Phosphorous Modified ZSM-5 Zeolites: Impact on Methanol Conversion into Olefins

Losch, Pit; Laugel, Guillaume; Martínez-Espín, Juan S.; Chavan, Sachin; Olsbye, Unni; Louis, Benoît

doi:10.1007/s11244-015-0449-y

Cited by 21 publications

(15 citation statements)

References 31 publications

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“…[39] We thus prepared various ZSM-5 zeolites (named ZSM-5F) in fluoride aqueous solution at neutral pH, under conditions adapted from our previous studies. [40,41,42] Several factors, such as silicon source, fluoride concentration, volume, pH, chemical composition, were systematically evaluated (Table S1). To favor the formation of single, large (as perfect as possible) crystals, highly diluted gels were used.…”

Section: Synthesis Of Perfect Zsm-5 Crystalsmentioning

confidence: 99%

H-ZSM-5 zeolite model crystals: Structure-diffusion-activity relationship in methanol-to-olefins catalysis

Losch

Pinar

Willinger

et al. 2017

Journal of Catalysis

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106

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Large ZSM-5 zeolite crystals synthesized in fluoride medium show an astonishing activity, stability as well as selectivity towards light olefins in the Methanol-To-Olefins (MTO) reaction. By proper control of the synthesis parameters, ZSM-5 single crystals of unprecedented high quality are produced. The absence of usually uncontrollable variables such as structural defects, external non selective surface acid sites and extra-framework aluminium (EFAl) species was evidenced by SEM, HRTEM, CO-FTIR, ²⁷Al and ¹⁹F MAS-NMR, Rietveld structure refinement and N₂- and Ar-gas sorption measurements. Interestingly, diffusivity evaluation of different probe molecules (toluene, benzene and neopentane) has been carried out with PFG-NMR, allowing casting light on an interesting structure-diffusion-activity relationship. A “levitation” effect could be experimentally demonstrated and its impact on catalysis is highlighted in a rationalization attempt: Maxwell-Boltzmann based diffusion models properly predict product distributions for this counter-intuitively outstanding Methanol-To-Propylene (MTP) catalyst

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Section: Synthesis Of Perfect Zsm-5 Crystalsmentioning

confidence: 99%

H-ZSM-5 zeolite model crystals: Structure-diffusion-activity relationship in methanol-to-olefins catalysis

Losch

Pinar

Willinger

et al. 2017

Journal of Catalysis

Self Cite

106

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“…The higher the acid site dispersion is, the higher the selectivity towards C 2 -C 4 olefins is. [48] (c) [40] and (d) [49].…”

Section: Entry Zeolite Conversion [%] S(para) [%] S(ortho) [%] a Tof mentioning

confidence: 99%

“…Hyperbolic correlation between light olefins selectivity over tested ZSM-5 zeolites and their respective calculated surface acid site densities (calculated using their total exchangeable hydrons, obtained by H/D-isotope exchange technique, and the total BET surface area). (a) Reported in [47] (b) [48] (c) [40] and (d) [49].…”

Section: Zeolitesmentioning

confidence: 99%

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

et al. 2017

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Abstract:A top-down desilication of Al-rich ZSM-5 zeolites and a bottom-up mesopores creating method were evaluated in this study. Three liquid-solid and one gas-solid heterogeneously-catalysed reactions were chosen to establish relationships between zeolites textural properties and their catalytic behavior in acid-catalysed model reactions that are influenced by shape selectivity: Diels-Alder cyclization between isoprene and methylacrylate, Methanol-to-Olefins (MTO) reaction, chlorination of iodobenzene with trichloroisocyanuric acid (TCCA), and Friedel-Crafts acylation of anisole by carboxylic acids with differing sizes. It is found amongst others that no optimal mesoporosity for all the different reactions can be easily obtained, but depending on the chosen application, a specific treatment has to be set to achieve high activity/selectivity and stability.

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“…Table shows the concentration and strength distribution of acid sites of these samples. The concentration of three acid sites of H[P, Al]‐ZSM‐5 is decreased after introduction of phosphorus species into HZSM‐5 structure, indicating that phosphorus is interacted with the acid sites of ZSM‐5 and engenders adjacent OH groups by isomorphously substituted of phosphorus element with Al . Similarly, the concentration of three kind acid sites on H[P, Al]‐ZSM‐5‐AT‐0.05 M and H[P, Al]‐ZSM‐5‐HT‐0.1 M is decreased compared to H[P, Al]‐ZSM‐5.…”

Section: Introductionmentioning

confidence: 99%

Synthesis of Hierarchically Porous H[P, Al]‐ZSM‐5 and its Catalytic Performance in Coupling Transformation of Methanol with 1‐Butene

et al. 2019

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Hierarchically porous P substituted HZSM‐5 (H[P, Al]‐ZSM‐5‐AT‐0.05 M ) was successfully synthesized by isomorphous substitution method with introduced P atoms into ZSM‐5 zeolite frameworks followed by alkali treatment. H[P, Al]‐ZSM‐5‐AT‐0.05 M was characterized by XRD, ICP‐OES, SEM, FT‐IR, N2 adsorption‐desorption, NH3‐TPD, XPS, Py‐IR, and TG‐DTA, respectively. The surface area, pore volume, particle size and P/Al (molar ratio) are 328 m2.g−1, 0.23 cm3.g−1, 563 nm and 0.027, respectively. The catalytic performance of H[P, Al]‐ZSM‐5‐AT‐0.05 M in coupling reaction of methanol with 1‐butene was investigated in the fixed‐bed reactor. On the condition of reaction temperature at 500°C under atmosphere pressure, the main product is propylene with the selectivity and yield of 33.7% and 31.0%, respectively. Hydrogen transfer index was calculated to 0.24. Moreover, its diffusion limitation was investigated with the self‐etherification of benzyl alcohol reaction. The value of Thiele modulus (η ) and effectiveness factor (ϕ ) are 0.08 and 16.9, respectively.

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Phosphorous Modified ZSM-5 Zeolites: Impact on Methanol Conversion into Olefins

Cited by 21 publications

References 31 publications

H-ZSM-5 zeolite model crystals: Structure-diffusion-activity relationship in methanol-to-olefins catalysis

H-ZSM-5 zeolite model crystals: Structure-diffusion-activity relationship in methanol-to-olefins catalysis

Mesoporous ZSM-5 Zeolites in Acid Catalysis: Top-Down vs. Bottom-Up Approach

Synthesis of Hierarchically Porous H[P, Al]‐ZSM‐5 and its Catalytic Performance in Coupling Transformation of Methanol with 1‐Butene

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