Synchronizing Lewis‐Acid C─O Bond Activation and Ethanol‐Derived Hydrogen Transfer Over RuO 2 /ZnO Carbon Aerogels for Technical Lignin Depolymerization

ABSTRACT Technical lignin depolymerization is constrained by a kinetic mismatch between the cleavage of residual aryl ether bonds and the stabilization of the resulting highly reactive fragments that are generated. This imbalance promotes rapid C─C condensation, and thereby limits aromatic monomers formation. Herein, a lignosulfonate‐derived RuO 2 /ZnO carbon aerogel is constructed to synchronize C─O bond activation by Lewis acid sites with ethanol‐mediated hydrogen transfer depolymerization of enzymatic hydrolysis lignin under N 2 . A metal‐directed gelation calcination route that organized Ru and Zn species within a polyacrylamide‐lignosulfonate network. This process yields a hierarchically porous, N‐doped carbon framework with closely connected and electronically coupled RuO 2 /ZnO domains, this architecture creates a coupled catalytic microenvironment. Zn‐containing Lewis acidic sites polarize oxygenated linkages, whereas Ru sites activate ethanol to deliver transferable hydrogen species. ZnCl 2 serves as a mobile Lewis acid cocatalyst to further promote aryl ether and β– O–4 activation. Under optimized conditions, phenol, guaiacol, and syringol type monomers are produced without external H 2 , increasing the aromatic monomer yield from 16.5% to 21.2%. Mechanistic studies and calculations reveal that ZnCl 2 accelerates C─O bond activation, while the RuZn interface stabilizes quinone methide‐like intermediates through ethanol‐derived hydrogen transfer.