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Hydrodeoxygenation (HDO) of phenolics is crucial for lignin-to-fuel production via fast pyrolysis. The reaction under atmospheric H2 pressure offers compatibility with pyrolysis conditions, high aromatic selectivity and low H2 consumption, but suffers from coking-induced catalyst deactivation. In this work, we report a TiOx-decorated NiSn/SiO2 catalyst (Ti-NiSn/SiO2), achieving 100% deoxygenation selectivity and enhanced stability in m-cresol HDO. The superior performance stems from: (i) the interfacial synergy between TiOx and NiSn alloy that facilitates C-O bond cleavage with a reduced energy barrier; (ii) the geometric isolation and electron-donating properties of Sn, which suppress undesirable side reactions and mitigate coke formation; and (iii) the inverse TiOx decoration strategy, which enables effective interface chemistry while minimizing acidic sites that could otherwise accelerate coking. This study presents a design strategy for constructing inverse oxide–alloy interface catalysts, offering multi-faceted advantages for HDO and other complex catalytic transformations. Hydrodeoxygenation (HDO) of phenolics is essential for converting lignin into fuels via fast pyrolysis, but catalyst deactivation from coking remains a major challenge. Here, the authors present a TiOx-decorated NiSn/SiO₂ catalyst that delivers 100% deoxygenation selectivity and significantly improved stability in the HDO of m-cresol.

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