Boosting the Fischer-Tropsch synthesis performances of cobalt-based catalysts via geometric and electronic engineering: Construction of hollow structures

作者：Zhan, Weiteng; Wang, Yajing^*; Chen, Jianmin; Chen, Zhijie; Li, Yingwei^*

来源：Applied Catalysis B: Environmental , 2022, 313: 121469.

DOI：10.1016/j.apcatb.2022.121469

• Metal-organic frameworks
• Co-based catalysts
• Hollow structure
• Fischer-Tropsch synthesis
• Nanoparticles

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 C5+ space time yield of 1.67 x 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-2 pi* /p coupling between Co active sites and adsorbed CO/intermediates.