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Solvent inhibition in the liquid-phase catalytic oxidation of 1,4-butanediol: understanding the catalyst behaviour from NMR relaxation time measurements
Catalytic reaction studies and nuclear magnetic resonance (NMR) relaxation time measurements have been compared to study the influence of competitive adsorption of reactant and solvent on catalytic conversion. The reaction chosen is the aerobic catalytic oxidation of 1,4-butanediol in methanol over...
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| Published in: | Catalysis science & technology 2016-01, Vol.6 (21), p.7896-7901 |
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| Main Authors: | , , , , , , , |
| Format: | Article |
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| cited_by | cdi_FETCH-LOGICAL-c337t-de3158d60d8e5f3c75ada0fc03a1aaa27b186f4443fbc1874a327bd7f36309c53 |
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| container_title | Catalysis science & technology |
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| creator | D'Agostino, Carmine Feaviour, Mark R. Brett, Gemma L. Mitchell, Jonathan York, Andrew P. E. Hutchings, Graham J. Mantle, Mick D. Gladden, Lynn F. |
| description | Catalytic reaction studies and nuclear magnetic resonance (NMR) relaxation time measurements have been compared to study the influence of competitive adsorption of reactant and solvent on catalytic conversion. The reaction chosen is the aerobic catalytic oxidation of 1,4-butanediol in methanol over different supported-metal catalysts. From the NMR
T
1
/
T
2
ratio, where
T
1
is the longitudinal and
T
2
the transverse spin relaxation time, the relative affinity of reactant and solvent for different catalytic surfaces is determined. The catalysts with the lowest activity show a preferential surface affinity for the solvent compared to the reactant. Conversely, the catalyst with the highest activity shows a preferential surface affinity for the reactant compared to the solvent. Significantly, Ru/SiO
2
, which is totally inactive for the oxidation of 1,4-butanediol, exhibited a lower
T
1
/
T
2
ratio (surface affinity) for 1,4-butanediol (reactant) than for a “weakly-interacting” alkane, indicating a very poor surface affinity for the diol functionality. The results provide direct evidence of the importance of the adsorbate–adsorbent interactions on catalyst activity in liquid-phase oxidations and indicate that the competitive adsorption of the solvent plays an important role in these reactions. This work demonstrates that NMR relaxation time analysis is a powerful method for comparing adsorption of liquids in porous catalysts, providing valuable information on the affinity of different chemical species for a catalyst surface. Moreover, the results demonstrate that NMR relaxation time measurements can be used not only to guide selection of solvent for use with a specific catalyst, but also selection of the catalyst itself. The results suggest that this method may be used to predict catalyst behaviour, enabling improved design and optimisation of heterogeneous catalytic processes. |
| doi_str_mv | 10.1039/C6CY01458E |
| format | article |
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T
1
/
T
2
ratio, where
T
1
is the longitudinal and
T
2
the transverse spin relaxation time, the relative affinity of reactant and solvent for different catalytic surfaces is determined. The catalysts with the lowest activity show a preferential surface affinity for the solvent compared to the reactant. Conversely, the catalyst with the highest activity shows a preferential surface affinity for the reactant compared to the solvent. Significantly, Ru/SiO
2
, which is totally inactive for the oxidation of 1,4-butanediol, exhibited a lower
T
1
/
T
2
ratio (surface affinity) for 1,4-butanediol (reactant) than for a “weakly-interacting” alkane, indicating a very poor surface affinity for the diol functionality. The results provide direct evidence of the importance of the adsorbate–adsorbent interactions on catalyst activity in liquid-phase oxidations and indicate that the competitive adsorption of the solvent plays an important role in these reactions. This work demonstrates that NMR relaxation time analysis is a powerful method for comparing adsorption of liquids in porous catalysts, providing valuable information on the affinity of different chemical species for a catalyst surface. Moreover, the results demonstrate that NMR relaxation time measurements can be used not only to guide selection of solvent for use with a specific catalyst, but also selection of the catalyst itself. The results suggest that this method may be used to predict catalyst behaviour, enabling improved design and optimisation of heterogeneous catalytic processes.</description><identifier>ISSN: 2044-4753</identifier><identifier>EISSN: 2044-4761</identifier><identifier>DOI: 10.1039/C6CY01458E</identifier><language>eng</language><subject>Affinity ; Catalysis ; Catalysts ; Nuclear magnetic resonance ; Oxidation ; Relaxation time ; Solvents ; Surface chemistry</subject><ispartof>Catalysis science & technology, 2016-01, Vol.6 (21), p.7896-7901</ispartof><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c337t-de3158d60d8e5f3c75ada0fc03a1aaa27b186f4443fbc1874a327bd7f36309c53</citedby><cites>FETCH-LOGICAL-c337t-de3158d60d8e5f3c75ada0fc03a1aaa27b186f4443fbc1874a327bd7f36309c53</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>315,786,790,27957,27958</link.rule.ids></links><search><creatorcontrib>D'Agostino, Carmine</creatorcontrib><creatorcontrib>Feaviour, Mark R.</creatorcontrib><creatorcontrib>Brett, Gemma L.</creatorcontrib><creatorcontrib>Mitchell, Jonathan</creatorcontrib><creatorcontrib>York, Andrew P. E.</creatorcontrib><creatorcontrib>Hutchings, Graham J.</creatorcontrib><creatorcontrib>Mantle, Mick D.</creatorcontrib><creatorcontrib>Gladden, Lynn F.</creatorcontrib><title>Solvent inhibition in the liquid-phase catalytic oxidation of 1,4-butanediol: understanding the catalyst behaviour from NMR relaxation time measurements</title><title>Catalysis science & technology</title><description>Catalytic reaction studies and nuclear magnetic resonance (NMR) relaxation time measurements have been compared to study the influence of competitive adsorption of reactant and solvent on catalytic conversion. The reaction chosen is the aerobic catalytic oxidation of 1,4-butanediol in methanol over different supported-metal catalysts. From the NMR
T
1
/
T
2
ratio, where
T
1
is the longitudinal and
T
2
the transverse spin relaxation time, the relative affinity of reactant and solvent for different catalytic surfaces is determined. The catalysts with the lowest activity show a preferential surface affinity for the solvent compared to the reactant. Conversely, the catalyst with the highest activity shows a preferential surface affinity for the reactant compared to the solvent. Significantly, Ru/SiO
2
, which is totally inactive for the oxidation of 1,4-butanediol, exhibited a lower
T
1
/
T
2
ratio (surface affinity) for 1,4-butanediol (reactant) than for a “weakly-interacting” alkane, indicating a very poor surface affinity for the diol functionality. The results provide direct evidence of the importance of the adsorbate–adsorbent interactions on catalyst activity in liquid-phase oxidations and indicate that the competitive adsorption of the solvent plays an important role in these reactions. This work demonstrates that NMR relaxation time analysis is a powerful method for comparing adsorption of liquids in porous catalysts, providing valuable information on the affinity of different chemical species for a catalyst surface. Moreover, the results demonstrate that NMR relaxation time measurements can be used not only to guide selection of solvent for use with a specific catalyst, but also selection of the catalyst itself. The results suggest that this method may be used to predict catalyst behaviour, enabling improved design and optimisation of heterogeneous catalytic processes.</description><subject>Affinity</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Nuclear magnetic resonance</subject><subject>Oxidation</subject><subject>Relaxation time</subject><subject>Solvents</subject><subject>Surface chemistry</subject><issn>2044-4753</issn><issn>2044-4761</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2016</creationdate><recordtype>article</recordtype><recordid>eNpFUctOwzAQtBBIVKUXvsBHhAjYtZ2k3FDFSyog8ThwijZ-EKMkbm2nav-EzyU0CPays6vZ0awGoWNKzilhs4t5On8nlIv8eg-NpoTzhGcp3f_Dgh2iSQifpC8-oySfjtDXi6vXuo3YtpUtbbSu7SGOlca1XXVWJcsKgsYSItTbaCV2G6tgx3MG0zOelF2EVivr6kvctUr70M_Kth87leEwRFzqCtbWdR4b7xr8-PCMva5hM2hF22jcaAid103vJxyhAwN10JPfPkZvN9ev87tk8XR7P79aJJKxLCZKMypylRKVa2GYzAQoIEYSBhQApllJ89RwzpkpJc0zDqzfqcywlJGZFGyMTgbdpXerTodYNDZIXdf9T64LBc2FYDkhgvbU04EqvQvBa1MsvW3AbwtKip8Eiv8E2Df8h3vh</recordid><startdate>20160101</startdate><enddate>20160101</enddate><creator>D'Agostino, Carmine</creator><creator>Feaviour, Mark R.</creator><creator>Brett, Gemma L.</creator><creator>Mitchell, Jonathan</creator><creator>York, Andrew P. 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E.</au><au>Hutchings, Graham J.</au><au>Mantle, Mick D.</au><au>Gladden, Lynn F.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Solvent inhibition in the liquid-phase catalytic oxidation of 1,4-butanediol: understanding the catalyst behaviour from NMR relaxation time measurements</atitle><jtitle>Catalysis science & technology</jtitle><date>2016-01-01</date><risdate>2016</risdate><volume>6</volume><issue>21</issue><spage>7896</spage><epage>7901</epage><pages>7896-7901</pages><issn>2044-4753</issn><eissn>2044-4761</eissn><notes>ObjectType-Article-1</notes><notes>SourceType-Scholarly Journals-1</notes><notes>ObjectType-Feature-2</notes><notes>content type line 23</notes><abstract>Catalytic reaction studies and nuclear magnetic resonance (NMR) relaxation time measurements have been compared to study the influence of competitive adsorption of reactant and solvent on catalytic conversion. The reaction chosen is the aerobic catalytic oxidation of 1,4-butanediol in methanol over different supported-metal catalysts. From the NMR
T
1
/
T
2
ratio, where
T
1
is the longitudinal and
T
2
the transverse spin relaxation time, the relative affinity of reactant and solvent for different catalytic surfaces is determined. The catalysts with the lowest activity show a preferential surface affinity for the solvent compared to the reactant. Conversely, the catalyst with the highest activity shows a preferential surface affinity for the reactant compared to the solvent. Significantly, Ru/SiO
2
, which is totally inactive for the oxidation of 1,4-butanediol, exhibited a lower
T
1
/
T
2
ratio (surface affinity) for 1,4-butanediol (reactant) than for a “weakly-interacting” alkane, indicating a very poor surface affinity for the diol functionality. The results provide direct evidence of the importance of the adsorbate–adsorbent interactions on catalyst activity in liquid-phase oxidations and indicate that the competitive adsorption of the solvent plays an important role in these reactions. This work demonstrates that NMR relaxation time analysis is a powerful method for comparing adsorption of liquids in porous catalysts, providing valuable information on the affinity of different chemical species for a catalyst surface. Moreover, the results demonstrate that NMR relaxation time measurements can be used not only to guide selection of solvent for use with a specific catalyst, but also selection of the catalyst itself. The results suggest that this method may be used to predict catalyst behaviour, enabling improved design and optimisation of heterogeneous catalytic processes.</abstract><doi>10.1039/C6CY01458E</doi><tpages>6</tpages><oa>free_for_read</oa></addata></record> |
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| language | eng |
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| source | Royal Society of Chemistry:Jisc Collections:Royal Society of Chemistry Read and Publish 2022-2024 (reading list) |
| subjects | Affinity Catalysis Catalysts Nuclear magnetic resonance Oxidation Relaxation time Solvents Surface chemistry |
| title | Solvent inhibition in the liquid-phase catalytic oxidation of 1,4-butanediol: understanding the catalyst behaviour from NMR relaxation time measurements |
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