The selective transformation of lignin into valuable products remains challenging due to its structural heterogeneity and tendency to undergo recondensation. Here we report a spatially engineered bifunctional core–shell catalyst, Ni@H-beta, featuring nanodispersed Ni species on the external shell of a zeolite containing Brønsted acid sites within the core. This architecture enables a relay catalytic process involving hydrogenation on the Ni-rich surface followed by acid-catalyzed deoxygenation within the microporous framework. Under optimized conditions, Ni@H-beta achieves complete liquefaction of enzymatic hydrolysis lignin without char formation, yielding 50.1 wt% monomers predominantly composed of jet-fuel-range cycloalkanes. Operando NMR spectroscopy combined with density functional theory reveals a hydrogenation-first pathway that reduces deoxygenation barriers and enhances selectivity. Integrated process simulation, techno-economic analysis and life-cycle assessment further indicate that the EHL-to-jet-fuel process is economically competitive and environmentally advantageous compared with conventional petroleum-derived jet fuel. Structural complexity often hinders the efficient conversion of lignin into sustainable high-value products. This bifunctional core–shell catalyst enables a relay reaction that transforms lignin into jet-fuel range cycloalkanes with high yields.
Gong et al. (Tue,) studied this question.