Tailoring the Hybrid Texture and Pore Structure of Pitch-Based Carbon to Disperse and Support Ni Nanoparticles for Efficient Phenol Hydrogenation

材料科学 化学工程 催化作用 碳化 介孔材料 环己醇 纹理(宇宙学) 聚丙烯腈 苯酚 碳纤维 选择性 热解 纳米颗粒 聚合 多孔性 粒径 微型多孔材料 多孔介质 粒子(生态学) 双功能
作者
Tiantian Li,Zhepeng Zhao,Marcos Millán,Xiangyi Long,Zhengwei Cui,Guanming Yuan
出处
期刊:Industrial & Engineering Chemistry Research [American Chemical Society]
卷期号:65 (5): 2529-2542
标识
DOI:10.1021/acs.iecr.5c04030
摘要

The design and development of porous carbons and their supported Ni-based catalysts, characterized by high activity, stability, and low cost, remain challenging in green chemical processes. In this study, petroleum pitch (PP) and biomass pitch (BP) were employed as inexpensive carbon sources, with polyacrylonitrile (PAN) serving as a texture-modifying agent, to prepare modified carbons (MCs). Porous modified carbons (PMCs) with tailored pore sizes and distributions were comparatively prepared using a nanoscale CaCO 3 template and a steam activation method. The results show that pitch-based MCs with a hybrid texture can be produced by mixing 50 wt % PAN with PP or BP, followed by thermal polymerization at 400 °C and carbonization at 600 °C. Steam activation at 800 °C for 1 h enhances pore formation in hybrid MCs derived from PAN-BP compared to those derived from PAN–PP, due to differences in the molecular structures of PP and BP. In contrast, the CaCO 3 template method primarily produces mesopores and macropores, whereas steam activation generates abundant micropores and mesopores in PMCs, thereby creating ideal conditions for high-quality catalyst supports. The resulting 10 wt % Ni/PMC BP catalysts demonstrate an impressive phenol conversion of 99.4% and a cyclohexanol selectivity of 94.1% after reaction at 180 °C for 2 h, outperforming reference Ni-based catalysts. Additionally, the catalytic performance of phenol hydrogenation is significantly influenced by Ni particle size, which is closely related to the texture and pore characteristics of the carbon supports. This research provides valuable insights into the rational design of PMCs as effective supports for advanced catalytic applications.
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