickel dispersion is relatively uniform. Under theoptimum conditions of reaction temperature of 150 ℃, reaction pressure of 0.4 MPa, reaction time of 2.0 h, 20%Ni/N-rGO catalyst/phenolmass ratio of 0.35, the conversion rate of phenol is 91.93% and the selectivityof cyclohexanone is 61.75%, respectively. However, the catalytic performance of20%Ni/N-rGO catalyst remarkably decreases after 5 times reuse, with phenolconversion and cyclohexanone selectivity decreasing to 82.17% and 50.93%respectively.
Keywords:nitrogen doped graphene  catalyst,phenol,selective hydrogenation,cyclohexanone,
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