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Hydrodeoxygenation of Oxygen-Containing Aromatic Plastic Wastes to Liquid Organic Hydrogen Carriers.
Angewandte Chemie 2023 August 4
To address the global plastic pollution issues and the challenges of hydrogen storage and transportation, we report a new class of liquid organic hydrogen carriers (LOHCs) system based on the hydrodeoxygenation (HDO) of oxygen-containing aromatic plastic wastes. We developed a catalytic system comprised of Ru-ReOx/SiO2 + 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 yield up to 99% under mild reaction conditions. The theoretical hydrogen storage capacity can reach to ~5.74 wt%. The reaction pathway involves depolymerization of PC into C15 aromatics and C15 monophenols by direct hydrogenolysis of the C-O bond between the benzene ring and ester group, and subsequent parallel hydrogenation of C15 aromatics and HDO of C15 monophenols. HDO of cyclic alcohol is the rate determining step. The active site is Ru metallic nanoparticles with partially covered ReOx species. The excellent performance is attributed to the synergetic effect of oxophilic ReOx 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 stably dehydrogenation of cycloalkanes over Pt/γ-Al2O3 confirms that HDO products can act as LOHCs.
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