Effects of crystal size on methanol to hydrocarbon conversion over single crystals of ZSM-5 studied by synchrotron infrared microspectroscopy

Ivalina B Minova, Santhosh K. Matam, Alex Greenaway, C. Richard A. Catlow, Mark D. Frogley, Gianfelice Cinque, Paul A. Wright* (Corresponding Author), Russell F. Howe* (Corresponding Author)

*Corresponding author for this work

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Abstract

Operando synchrotron infrared microspectroscopy (OIMS) was used to study the conversion of methanol over coffin-shaped HZSM-5 crystals of different sizes: large (∼250 × 80 × 85 μm3), medium (∼160 × 60 × 60 μm3) and small (∼55 × 30 × 30 μm3). The induction period, for direct alkene formation by deprotonation of surface methoxy groups, was found to decrease with decreasing crystal size and with increasing reaction temperature. Experiments with a continuous flow of dimethylether showed that evolution of the hydrocarbon pool and indirect alkene formation is also strongly dependent on crystal size. These measurements suggest that the hydrocarbon pool formation and indirect alkene generation should be almost instantaneous at reaction temperatures used in practical catalysis with crystal sizes typically ∼1 μm3.

Original languageEnglish
Pages (from-to)18849-18859
Number of pages11
JournalPhysical Chemistry Chemical Physics
Volume22
Issue number34
Early online date5 Mar 2020
DOIs
Publication statusPublished - 8 Sept 2020

Bibliographical note

IBM and PAW would like to thank the EPSRC and CRITICAT Centre for Doctoral Training for Financial Support [PhD studentship to IBM, and supplementary equipment grant EP/L016419/1]. The UK Catalysis Hub is thanked for resources and support provided via membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/I038748/1, EP/I019693/1, EP/K014706/1, EP/K014668/1, EP/K014854/1, EP/K014714/1 and EP/M013219/1). We thank the Diamond Light Source for provision of beam time and support facilities at the MIRIAM beamline B22 (Experiments SM13725-1, SM16257-1, SM18680-1, SM20906-1). IBM and PAW thank EPSRC and CRTICAT Centre for Doctoral Training for a PhD Studentship (grant EP/IO17008/1) and Supplementary Equipment Grant (EP/L016419/1). We thank Pit Losch and Hans J. Bongard, Max-Planck-Institut fur Kohlenforschung for cross-sectional SEM-EDX analysis, Daniel M. Dawson, University of St Andrews, for solid state NMR, and Juan M.Gonzalez-Carballo, University of St Andrews, for assistance with ammonia TPD. The research data supporting this publication can be accessed at https://doi.org/10.17630/306bd3c3-014b-466f-9538-b107628c847d.

Keywords

  • SURFACE METHOXY GROUPS
  • IR MICROSPECTROSCOPY
  • ZEOLITES
  • OLEFINS
  • PROFILES
  • HZSM-5

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