Ruthenium/TiO2‐Catalyzed Hydrogenolysis of Polyethylene Terephthalate: Reaction Pathways Dominated by Coordination Environment

• DOI: 10.1002/anie.202301024
• Publication Date: 2023-03-13T13:32:02Z
• Authors: Mingxing Ye; Yurou Li; Zhirong Yang; Chang Yao; Weixiao Sun; Xiangxue Zhang; Wenyao Chen; Gang Qian; Xuezhi Duan; Yueqiang Cao; Lina Li; Xinggui Zhou; Jing Zhang
• Keywords: Hydrogenolysis

Polyethylene terephthalate (PET) hydrogenolysis can produce benzene, toluene, and xylene (BTX), where the selectivity control is challenging. We report a reaction pathway dictated by Ru coordination environment examining binding geometries of adsorbates on differently coordinated centers their evolution during PET hydrogenolysis. A BTX yield 77 % was obtained using Ru/TiO2 with number ca. 5.0 edge/corner sites are dominant, while more gas saturated products were formed for containing primarily terrace sites. Density functional theory isotopic labelling revealed that under-coordinated edge favor "upright" adsorption aromatic well-coordinated "flat-lying" adsorption, former mitigates ring hydrogenation opening. This study demonstrates pathways be directed through controlled reactant/intermediate via tuning efficient conversion to BTX.