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Pd/mpg-C3N4催化剂的制备、表征及其对松香加氢反应的催化性能

Preparation, Characterization and Performance for Rosin Hydrogenation of Pd/mpg-C3N4 Catalyst

  • 摘要: 以SiO2和三聚氰胺为原料,通过高温焙烧法制得介孔类石墨相氮化碳(mpg-C3N4),以浸渍法负载Pd纳米粒子制得Pd/mpg-C3N4,并用于催化松香加氢反应。采用XRD、FT-IR、TEM、ICP-AES、XPS、氮气吸附-脱附及GC分析对催化剂的结构、形貌特征、Pd负载量、金属价态、比表面积和孔径以及催化活性进行分析。结果表明:Pd纳米粒子成功地均匀分散在了氮化碳的层状结构中,Pd的负载并没有改变mpg-C3N4的骨架结构,Pd/mpg-C3N4仍然保持着介孔结构;但是Pd的负载使mpg-C3N4的比表面积、孔容和孔径均有所减小,Pd/mpg-C3N4的比表面积、孔容和孔径分别为47.73 m2/g、0.17 cm3/g和3.39 nm。在负载量为7.96%,5 MPa H2、150 ℃和反应4 h的松香催化加氢优化条件下制得去氢枞酸GC含量5.99%,枞酸GC含量小于1%的氢化松香产品(其中四氢枞酸为37.12%,二氢枞酸为56.71%)。催化剂Pd/mpg-C3N4重复使用4次后,四氢枞酸GC含量由37.12%下降至24.71%,去氢枞酸GC含量由5.99%上升至9.76%。

     

    Abstract: Using SiO2 and melamine as raw materials, mesoporous graphitic carbon nitride(mpg-C3N4) was prepared by high-temperature baking method. Pd/mpg-C3N4 was then prepared by impregnating of Pd nanoparticles and used to catalyze the hydrogenation of rosin. XRD, FT-IR, TEM, ICP-AES, XPS, nitrogen adsorption-desorption and GC were used to analyze the structure, morphology, actual loading of Pd, metal valence, specific surface area, pore size and catalytic activity of the catalyst. The results showed that nano-Pd was successfully uniformly dispersed in the layered structure of carbon nitride. Pd/mpg-C3N4 still maintained the mesoporous structure after Pd loading. However, due to Pd loading, the BET surface area, pore volume and pore diameter of mpg-C3N4 were reduced to 47.73 m2/g, 0.17 cm3/g and 3.39 nm, respectively. Hydrogenated rosin products with 5.99% dehydroabietic acid and less than 1% abietic acid were obtained under the optimized conditions for the hydrogenation of rosin (7.96% Pd loading, 5 MPa H2, 150 ℃, 4 h). After four cycles for the catalyst, the GC content of tetrahydroabietic acid decreased from 37.12% to 24.71%, and the GC content of dehydroabietic acid increased from 5.99% to 9.76%.

     

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