Hydrogen-enriched Rh clusters on layered calcium silicate for high-efficiency hydrogenation of aromatics at room temperature

The deep hydrogenation of aromatic rings remains challenging due to their inherent stability and low hydrogen solubility in solvents. Addressing both kinetic limitations and gas–liquid–solid mass transfer resistance under mild conditions requires innovative catalyst design. Herein, we address this hurdle by developing “hydrogen pumping catalysts” featuring ultrafine Rh nanoclusters within CAS-1, a novel potassium calcium silicate material (Ca₄K₄(H₂O)₈Si₁₆O₃₈). The outstanding advantage of the RhCAS-1 catalyst lies in its superior hydrogen storage capability, which ensures an uninterrupted hydrogen provision to catalytic active sites. Operating at ambient temperature, RhCAS-1 enables fully saturated hydrogenation of polycyclic aromatic hydrocarbons (e.g., naphthalene, toluene, and anthracene) with high conversion efficiency, while maintaining high catalytic stability over 20 consecutive operational cycles without detectable degradation. These findings establish a multifunctional framework for heterogeneous catalyst design that seamlessly integrates H₂ storage and activation, enabling energy-efficient hydrogenation of aromatic compounds.