Spatial Ensembles of Copper-Silica with Carbon Nanotubes as Ultrastable Nanostructured Catalysts for Selective...

Catalyst deactivation is one of the most important issues in heterogeneous catalysis. Constructing a stable nanoscale structure that maintains efficient activity and prolonged stability under redox conditions for catalysis, particularly hydrogenation reactions, remains attractive albeit the flourishing nanoscience. This work presents a facile route to synthesize a semi-encapsulated transition metal by assembling three-dimensional transition metal silicate nanotubes onto carbon nanotubes (CNTs) as precursors. The obtained materials expose an active surface of the transition metal for efficient catalysis and form a specific structure to inhibit the migration of metal nanoparticles (NPs) by establishing strong metal-support interactions. Cu@SiO₂ prepared by common precipitation shows an inferior activity, and its performance is easily attenuated because of the aggregation of Cu NPs. The addition of CNTs as a carrier doubles the intrinsic activity of Cu catalysts. This hybrid catalyst, which consists of Cu species, SiO₂, and CNTs, is among the best catalysts for dimethyl oxalate hydrogenation with boosting activity of 25 h^-1 and enhanced stability of more than 200 h.