Engineering Cobalt–Nitrogen–Carbon Interfaces on Spherical Supports for Tunable Furfural Hydrogenation Selectivity

We report a cobalt catalyst supported on spherical nitrogen-doped carbon (CoNC) prepared via a coordinated assembly of EDTA, melamine, and chitosan followed by pyrolysis. This strategy generates uniformly dispersed Co nanoparticles strongly anchored by N functionalities. The optimized CoNC2 catalyst (4 wt % Co) exhibits outstanding performance in liquid-phase furfural hydrogenation, achieving >99% conversion and >99% selectivity toward furfuryl alcohol under mild conditions (160 °C, 30 bar H2). In situ DRIFTS, XPS, catalytic controls, and DFT calculations support a bifunctional working model in which metallic Co promotes H2 activation while adjacent N-containing environments favor selective carbonyl adsorption. This synergistic interaction suppresses competing ring hydrogenation and hydrogenolysis pathways. The catalyst shows excellent stability and recyclability. Owing to the use of earth-abundant cobalt and renewable carbon precursors, this approach provides a scalable and sustainable platform for the selective upgrading of biomass-derived aldehydes.