Abstract Selective depolymerization of industrial lignin into separable aromatic chemicals is crucial for a renewable carbon cycle, yet its condensed structure and parallel reactions severely limit monomer yield and selectivity. We report a hierarchical porous NiCo alloy catalyst with a Lewis acid‐enriched metal–acid interface for efficient lignin hydrogenolysis. Alloying‐induced electronic reconstruction promotes charge transfer from Ni to Co, downshifting the d‐band center to optimize oxygenated intermediate adsorption, lower C–O cleavage energy barriers, and suppress overhydrogenation and recondensation. The optimized Ni:Co = 1:2 catalyst affords approximately 22 wt% phenolic monomers with 92.3% selectivity under mild conditions. Structural analyses confirm extensive cleavage of β‐O‐4, β‐β, and β‐5 linkages with reduced molecular weight, and the catalyst shows good magnetic recyclability. This work establishes a direct correlation between electronic structure modulation and interfacial catalytic synergy, providing a scalable strategy for the efficient valorization of technical lignin into aromatic chemicals.
Zou et al. (Sun,) studied this question.