Abstract
It is highly desirable but challenging to accelerate the dissociative adsorption of CO and lower the energy barriers of C-C coupling in the Fischer-Tropsch synthesis (FTS), both of which are prerequisite for high productivities of long-chain hydrocarbons. Herein, we report the fabrication of N-doped carbon nanotubes assembled hollow polyhedrons with embedded hollow Co (H-Co) nanoparticles (NPs) (H-Co@NCNHP) for highly efficient FTS. H-Co@NCNHP affords an extremely high C_(5+) space time yield of 1.67 × 10~(-5) mol g_(cat)~(-1) s~(-1), outperforming most of Co-based catalysts reported to date. Theoretical calculations demonstrate that, as compared with solid Co NPs with symmetric arrangement of d-orbital electrons, H-Co NPs induce the electron rearrangement of d orbitals (especially d_(z2)) toward the Fermi level, promoting the d-2π* /p coupling between Co active sites and adsorbed CO/intermediates.
NSTL