Affiliation:
1. National Center for Magnetic Resonance in Wuhan State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics Wuhan Institute of Physics and Mathematics Innovation Academy for Precision Measurement Science and Technology Chinese Academy of Sciences 430071 Wuhan China
2. University of Chinese Academy of Sciences 100049 Beijing China
3. Key Laboratory for Advanced Materials and Joint International Research Laboratory of Precision Chemistry and Molecular Engineering Feringa Nobel Prize Scientist Joint Research Center Research Institute of Industrial Catalysis and Centre for Computational Chemistry School of Chemistry and Molecular Engineering East China University of Science and Technology 200237 Shanghai China) + These authors contributed equally to this work.
Abstract
AbstractWater is a ubiquitous component in heterogeneous catalysis over zeolites and can significantly influence the catalyst performance. However, the detailed mechanism insights into zeolite‐catalyzed reactions under microscale aqueous environment remain elusive. Here, using multiple dimensional solid‐state NMR experiments coupled with ultrahigh magic angle spinning technique and theoretical simulations, we establish a fundamental understanding of the role of water in benzene methylation over ZSM‐5 zeolite under water vapor conditions. We show that water competes with benzene for the active sites of zeolite and facilitates the bimolecular reaction mechanism. The growth of water clusters induces a micro‐hydrophobic effect in zeolite pores, which reorients benzene molecules and drives their interactions with surface methoxy species (SMS) on zeolite. We identify the formation and evolution of active SMS‐Benzene complexes in a microscale aqueous environment and demonstrate that their accumulation in zeolite pores boosts benzene conversion and methylation.
Funder
National Key Research and Development Program of China
National Natural Science Foundation of China
Youth Innovation Promotion Association of the Chinese Academy of Sciences
Natural Science Foundation of Hubei Province
Ten Thousand Talent Plans for Young Top-notch Talents of Yunnan Province
Subject
General Chemistry,Catalysis
Cited by
3 articles.
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