Reversing sintering effect of Ni particles on γ-Mo2N via strong metal support interaction

Abstract

Reversing the thermal induced sintering phenomenon and forming high temperature stable fine dispersed metallic centers with unique structural and electronic properties is one of the ever-lasting targets of heterogeneous catalysis. Here we report that the dispersion of metallic Ni particles into under-coordinated two-dimensional Ni clusters over γ-Mo₂N is a thermodynamically favorable process based on the AIMD simulation. A Ni-4nm/γ-Mo₂N model catalyst is synthesized and used to further study the reverse sintering effect by the combination of multiple in-situ characterization methods, including in-situ quick XANES and EXAFS, ambient pressure XPS and environmental SE/STEM etc. The under-coordinated two-dimensional layered Ni clusters on molybdenum nitride support generated from the Ni-4nm/γ-Mo₂N has been demonstrated to be a thermally stable catalyst in 50 h stability test in CO₂ hydrogenation, and exhibits a remarkable catalytic selectivity reverse compared with traditional Ni particles-based catalyst, leading to a chemo-specific CO₂ hydrogenation to CO.

Reversing the thermal induced sintering phenomenon and forming high temperature stable fine dispersed metallic centers is one of the ever-lasting targets in heterogeneous catalysis. Here the authors report the dispersion of metallic Ni particles into under-coordinated two-dimensional Ni clusters over γ-Mo₂N.