Probing the dynamics of methanol in copper-loaded zeolites via quasi-elastic and inelastic neutron scattering

被引:0
作者
Skukauskas, Vainius [1 ,2 ]
De Souza, Nicolas [3 ]
Gibson, Emma K. [1 ,2 ]
Silverwood, Ian P. [1 ,4 ]
机构
[1] Harwell Sci & Innovat Campus, Rutherford Appleton Lab, UK Catalysis Hub, Res Complex Harwell, Harwell OX11 0FA, England
[2] Univ Glasgow, Sch Chem, Glasgow City G12 8QQ, Scotland
[3] Australian Nucl Sci & Technol Org ANSTO, Melbourne, NSW 2232, Australia
[4] Harwell Sci & Innovat Campus, Sci & Technol Facil Council, Rutherford Appleton Lab, ISIS Neutron & Muon Facil, Harwell OX11 0QX, England
关键词
quasielastic neutron scattering; inelastic neutron scattering; methanol; diffusion; zeolites; DIFFUSION; ALKANES; VISUALIZATION;
D O I
10.1007/s11705-024-2506-1
中图分类号
TQ [化学工业];
学科分类号
0817 ;
摘要
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 x 10-10 and 2.59 x 10-10 m2<middle dot>s-1. Non-Arrhenius behavior was observed with varying temperature due to methoxy formation at Br & oslash;nsted acid sites and methanol clustering around copper cations.
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页数:6
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共 26 条
[1]   Mantid-Data analysis and visualization package for neutron scattering and μ SR experiments [J].
Arnold, O. ;
Bilheux, J. C. ;
Borreguero, J. M. ;
Buts, A. ;
Campbell, S. I. ;
Chapon, L. ;
Doucet, M. ;
Draper, N. ;
Leal, R. Ferraz ;
Gigg, M. A. ;
Lynch, V. E. ;
Markvardsen, A. ;
Mikkelson, D. J. ;
Mikkelson, R. L. ;
Miller, R. ;
Palmen, K. ;
Parker, P. ;
Passos, G. ;
Perring, T. G. ;
Peterson, P. F. ;
Ren, S. ;
Reuter, M. A. ;
Savici, A. T. ;
Taylor, J. W. ;
Taylor, R. J. ;
Tolchenoy, R. ;
Zhou, W. ;
Zikoysky, J. .
NUCLEAR INSTRUMENTS & METHODS IN PHYSICS RESEARCH SECTION A-ACCELERATORS SPECTROMETERS DETECTORS AND ASSOCIATED EQUIPMENT, 2014, 764 :156-166
[2]   DAVE: A Comprehensive Software Suite for the Reduction, Visualization, and Analysis of Low Energy Neutron Spectroscopic Data [J].
Azuah, Richard Tumanjong ;
Kneller, Larry R. ;
Qiu, Yiming ;
Tregenna-Piggott, Philip L. W. ;
Brown, Craig M. ;
Copley, John R. D. ;
Dimeo, Robert M. .
JOURNAL OF RESEARCH OF THE NATIONAL INSTITUTE OF STANDARDS AND TECHNOLOGY, 2009, 114 (06) :341-358
[3]  
Be M., 1988, Biology and Materials Science
[4]   Influence of Topology and Bronsted Acid Site Presence on Methanol Diffusion in Zeolites Beta and MFI [J].
Botchway, Cecil H. ;
Tia, Richard ;
Adei, Evans ;
O'Malley, Alexander J. ;
Dzade, Nelson Y. ;
Hernandez-Tamargo, Carlos ;
de Leeuw, Nora H. .
CATALYSTS, 2020, 10 (11) :1-18
[5]   SOLUBLE METHANE MONO-OXYGENASE OF METHYLOCOCCUS-CAPSULATUS-(BATH) - ABILITY TO OXYGENATE NORMAL-ALKANES, NORMAL-ALKENES, ETHERS, AND ALICYCLIC, AROMATIC AND HETEROCYCLIC-COMPOUNDS [J].
COLBY, J ;
STIRLING, DI ;
DALTON, H .
BIOCHEMICAL JOURNAL, 1977, 165 (02) :395-402
[6]  
de Souza Nicolas R., 2016, Neutron News, V27, P20, DOI 10.1080/10448632.2016.1163985
[7]  
Gibson E., 2022, STFC ISIS Neutron and Muon Source
[8]   HIGH-TEMPERATURE PULSED FIELD GRADIENT NUCLEAR-MAGNETIC-RESONANCE SELF-DIFFUSION MEASUREMENTS OF N-ALKANES IN MFI-TYPE ZEOLITES [J].
HEINK, W ;
KARGER, J ;
PFEIFER, H ;
DATEMA, KP ;
NOWAK, AK .
JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1992, 88 (23) :3505-3509
[9]  
Lin D H., 1989, Studies in Surface Science and Catalysis, V46, P615, DOI [10.1016/S0167-2991(08)61016-2, DOI 10.1016/S0167-2991(08)61016-2]
[10]   Methanol dynamics in H-ZSM-5 with Si/Al ratio of 25: a quasi-elastic neutron scattering (QENS) study [J].
Matam, Santhosh K. ;
Catlow, C. Richard A. ;
Silverwood, Ian P. ;
O'Malley, Alexander J. .
TOPICS IN CATALYSIS, 2021, 64 (9-12) :699-706