Probing the dynamics and structure of confined benzene in MCM-41 based catalysts

Daniel Dervin; Alexander O'Malley; Marta Falkowska; Sarayute Chansai; Ian Silverwood; Christopher Hardacre; C. Richard A.  Catlow

doi:10.1039/D0CP01196G

Probing the dynamics and structure of confined benzene in MCM-41 based catalysts

Daniel Dervin, Alexander O'Malley, Marta Falkowska, Sarayute Chansai, Ian Silverwood, Christopher Hardacre, C. Richard A. Catlow

Department of Chemistry

Research output: Contribution to journal › Article › peer-review

13 Citations (SciVal)

Abstract

A combination of Molecular Dynamics (MD) simulations and Quasielastic Neutron Scattering (QENS) experiments has been used to investigate the dynamics and structure of benzene in MCM-41 based catalysts. QENS experiments of benzene as both an unconfined liquid and confined in the catalyst Pt/MCM-41 find that the mobility of benzene decreases upon confinement as shown by the decreased diffusion coefficients. Complementary MD simulations on benzene in MCM-41 show agreement with the QENS experiments when using a novel fully flexible model of MCM-41. Structural information from the MD simulations show that benzene in MCM-41 has a significantly different structure from that of the bulk liquid; with benzene molecules closer together and no prefered orientation.

Original language	English
Journal	Physical Chemistry Chemical Physics
DOIs	https://doi.org/10.1039/D0CP01196G
Publication status	Published - 11 May 2020

Funding

The authors acknowledge the use of the UCL Legion High Performance Computing Facility (Legion@UCL), and associated support services, in the completion of this work. UK Catalysis Hub is kindly thanked for resources and support provided via our membership of the UK Catalysis Hub Consortium and funded by EPSRC (grants EP/K014706/2, EP/ K014668/1, EP/K014854/1, EP/K014714/1 and EP/M013219/1) as well as the EPSRC grant EP/N008995/1. We are grateful to Robert Bell for suppling the coordinates for his model of MCM 41. AJOM acknowledges the Ramsay Memorial Trust for provision of the Ramsay Fellowship. Experiments at the ISIS Pulsed Neutron and Muon Source were supported by a beamtime allocation from the Science and Technology Facilities Council (RB1610076).

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The UK Catalysis Hub
Davidson, M. (PI)
Engineering and Physical Sciences Research Council
1/06/13 → 30/11/18
Project: Research council

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title = "Probing the dynamics and structure of confined benzene in MCM-41 based catalysts",

abstract = "A combination of Molecular Dynamics (MD) simulations and Quasielastic Neutron Scattering (QENS) experiments has been used to investigate the dynamics and structure of benzene in MCM-41 based catalysts. QENS experiments of benzene as both an unconfined liquid and confined in the catalyst Pt/MCM-41 find that the mobility of benzene decreases upon confinement as shown by the decreased diffusion coefficients. Complementary MD simulations on benzene in MCM-41 show agreement with the QENS experiments when using a novel fully flexible model of MCM-41. Structural information from the MD simulations show that benzene in MCM-41 has a significantly different structure from that of the bulk liquid; with benzene molecules closer together and no prefered orientation.",

author = "Daniel Dervin and Alexander O'Malley and Marta Falkowska and Sarayute Chansai and Ian Silverwood and Christopher Hardacre and Catlow, {C. Richard A.}",

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AU - Dervin, Daniel

AU - O'Malley, Alexander

AU - Falkowska, Marta

AU - Chansai, Sarayute

AU - Silverwood, Ian

AU - Hardacre, Christopher

AU - Catlow, C. Richard A.

PY - 2020/5/11

Y1 - 2020/5/11

N2 - A combination of Molecular Dynamics (MD) simulations and Quasielastic Neutron Scattering (QENS) experiments has been used to investigate the dynamics and structure of benzene in MCM-41 based catalysts. QENS experiments of benzene as both an unconfined liquid and confined in the catalyst Pt/MCM-41 find that the mobility of benzene decreases upon confinement as shown by the decreased diffusion coefficients. Complementary MD simulations on benzene in MCM-41 show agreement with the QENS experiments when using a novel fully flexible model of MCM-41. Structural information from the MD simulations show that benzene in MCM-41 has a significantly different structure from that of the bulk liquid; with benzene molecules closer together and no prefered orientation.

AB - A combination of Molecular Dynamics (MD) simulations and Quasielastic Neutron Scattering (QENS) experiments has been used to investigate the dynamics and structure of benzene in MCM-41 based catalysts. QENS experiments of benzene as both an unconfined liquid and confined in the catalyst Pt/MCM-41 find that the mobility of benzene decreases upon confinement as shown by the decreased diffusion coefficients. Complementary MD simulations on benzene in MCM-41 show agreement with the QENS experiments when using a novel fully flexible model of MCM-41. Structural information from the MD simulations show that benzene in MCM-41 has a significantly different structure from that of the bulk liquid; with benzene molecules closer together and no prefered orientation.

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DO - 10.1039/D0CP01196G

M3 - Article

SN - 1463-9076

JO - Physical Chemistry Chemical Physics

JF - Physical Chemistry Chemical Physics

ER -

Probing the dynamics and structure of confined benzene in MCM-41 based catalysts

Abstract

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The UK Catalysis Hub

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