氢解
催化作用
化学
苯
钌
甲苯
吸附
选择性
光化学
密度泛函理论
无机化学
有机化学
计算化学
作者
Mingxing Ye,Yurou Li,Zhirong Yang,Chang Yao,Weixiao Sun,Xiangxue Zhang,Wenyao Chen,Gang Qian,Xuezhi Duan,Yueqiang Cao,Lina Li,Xin Zhou,Jing Zhang
标识
DOI:10.1002/ange.202301024
摘要
Abstract Polyethylene terephthalate (PET) hydrogenolysis can produce benzene, toluene, and xylene (BTX), where the selectivity control is challenging. We report a reaction pathway dictated by the Ru coordination environment by examining the binding geometries of adsorbates on differently coordinated Ru centers and their evolution during PET hydrogenolysis. A BTX yield of 77 % was obtained using a Ru/TiO 2 with a Ru coordination number of ca. 5.0 where edge/corner sites are dominant, while more gas and saturated products were formed for Ru/TiO 2 containing primarily terrace sites. Density functional theory and isotopic labelling revealed that under‐coordinated Ru edge sites favor “upright” adsorption of aromatic adsorbates while well‐coordinated Ru sites favor “flat‐lying” adsorption, where the former mitigates ring hydrogenation and opening. This study demonstrates that reaction pathways can be directed through controlled reactant/intermediate binding via tuning of the Ru coordination environment for efficient conversion of PET to BTX.
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