Hydroxide‐Anchored Ruthenium on N‐Doped Biomass‐Derived Carbon for Stable CO ₂ Hydrogenation to Formate

ABSTRACT A scalable, one‐pot synthesis strategy was developed for the in situ formation and stabilization of Ru(OH) 3 species on a nitrogen‐doped carbon (NC) support. The synthesized Ru(OH) 3 /NC exhibits outstanding performance for CO 2 hydrogenation to formate under mild conditions, achieving the highest turnover frequency (TOF) up to 918 h −1 . Structural analysis (BET, XPS, STEM) confirms a mesopore network and nitrogen functionalities essential for stabilizing active Ru species. TOF‐SIMS and XPS measurements verify the exclusive presence of Ru(OH) 3 species in the +3‐oxidation state, while ICP reveals an increased Ru loading relative to chloride‐impregnated analogues. The catalyst retains 87% of its initial activity after five consecutive cycles, with minimum Ru leaching. Moreover, heat treatment further provided highly stable catalysts. DFT studies attribute the increased catalytic stability to strong Ru‐N interactions, particularly at Pyridinic and Pyrrolic sites. These results highlight the importance of nitrogen coordination environment and facile synthesis for the design of robust and scalable heterogeneous catalysts in CO 2 valorization.