Design and Construction of High-Efficiency Heavy-Oil-Based Catalysts for Selective Hydrogenation

Given the growing prevalence of heavy crude oil in global petroleum reserves, refinery outputs of heavy oil byproducts (including petroleum asphalt and FCC slurry) have exhibited consistent annual growth. The realization of clean, high-value applications for heavy oil resources has emerged as a pivotal challenge confronting the petroleum refining sector. Characterized by abundant availability, cost-effectiveness, and elevated carbon content, heavy oil represents an exceptional precursor material for carbon-based nanomaterials. Herein, we employed heavy oil derivatives such as petroleum asphalt and FCC slurry as carbon sources to synthesize two-dimensional ultrathin graphene-like materials through an innovative "bottom-up" synthesis strategy incorporating template-assisted and molten salt-mediated methodologies. By introducing metal species in situ during carbonization, we successfully achieved the self-assembly of two-dimensional graphene-analogous frameworks incorporating atomically dispersed metal sites (M-Nx-C, where M = Fe, Co, Pd, etc.), with precise engineering of electronic coupling between the metallic centers and carbon matrices. Through systematic modulation of the metal centers' coordination environments, the developed single-atom M-Nx-C catalysts exhibited remarkable catalytic performance and exceptional chemoselectivity in hydrogenating nitroaromatics containing diverse sensitive functional groups (such as -CHO and -C≡C). This research establishes a fundamental framework for developing next-generation catalysts for selective hydrogenation processes while pioneering an innovative approach to the high-value transformation of heavy oil resources.