The production of aromatic hydrocarbons from cellulose by zeolite-catalyzed fast pyrolysis involves a complex reaction network sensitive to the zeolite structure, crystallinity, elemental composition, porosity, and acidity. The interplay of these parameters under the reaction conditions represents a major roadblock that has hampered significant improvement in catalyst design for over a decade. Here, we studied commercial and laboratory-synthesized ZSM-5 zeolites and combined data from 10 complementary characterization techniques in an attempt to identify parameters common to high-performance catalysts. Crystallinity and framework aluminum site accessibility were found to be critical to achieve high aromatic yields. These findings enabled us to synthesize a ZSM-5 catalyst with enhanced activity, which offers the highest aromatic hydrocarbon yield reported to date.
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http://dx.doi.org/10.1002/cssc.201600186 | DOI Listing |
Inorg Chem
January 2025
State Key Laboratory of Molecular & Process Engineering, SINOPEC Research Institute of Petroleum Processing, Beijing 100083, China.
The ZSM-5 zeolite is the key active component in high-severity fluid catalytic cracking (FCC) catalysts and is routinely activated by phosphorus compounds in industrial production. To date, however, the detailed structure and function of the introduced phosphorus still remain ambiguous, which hampers the rational design of highly efficient catalysts. In this work, using advanced solid-state NMR techniques, we have quantitatively identified a total of seven types of P-containing complexes in P-modified ZSM-5 zeolite and clearly revealed their structure, location, and catalytic role.
View Article and Find Full Text PDFPhys Chem Chem Phys
January 2025
UK Catalysis Hub, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, OX11 0FA, UK.
Methanol adsorption isotherms of fresh f-ZSM-5 and steamed s-ZSM-5 (Si/Al ≈ 40) are investigated experimentally at room temperature under equilibrium and by grand canonical Monte Carlo (GCMC) simulations with the aim of understanding the adsorption capacity, geometry and sites as a function of steam treatment (at 573 K for 24 h). Methanol adsorption energies calculated by GCMC are complemented by density functional theory (DFT) employing both periodic and quantum mechanics/molecular mechanics (QM/MM) techniques. Physical and textural properties of f-ZSM-5 and s-ZSM-5 are characterised by diffuse reflectance infrared Fourier transformed spectroscopy (DRIFTS) and N-physisorption, which form a basis to construct models for f-ZSM-5 and s-ZSM-5 to simulate methanol adsorption isotherms by GCMC.
View Article and Find Full Text PDFEnviron Sci Technol
January 2025
Tianjin Key Lab of Indoor Air Environmental Quality Control, School of Environmental Science and Engineering, Tianjin University, Tianjin 300350, P. R. China.
Designing catalysts with both activity and stability remains a grand challenge for the removal of chlorinated volatile organic compounds (CVOCs) by catalytic oxidation. Herein, the Ru-Mn subnanometric species encapsulated in ZSM-5 zeolite (RuMn@Z) was synthesized. It shows that the 90% conversion of dichloromethane is as low as 320 °C, which is significantly lower than that of Ru@Z (350 °C) and the impregnation catalyst (RuMn/Z, 355 °C).
View Article and Find Full Text PDFChemistry
January 2025
Boreskov Institute of Catalysis SB RAS, Siberian Branch of Russian Academy of Sciences, RUSSIAN FEDERATION.
Cu-modified zeolites provide methane conversion to methanol with high selectivity under mild conditions. The activity of different possible Cu-sites for methane transformation is still under discussion. Herein, ZSM-5 zeolite has been loaded with Cu2+ cations (1.
View Article and Find Full Text PDFPharmaceuticals (Basel)
November 2024
Faculty of Physics, Sofia University "St. Kliment Ohridski", 5 James Bourchier Blvd, 1164 Sofia, Bulgaria.
Objectives: The antimicrobial, oxidative activities, and ecotoxicity of synthesized silver-loaded zeolites (X and ZSM-5(MFI), Si-to-Al ratios 12 and 25) were studied, linking antimicrobial properties to material structure and released active silver species.
Methods: The materials were characterized by SEM, EDX, TEM, and XRPD. All materials, with a silver content of 1-3%wt for the Ss and about 35%wt for the X-zeolites, were tested against and .
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