Dynamics of water confined in mesopores with variable surface interaction
We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the w...
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Veröffentlicht in: | The Journal of chemical physics 2021-03, Vol.154 (9), p.094505-094505 |
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creator | Jani, Aîcha Busch, Mark Mietner, J. Benedikt Ollivier, Jacques Appel, Markus Frick, Bernhard Zanotti, Jean-Marc Ghoufi, Aziz Huber, Patrick Fröba, Michael Morineau, Denis |
description | We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5 nm–4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. This study provides a comprehensive microscopic view on the dynamics of liquid water confined in mesopores, with distinct surface chemistries, in terms of non-mobile/mobile fraction, self-diffusion coefficient, residence time, confining radius, local relaxation time, and their temperature dependence. Importantly, it demonstrates that the strength of the water/surface interaction determines the long-time tail of the dynamics, which we attributed to the translational diffusion of interfacial molecules, while the water dynamics in the pore center is barely affected by the interface hydrophilicity. |
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Benedikt ; Ollivier, Jacques ; Appel, Markus ; Frick, Bernhard ; Zanotti, Jean-Marc ; Ghoufi, Aziz ; Huber, Patrick ; Fröba, Michael ; Morineau, Denis</creator><creatorcontrib>Jani, Aîcha ; Busch, Mark ; Mietner, J. Benedikt ; Ollivier, Jacques ; Appel, Markus ; Frick, Bernhard ; Zanotti, Jean-Marc ; Ghoufi, Aziz ; Huber, Patrick ; Fröba, Michael ; Morineau, Denis</creatorcontrib><description>We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5 nm–4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. This study provides a comprehensive microscopic view on the dynamics of liquid water confined in mesopores, with distinct surface chemistries, in terms of non-mobile/mobile fraction, self-diffusion coefficient, residence time, confining radius, local relaxation time, and their temperature dependence. Importantly, it demonstrates that the strength of the water/surface interaction determines the long-time tail of the dynamics, which we attributed to the translational diffusion of interfacial molecules, while the water dynamics in the pore center is barely affected by the interface hydrophilicity.</description><identifier>ISSN: 0021-9606</identifier><identifier>EISSN: 1089-7690</identifier><identifier>DOI: 10.1063/5.0040705</identifier><identifier>PMID: 33685146</identifier><identifier>CODEN: JCPSA6</identifier><language>eng</language><publisher>United States: American Institute of Physics</publisher><subject>Backscattering ; Chemical Physics ; Chemical Sciences ; Comparative studies ; Diffusion coefficient ; Material chemistry ; Molecular dynamics ; Neutron scattering ; Neutron spectrometers ; Physics ; Pore size ; Porosity ; Relaxation time ; Self diffusion ; Silicon dioxide ; Temperature dependence ; Translational motion ; Water</subject><ispartof>The Journal of chemical physics, 2021-03, Vol.154 (9), p.094505-094505</ispartof><rights>Author(s)</rights><rights>2021 Author(s). 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Benedikt</creatorcontrib><creatorcontrib>Ollivier, Jacques</creatorcontrib><creatorcontrib>Appel, Markus</creatorcontrib><creatorcontrib>Frick, Bernhard</creatorcontrib><creatorcontrib>Zanotti, Jean-Marc</creatorcontrib><creatorcontrib>Ghoufi, Aziz</creatorcontrib><creatorcontrib>Huber, Patrick</creatorcontrib><creatorcontrib>Fröba, Michael</creatorcontrib><creatorcontrib>Morineau, Denis</creatorcontrib><title>Dynamics of water confined in mesopores with variable surface interaction</title><title>The Journal of chemical physics</title><addtitle>J Chem Phys</addtitle><description>We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5 nm–4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. 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Benedikt</au><au>Ollivier, Jacques</au><au>Appel, Markus</au><au>Frick, Bernhard</au><au>Zanotti, Jean-Marc</au><au>Ghoufi, Aziz</au><au>Huber, Patrick</au><au>Fröba, Michael</au><au>Morineau, Denis</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Dynamics of water confined in mesopores with variable surface interaction</atitle><jtitle>The Journal of chemical physics</jtitle><addtitle>J Chem Phys</addtitle><date>2021-03-07</date><risdate>2021</risdate><volume>154</volume><issue>9</issue><spage>094505</spage><epage>094505</epage><pages>094505-094505</pages><issn>0021-9606</issn><eissn>1089-7690</eissn><coden>JCPSA6</coden><abstract>We have investigated the dynamics of liquid water confined in mesostructured porous silica (MCM-41) and periodic mesoporous organosilicas (PMOs) by incoherent quasielastic neutron scattering experiments. The effect of tuning the water/surface interaction from hydrophilic to more hydrophobic on the water mobility, while keeping the pore size in the range 3.5 nm–4.1 nm, was assessed from the comparative study of three PMOs comprising different organic bridging units and the purely siliceous MCM-41 case. An extended dynamical range was achieved by combining time-of-flight (IN5B) and backscattering (IN16B) quasielastic neutron spectrometers providing complementary energy resolutions. Liquid water was studied at regularly spaced temperatures ranging from 300 K to 243 K. In all systems, the molecular dynamics could be described consistently by the combination of two independent motions resulting from fast local motion around the average molecule position and the confined translational jump diffusion of its center of mass. All the molecules performed local relaxations, whereas the translational motion of a fraction of molecules was frozen on the experimental timescale. This study provides a comprehensive microscopic view on the dynamics of liquid water confined in mesopores, with distinct surface chemistries, in terms of non-mobile/mobile fraction, self-diffusion coefficient, residence time, confining radius, local relaxation time, and their temperature dependence. Importantly, it demonstrates that the strength of the water/surface interaction determines the long-time tail of the dynamics, which we attributed to the translational diffusion of interfacial molecules, while the water dynamics in the pore center is barely affected by the interface hydrophilicity.</abstract><cop>United States</cop><pub>American Institute of Physics</pub><pmid>33685146</pmid><doi>10.1063/5.0040705</doi><tpages>13</tpages><orcidid>https://orcid.org/0000-0003-0877-7968</orcidid><orcidid>https://orcid.org/0000-0002-2126-9100</orcidid><orcidid>https://orcid.org/0000-0001-8570-4549</orcidid><orcidid>https://orcid.org/0000-0001-6474-3944</orcidid><orcidid>https://orcid.org/0000-0001-5954-1774</orcidid><orcidid>https://orcid.org/0000-0002-9064-4314</orcidid><orcidid>https://orcid.org/0000-0002-3378-6674</orcidid><orcidid>https://orcid.org/0000-0001-6927-0509</orcidid><orcidid>https://orcid.org/0000-0001-6069-7573</orcidid><orcidid>https://orcid.org/0000-0003-2806-8130</orcidid><orcidid>https://orcid.org/0000-0002-8784-3021</orcidid><orcidid>https://orcid.org/0000000160697573</orcidid><orcidid>https://orcid.org/0000000287843021</orcidid><orcidid>https://orcid.org/0000000233786674</orcidid><orcidid>https://orcid.org/0000000221269100</orcidid><orcidid>https://orcid.org/0000000328068130</orcidid><orcidid>https://orcid.org/0000000169270509</orcidid><orcidid>https://orcid.org/0000000308777968</orcidid><orcidid>https://orcid.org/0000000290644314</orcidid><orcidid>https://orcid.org/0000000159541774</orcidid><orcidid>https://orcid.org/0000000185704549</orcidid><orcidid>https://orcid.org/0000000164743944</orcidid><oa>free_for_read</oa></addata></record> |
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subjects | Backscattering Chemical Physics Chemical Sciences Comparative studies Diffusion coefficient Material chemistry Molecular dynamics Neutron scattering Neutron spectrometers Physics Pore size Porosity Relaxation time Self diffusion Silicon dioxide Temperature dependence Translational motion Water |
title | Dynamics of water confined in mesopores with variable surface interaction |
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