Characterization of Ni/N-rGO catalyst and study on the hydrogenation performance of phenol
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摘要: 以325目鳞片石墨为原料,采用改进Hummers法合成氧化石墨(GO),再以尿素为氮源,通过水热法制备了氮掺杂还原氧化石墨烯(N-rGO)载体,然后通过浸渍法制备出负载型Ni/N-rGO催化剂。通过N2吸附-脱附、XRD、SEM、H2-TPR等测试方法对所制备的催化剂进行表征分析。以苯酚选择性加氢制备环己酮为反应体系,在反应温度150 ℃、压力0.4 MPa、时间2.0 h的条件下,对比了N-rGO、还原氧化石墨烯(rGO)、活性炭(AC)等载体负载Ni催化剂的加氢性能。结果表明,N-rGO载体不但具有较大的比表面积和适宜的孔结构,而且N-rGO和金属镍之间有较好的协同作用,Ni/N-rGO催化剂展现出优异的催化活性和选择性。Abstract: Using 325 mesh flake graphite as raw material, graphite oxide (GO) was synthesized by improved Hummers method. Nitrogen-doped reduced graphene oxide (N-rGO) carrier was prepared by hydrothermal method using urea as nitrogen source, and then supported Ni/N-rGO catalyst was prepared by impregnation method. The prepared catalysts were characterized and analyzed by N2 adsorption-desorption, XRD, SEM, H2-TPR and other methods. The hydrogenation performance of Ni catalysts supported by N-rGO, reduced graphene oxide (rGO) and activated carbon (AC) were compared under the reaction conditions of 150 ℃, 0.4 MPa and 2.0 h with selective hydrogenation of phenol to cyclohexanone as probe reaction. The results show that the N-rGO support not only has a large specific surface area and suitable pore structure, but also has good synergistic effect with nickel metal, and the Ni/N-rGO catalyst thus shows excellent catalytic activity and selectivity.
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Key words:
- N-rGO carrier /
- catalytic hydrogenation /
- phenol /
- cyclohexanone /
- reaction mechanism
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表 1 各催化剂的物理结构性质
Table 1 Physical structural properties of each catalyst
Sample Specific surface
area/(m2·g−1)Average pore size/nm Pore volume
/(cm3·g−1)GO 70 2.0 0.03 N-rGO 352 4.8 0.42 rGO 315 4.5 0.40 AC 483 1.9 0.33 Ni/N-rGO 273 5.4 0.37 Ni/rGO 215 5.1 0.35 Ni/AC 348 2.1 0.27 表 2 不同镍基催化剂的活性和选择性
Table 2 Activity and selectivity of different nickel-based catalysts
Sample Phenol conversion rate/% Cyclohexanone selectivity/% rGO 48.1 30.6 N(30)-rGO 59.7 39.9 10%Ni/N(30)-rGO 81.2 47.3 20%Ni/N(30)-rGO 91.9 61.8 30%Ni/N(30)-rGO 86.2 55.2 20%Ni/rGO 82.7 45.4 20%Ni/AC 67.2 32.6 -
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