Spatially Orthogonal Metal–Zeolite Catalysts for One-Step Phenol Synthesis from Birch Lignin Oil

Phenol, a cornerstone of chemical manufacturing, is currently derived from fossil resources via the energy-intensive cumene process. Lignin, the most abundant renewable source of aromatic rings, is an attractive alternative, yet its direct conversion to phenol remains unachieved due to the poor reactivity of syringyl (S)-type monomers and the difficulty of integrating demethoxylation and dealkylation within a stable catalyst. Here we report a spatially orthogonal metal-zeolite catalyst that resolves these challenges. Mo⁰ sites, generated with exceptionally high enrichment from CuMoO₄ precursors, interact strongly with aromatic rings, enabling flat adsorption and selective methoxy removal from both guaiacyl (G)- and S-type monomers, assisted by hydrogen spillover from Cu⁰. A nanoscale silica shell encapsulates HZSM-5 nanosheets, spatially shielding Brønsted acid sites from phenolic-induced coking and deactivation while preserving their accessibility for selective dealkylation. This integrated architecture achieves near-quantitative conversion of both G- and S-type monomers and, crucially, enables the first direct one-step phenol production from birch lignin oil with exceptional yield and stability.