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Ruthenium/TiO2 -Catalyzed Hydrogenolysis of Polyethylene Terephthalate: Reaction Pathways Dominated by Coordination Environment.
Ye, Mingxing; Li, Yurou; Yang, Zhirong; Yao, Chang; Sun, Weixiao; Zhang, Xiangxue; Chen, Wenyao; Qian, Gang; Duan, Xuezhi; Cao, Yueqiang; Li, Lina; Zhou, Xinggui; Zhang, Jing.
Afiliação
  • Ye M; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Li Y; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Yang Z; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Yao C; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Sun W; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Zhang X; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Chen W; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Qian G; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Duan X; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Cao Y; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Li L; Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201204, China.
  • Zhou X; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
  • Zhang J; State Key Laboratory of Chemical Engineering, East China University of Science and Technology, Shanghai, 200237, China.
Angew Chem Int Ed Engl ; 62(19): e202301024, 2023 May 02.
Article em En | MEDLINE | ID: mdl-36912609
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/TiO2 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/TiO2 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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Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2023 Tipo de documento: Article
Texto completo
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XML
PubMed Links
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Texto completo: 1 Base de dados: MEDLINE Idioma: En Ano de publicação: 2023 Tipo de documento: Article