Metal-free catalytic hydropyrolysis of cellulose-rich waste to jet-fuel aromatics via zeolite-enabled hydrogen activation and deep deoxygenation

Sustainable aviation fuel (SAF) requires aromatic hydrocarbons for maintaining jet fuel compatibility and performance; however, current aromatics are primarily fossil-derived, necessitating renewable routes from biomass. Herein, we demonstrate an integrated, metal-free catalytic hydropyrolysis approach to convert cellulose-derived waste directly into SAF-relevant aromatic hydrocarbons using ZSM-5 zeolites. Under a pressurized hydrogen atmosphere (0.4 MPa), cellulose predominantly yields stable ketone-rich oxygenates. Introducing ZSM-5 dramatically transforms these intermediates, with aromatic hydrocarbons accounting for approximately 98% of the total GC-MS peak area of the detected volatile organic products. The major aromatic products were further quantified using compound-specific external calibration with authentic standards. Comprehensive studies reveal that ZSM-5 with a low SiO 2 /Al 2 O 3 ratio (27) exhibits superior catalytic performance, completely deoxygenating oxygenates through Brønsted-acid-mediated hydrogen activation without metal assistance. Increasing the catalyst-to-feedstock ratio significantly enhances aromatic yields, facilitating polycyclic aromatic formation via intensified secondary condensation reactions. Furthermore, extending the optimized conditions to diverse real-world feedstocks—including pinewood and textile wastes—validates the process robustness, consistently achieving high aromatic selectivity (>90%). This work provides new perspectives on metal-free hydrogen activation by zeolite acidity, paving a promising pathway for converting cellulose-rich wastes into SAF-precursor aromatic hydrocarbons.