Direct and quantitative monitoring of catalytic organic reactions under heterogeneous conditions using direct analysis in real time mass spectrometry
This new method overcomes problems of conventional analytical methodologies such as light scattering and sampling reproducibility issues. We used this method for mechanistic studies of catalytic reactions under heterogeneous conditions. Direct-type hydroxymethylation reactions and Mukaiyama-type hyd...
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| Veröffentlicht in: | Chemical science (Cambridge) 2020-05, Vol.11 (19), p.515-5112 |
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| creator | Masuda, Koichiro Kobayashi, Sh |
| description | This new method overcomes problems of conventional analytical methodologies such as light scattering and sampling reproducibility issues. We used this method for mechanistic studies of catalytic reactions under heterogeneous conditions. Direct-type hydroxymethylation reactions and Mukaiyama-type hydroxymethylation reactions both catalyzed by a scandium-bipyridine ligand complex under micellar conditions were employed as examples of heterogeneous reactions. For direct-type hydroxymethylation reactions, initial reaction rate assays revealed first-order dependency on both substrate and catalyst. On the other hand, Mukaiyama-type hydroxymethylation reactions showed first-order rate dependency on substrate, zero-order on catalyst and saturation kinetics on formaldehyde.
A direct and quantitative method for monitoring heterogeneous organic reactions has been developed by using direct analysis in real time mass spectrometry (DART-MS) with an isotope-labeled reaction product as an internal standard. |
| doi_str_mv | 10.1039/d0sc00021c |
| format | Article |
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A direct and quantitative method for monitoring heterogeneous organic reactions has been developed by using direct analysis in real time mass spectrometry (DART-MS) with an isotope-labeled reaction product as an internal standard.</description><subject>Catalysts</subject><subject>Chemical reactions</subject><subject>Chemistry</subject><subject>Coordination compounds</subject><subject>Dependence</subject><subject>Light scattering</subject><subject>Mass spectrometry</subject><subject>Reaction kinetics</subject><subject>Scandium</subject><subject>Substrates</subject><subject>Technical information</subject><issn>2041-6520</issn><issn>2041-6539</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNp9ks9rFDEUx4MottRevAsRL1JYTTKT2clFKFurQsGDeg758WabMpNs8zKF_UP8f8121xU9eHqB74fPS94LIS85e8dZo957ho4xJrh7Qk4Fa_mik416ejwLdkLOEe8qw5qGS7F8Tk6alguhuv6U_LwKGVyhJnp6P5tYQjElPACdUgwl5RDXNA3UmWLGbQmOprw2sdYMxpWQItI5esj0FgrktIYIaUbqUvThEOPO4X-3qRoMSEPcGUZawlR7GUSKmwrkNEHJ2xfk2WBGhPNDPSM_rj9-X31e3Hz99GV1ebNwrVqWhfCDkNB2Xjpr-14Iy3ppFRhrwHaDGZwSfX0zODswVyFvwStoOtFYbv3QnJEPe-9mthN4B7FkM-pNDpPJW51M0H8nMdzqdXrQPZdKcFkFbw-CnO5nwKKngA7G0TzOQQvZsqVgy1ZV9M0_6F2ac51HpVrWdrJjUlTqYk-5nBAzDMfLcKZ3C9dX7NvqceGrCr_awxndkfvzIWr--n-53tQR_ALhDLfe</recordid><startdate>20200521</startdate><enddate>20200521</enddate><creator>Masuda, Koichiro</creator><creator>Kobayashi, Sh</creator><general>Royal Society of Chemistry</general><general>The Royal Society of Chemistry</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>7X8</scope><scope>5PM</scope><orcidid>https://orcid.org/0000-0002-9926-7308</orcidid><orcidid>https://orcid.org/0000-0002-8235-4368</orcidid></search><sort><creationdate>20200521</creationdate><title>Direct and quantitative monitoring of catalytic organic reactions under heterogeneous conditions using direct analysis in real time mass spectrometry</title><author>Masuda, Koichiro ; Kobayashi, Sh</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c497t-2df25e46d5cbb8822b085b9eabaeb6fafc928315ecbf0c5cbdbed9e3623b1bdf3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><topic>Catalysts</topic><topic>Chemical reactions</topic><topic>Chemistry</topic><topic>Coordination compounds</topic><topic>Dependence</topic><topic>Light scattering</topic><topic>Mass spectrometry</topic><topic>Reaction kinetics</topic><topic>Scandium</topic><topic>Substrates</topic><topic>Technical information</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Masuda, Koichiro</creatorcontrib><creatorcontrib>Kobayashi, Sh</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>MEDLINE - Academic</collection><collection>PubMed Central (Full Participant titles)</collection><jtitle>Chemical science (Cambridge)</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Masuda, Koichiro</au><au>Kobayashi, Sh</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Direct and quantitative monitoring of catalytic organic reactions under heterogeneous conditions using direct analysis in real time mass spectrometry</atitle><jtitle>Chemical science (Cambridge)</jtitle><date>2020-05-21</date><risdate>2020</risdate><volume>11</volume><issue>19</issue><spage>515</spage><epage>5112</epage><pages>515-5112</pages><issn>2041-6520</issn><eissn>2041-6539</eissn><abstract>This new method overcomes problems of conventional analytical methodologies such as light scattering and sampling reproducibility issues. We used this method for mechanistic studies of catalytic reactions under heterogeneous conditions. Direct-type hydroxymethylation reactions and Mukaiyama-type hydroxymethylation reactions both catalyzed by a scandium-bipyridine ligand complex under micellar conditions were employed as examples of heterogeneous reactions. For direct-type hydroxymethylation reactions, initial reaction rate assays revealed first-order dependency on both substrate and catalyst. On the other hand, Mukaiyama-type hydroxymethylation reactions showed first-order rate dependency on substrate, zero-order on catalyst and saturation kinetics on formaldehyde.
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| source | DOAJ Directory of Open Access Journals; Elektronische Zeitschriftenbibliothek - Frei zugängliche E-Journals; PubMed Central Open Access; PubMed Central |
| subjects | Catalysts Chemical reactions Chemistry Coordination compounds Dependence Light scattering Mass spectrometry Reaction kinetics Scandium Substrates Technical information |
| title | Direct and quantitative monitoring of catalytic organic reactions under heterogeneous conditions using direct analysis in real time mass spectrometry |
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