<p>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.</p>

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Direct conversion of enzymatic hydrolysis lignin to jet fuel via relay catalysis

  • Hanzhang Gong,
  • Lu Wang,
  • Xiang Li,
  • Yuan Zhuang,
  • Yuhan Ma,
  • Yushuai Sang,
  • Yongdan Li,
  • Zhaofu Fei,
  • Paul J. Dyson

摘要

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.