Abstract:
As the main constituent of coal tar, polycyclic aromatic hydrocarbons (PAHs) retain the unique polycyclic structure of coal, and its hydrogenation saturated product cycloalkanes are high-quality components of high energy density fuels. However, the high structure stability of the reactants, as well as the steric factors and competitive adsorption of the intermediates, hinder their adsorption activation, which make hydrogen saturation challenging. In this work, the characteristics of hydrogenation saturation reaction of PAHs were systematically analyzed, as a reversible exothermic reaction, the reaction conditions of low temperature and high pressure contribute to the hydrogenation saturation of polycyclic aromatic hydrocarbons. The total hydrogen product has high thermodynamic selectivity, but the reaction rate decreases with the deepening of hydrogenation. The regulation strategies of active metals and supports of catalysts were reviewed. For active metals, the adsorption mechanism between them and PAHs indicates that the suitable electron-deficient structure is conducive to the adsorption and activation of reactants, and the electronic structure of active metals can be regulated by the interaction between metal supports, doping other atoms to promote electron migration or lattice distortion, and using metal ensemble effect. In addition to acting as a dispersion platform for the active metal by means of porous structure, the supports can also regulate the surface properties by means of surface acidity, functionalization of functional groups or defect engineering, so as to realize the enrichment and transformation of reactants on the surface of the supports. In summary, catalysts with well dispersed electron-deficient active metals and supports that assist the diffusion adsorption of reactants are the key to the hydrogenation saturation of PAHs. Finally, the design of catalysts in the future should focus on the following three aspects: catalysts research ignoring the application limitations caused by multi-component competition of coal tar, the reaction of spilled hydrogen with PAHs on the surface of the support expands the reaction site, and the L-H (Langmuir-Hinshelwood) mechanism cannot be directly applied, which leads to the need to re-examine the catalytic hydrogenation saturation pathway and catalyst design, and the deactivation mechanism and anti-deactivation of hydrogenation saturated catalysts in different systems were studied.