Efficient CO Bond Cleavage in the Oxidized β‐O‐4 Lignin Motif Using a Carbon‐Supported Cobalt Catalyst

Herein, the synthesis and catalytic performance of cobalt‐based M–N–C materials are reported for the transfer hydrogenolysis of lignin‐derived compounds. The Co‐800 catalyst, comprising cobalt nanoparticles (CoNPs) and sub‐nanometric Co(II) species embedded in a nitrogen‐doped carbon matrix, demonstrates high activity and selectivity for CO bond cleavage in oxidized β‐O‐4 lignin model substrates using formic acid as a hydrogen donor. Subsequent acid treatment removes the CoNPs, yielding Co‐800‐AT , which retains significant catalytic activity, indicating that atomically dispersed cobalt species contribute to the observed reactivity. Both catalysts operate efficiently under mild conditions, with Co‐800 maintaining high conversion and recyclability over multiple cycles. These findings underscore the promise of Co‐based M–N–C systems as sustainable and robust catalysts for lignin depolymerization.