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Understanding the Fundamentals of Microporosity Upgrading in Zeolites: Increasing Diffusion and Catalytic Performances.
Qin, Zhengxing; Zeng, Shu; Melinte, Georgian; Bucko, Tomás; Badawi, Michael; Shen, Yanfeng; Gilson, Jean-Pierre; Ersen, Ovidiu; Wei, Yingxu; Liu, Zhongmin; Liu, Xinmei; Yan, Zifeng; Xu, Shutao; Valtchev, Valentin; Mintova, Svetlana.
Afiliación
  • Qin Z; State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China.
  • Zeng S; National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China
  • Melinte G; University of Chinese Academy of Sciences, Beijing, 100049, China.
  • Bucko T; Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess BP 43, Strasbourg, F-67034, France.
  • Badawi M; Department of Physical and Theoretical Chemistry, Faculty of Natural Sciences, Comenius University in Bratislava, Ilkovicova 6, Bratislava, SK-84215, Slovakia.
  • Shen Y; Institute of Inorganic Chemistry, Slovak Academy of Sciences, Dúbravská cesta 9, Bratislava, SK-84236, Slovakia.
  • Gilson JP; Laboratoire de Physique et Chimie Théoriques, UMR 7019, CNRS - Université de Lorraine, Nancy, F-54000, France.
  • Ersen O; State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China.
  • Wei Y; Normandie Univ, ENSICAEN, UNICAEN, CNRS, Laboratoire Catalyse et Spectrochimie, 6 Boulevard Maréchal Juin, Caen, 14050, France.
  • Liu Z; Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess BP 43, Strasbourg, F-67034, France.
  • Liu X; National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China
  • Yan Z; National Engineering Laboratory for Methanol to Olefins, Dalian National Laboratory for Clean Energy, iChEM (Collaborative Innovation Center of Chemistry for Energy Materials), State Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China
  • Xu S; University of Chinese Academy of Sciences, Beijing, 100049, China.
  • Valtchev V; State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China.
  • Mintova S; State Key Laboratory of Heavy Oil Processing, College of Chemical Engineering, China University of Petroleum (East China), Qingdao, 266580, China.
Adv Sci (Weinh) ; 8(17): e2100001, 2021 Sep.
Article en En | MEDLINE | ID: mdl-34219412
Hierarchical zeolites are regarded as promising catalysts due to their well-developed porosity, increased accessible surface area, and minimal diffusion constraints. Thus far, the focus has been on the creation of mesopores in zeolites, however, little is known about a microporosity upgrading and its effect on the diffusion and catalytic performance. Here the authors show that the "birth" of mesopore formation in faujasite (FAU) type zeolite starts by removing framework T atoms from the sodalite (SOD) cages followed by propagation throughout the crystals. This is evidenced by following the diffusion of xenon (Xe) in the mesoporous FAU zeolite prepared by unbiased leaching with NH4 F in comparison to the pristine FAU zeolite. A new diffusion pathway for the Xe in the mesoporous zeolite is proposed. Xenon first penetrates through the opened SOD cages and then diffuses to supercages of the mesoporous zeolite. Density functional theory (DFT) calculations indicate that Xe diffusion between SOD cage and supercage occurs only in hierarchical FAU structure with defect-contained six-member-ring separating these two types of cages. The catalytic performance of the mesoporous FAU zeolite further indicates that the upgraded microporosity facilitates the intracrystalline molecular traffic and increases the catalytic performance.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Sci (Weinh) Año: 2021 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Idioma: En Revista: Adv Sci (Weinh) Año: 2021 Tipo del documento: Article País de afiliación: China Pais de publicación: Alemania