Probing the dynamics of methanol in copper-loaded zeolites via quasi-elastic and inelastic neutron scattering
Vainius Skukauskas1,2, Nicolas De Souza3, Emma K. Gibson1,2, Ian P. Silverwood1,4()
. UK Catalysis Hub, Research Complex at Harwell, Rutherford Appleton Laboratory, Harwell Science and Innovation Campus, OX11 0FA, UK . School of Chemistry, University of Glasgow, Glasgow, G12 8QQ, UK . Australian Nuclear Science and Technology Organisation (ANSTO), NSW 2232, Australia . ISIS Neutron and Muon Facility, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Science and Innovation Campus, OX11 0QX, UK
The dynamics of methanol within prototype methanol synthesis catalysts were studied using quasi-elastic neutron scattering. Three Cu-exchanged zeolites (mordenite, SSZ-13 and ZSM-5) were studied after methanol loading and showed jump diffusion coefficients between 1.04 × 10−10 and 2.59 × 10−10 m2·s–1. Non-Arrhenius behavior was observed with varying temperature due to methoxy formation at Brønsted acid sites and methanol clustering around copper cations.
Just Accepted Date: 05 July 2024Issue Date: 28 November 2024
Cite this article:
Vainius Skukauskas,Nicolas De Souza,Emma K. Gibson, et al. Probing the dynamics of methanol in copper-loaded zeolites via quasi-elastic and inelastic neutron scattering[J]. Front. Chem. Sci. Eng.,
2025, 19(1): 5.
Fig.1 Fits applied to the data from (a, d, g) CuMOR, (b, e, h) CuSSZ13, and (c, f, i) CuZSM5 at 375 K for Q values of (a,b,c) 0.4, (d, e, f) 1.0, and (g, h, i) 1.8 ?–1.
Fig.2 Lorentzian linewidths of the quasielastic component from the QENS spectra and the SS jump diffusion model applied. (a), (b), (c) and (d) correspond to data obtained at 300, 325, 350, and 375 K respectively.
Sample
T/K
/?
/ps
Ds/( × 10?10 m2·s–1)
CuMOR
300
2.0 ± 0.3
47.8 ± 11.0
1.3 ± 0.5
CuMOR
325
2.9 ± 0.4
77.2 ± 13.2
1.8 ± 0.6
CuMOR
350
2.9 ± 0.4
76.4 ± 12.2
1.8 ± 0.6
CuMOR
375
1.8 ± 0.2
51.3 ± 10.3
1.0 ± 0.4
CuSSZ13
300
3.7 ± 0.3
90.2 ± 8.9
2.6 ± 0.5
CuSSZ13
325
3.3 ± 0.3
80.8 ± 7.2
2.2 ± 0.4
CuSSZ13
350
3.3 ± 0.2
72.8 ± 6.2
2.5 ± 0.4
CuSSZ13
375
2.7 ± 0.2
53.2 ± 5.0
2.3 ± 0.4
CuZSM5
300
2.4 ± 0.2
77.5 ± 10.3
1.2 ± 0.3
CuZSM5
325
2.7 ± 0.2
81.5 ± 9.1
1.5 ± 0.3
CuZSM5
350
3.1 ± 0.3
83.8 ± 8.4
1.9 ± 0.4
CuZSM5
375
2.4 ± 0.2
59.6 ± 6.3
1.6 ± 0.4
Tab.1 Jump lengths, residence times and diffusion coefficients derived from QENS
Fig.3 INS spectra of methanol adsorbed on the three zeolites at 350 K.
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