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Tailor and Control of acidic strength in Ordered Mesoporous Aluminosilicates by Using Preformed Zeolite Precursors

Chinese Journal of Chemistry 2004年第1期22卷 9-13页

作者：林森王利丰韩宇于沂邸岩王润伟蒋大振肖丰收 State Key Laboratory of Inorganic Synthesis and Preparative Chemistry & Department of Chemistry

The acidic strength of ordered mesoporous aluminosilicates of MAS-2, MAS-3, MAS-7 and MAS-9 and mi-croporous crystals of Y, L, beta, and ZSM-5 zeolites was systemically investigated by temperature-programmed desorption of ammonia (NH3-TPD). Due to the use of preformed zeolite precursors of Y, L, beta and ZSM-5, the ordered mesoporous aluminosilicates with distinguished acidic strength were obtained, being dependent on the type of preformed zeolite precursors. Therefore, the acidic strength of these mesoporous aluminosilicates could be tai-lored and controlled.

关键词： NH3-TPD acidic strength ordered mesoporous aluminosilicate preformed zeolite precursor

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构筑开放锡位点实现酸性增强的二甲醚羰基化丝光沸石催化剂设计

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Engineering 2024年第4期35卷 104-114页

作者： Ying Li Man Yu Guodong Qi Yunduo Liu Jing Lv Shouying Huang Xinbin Ma Key Laboratory for Green Chemical Technology of Ministry of Education Collaborative Innovation Center of Chemical Science and EngineeringSchool of Chemical Engineering and TechnologyTianjin UniversityTianjin 300350China National Center for Magnetic Resonance in Wuhan&State Key Laboratory of Magnetic Resonance and Atomic and Molecular Physics&Key Laboratory of Magnetic Resonance in Biological Systems Wuhan Institute of Physics and MathematicsInnovation Academy for Precision Measurement Science and TechnologyChinese Academy of SciencesWuhan 430071China Inner Mongolia Key Laboratory of Industrial Catalysis College of Chemical EngineeringInner Mongolia University of TechnologyHohhot 010051China

Due to their tunable acidity,shape selectivity,and excellent stability,zeolites are of great importance as solid acid materials in industrial *** the properties of the acid sites in zeolites allows for the rational design and fabrication of catalysts for target *** ether(DME)carbonylation,a critical chain-growth reaction for C1 resource utilization,is selectively catalyzed by the Brønsted acid sites within the eight-membered rings(8-MRs)of mordenite(MOR).It is anticipated that strengthening the Brønsted acidity—particularly in 8-MRs—will improve the catalytic performance of *** this work,density functional theory(DFT)calculations are first employed and the results used to design a modified MOR with stannum(Sn)and to predict the corresponding changes in *** by the theoretical studies,a series of Sn-modified MOR are synthesized via a defect-engineering and subsequent heteroatom-substitution *** partial desilication,isolated tetrahedral Sn species in an open configuration are successfully synthesized for the first time,within which tetrahedrally coordinated Al sites are *** acidic characterization is used to confirm that the acidity of the Brønsted acid sites is enhanced by the introduction of the Sn species;as a result,the sample exhibits excellent activity in DME carbonylation *** and DFT studies reveal that this strengthened acidity facilitates the adsorption of DME and reduces the activation barriers of DME dissociation and acetyl formation,accounting for the improved *** work demonstrates mechanistic insights into the promoting effects of strong acidity on DME carbonylation and offers a promising strategy to precisely control the acidic strength of zeolites.

关键词： Zeolite Sn modification Carbonylation Brønsted acid catalysis acidic strength

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