Hydrodeoxygenation of Oxygen‐Containing Aromatic Plastic Wastes to Liquid Organic Hydrogen Carriers

Abstract To address the global plastic pollution issues and the challenges of hydrogen storage and transportation, we report a system, based on the hydrodeoxygenation (HDO) of oxygen‐containing aromatic plastic wastes, from which organic hydrogen carriers (LOHCs) can be derived. We developed a catalytic system comprised of Ru‐ReO x /SiO 2 +HZSM‐5 for direct HDO of polycarbonate (PC), polyethylene terephthalate (PET), polybutylene terephthalate (PBT), polyphenylene oxide (PPO), and their mixtures, to cycloalkanes as LOHCs, with high yields up to 99 %, under mild reaction conditions. The theoretical hydrogen storage capacity reaches ca. 5.74 wt%. The reaction pathway involves depolymerization of PC into C 15 aromatics and C 15 monophenols by direct hydrogenolysis of the C−O bond between the benzene ring and ester group, and subsequent parallel hydrogenation of C 15 aromatics and HDO of C 15 monophenols. HDO of cyclic alcohol is the rate‐determining step. The active site is Ru metallic nanoparticles with partially covered ReO x species. The excellent performance is attributed to the synergetic effect of oxophilic ReO x species and Ru metallic sites for C−O hydrogenolysis and hydrogenation, and the promotion effect of HZSM‐5 for dehydration of cyclic alcohol. The highly efficient and stable dehydrogenation of cycloalkanes over Pt/γ‐Al 2 O 3 confirms that HDO products can act as LOHCs.