Synergizing metal-support interactions and spatial confinement boosts dynamics of atomic nickel for hydrogenations

Synergizing metal-support interactions and spatial confinement through atomic copper grippers boost the dynamics of highly loaded atomic nickel for high activity, high thermal/chemical stability and unprecedented coke inhibition in hydrogenation reactions. Atomically dispersed metal catalysts maximize atom efficiency and display unique catalytic properties compared with regular metal nanoparticles. However, achieving high reactivity while preserving high stability at appreciable loadings remains challenging. Here we solve the challenge by synergizing metal-support interactions and spatial confinement, which enables the fabrication of highly loaded atomic nickel (3.1 wt%) along with dense atomic copper grippers (8.1 wt%) on a graphitic carbon nitride support. For the semi-hydrogenation of acetylene in excess ethylene, the fabricated catalyst shows extraordinary catalytic performance in terms of activity, selectivity and stability-far superior to supported atomic nickel alone in the absence of a synergizing effect. Comprehensive characterization and theoretical calculations reveal that the active nickel site confined in two stable hydroxylated copper grippers dynamically changes by breaking the interfacial nickel-support bonds on reactant adsorption and making these bonds on product desorption. Such a dynamic effect confers high catalytic performance, providing an avenue to rationally design efficient, stable and highly loaded, yet atomically dispersed, catalysts.

Automated summary

The synergistic effect of metal-support interactions and spatial confinement enhances the catalytic performance of highly loaded atomic nickel on a graphitic carbon nitride support, leading to improved coke inhibition and outstanding activity in hydrogenation reactions. This approach provides a pathway to design efficient, stable, and highly loaded atomically dispersed catalysts with superior catalytic performance compared to traditional metal nanoparticles.