Aerobic oxidation of aqueous ethanol using heterogeneous gold catalysts: Efficient routes to acetic acid and ethyl acetate
The aerobic oxidation of aqueous ethanol to produce acetic acid and ethyl acetate was studied using heterogeneous gold catalysts. Comparing the performance of Au/MgAl 2O 4 and Au/TiO 2 showed that these two catalysts exhibited similar performance in the reaction. By proper selection of the reaction...
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| Veröffentlicht in: | Journal of catalysis 2007-10, Vol.251 (2), p.332-337 |
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| creator | Jørgensen, Betina Egholm Christiansen, Sofie Dahl Thomsen, Marie Louise Christensen, Claus Hviid |
| description | The aerobic oxidation of aqueous ethanol to produce acetic acid and ethyl acetate was studied using heterogeneous gold catalysts. Comparing the performance of Au/MgAl
2O
4 and Au/TiO
2 showed that these two catalysts exhibited similar performance in the reaction. By proper selection of the reaction conditions, yields of 90–95% of acetic acid could be achieved at moderate temperatures and pressures. Based on our findings, a reaction pathway for the catalytic oxidation of ethanol via acetaldehyde to acetic acid is proposed, and the rate-determining step (RDS) in the mechanism is found to be the (possibly oxygen-assisted) dehydrogenation of ethanol to produce acetaldehyde. It also is concluded that most of the CO
2 formed as a byproduct in the reaction results from the absorbed intermediate in the dehydrogenation of ethanol to produce acetaldehyde. By varying the amount of water in the reaction mixture, the possibilities for producing ethyl acetate by the aerobic oxidation of ethanol is also studied. At low ethanol concentrations, the main product is acetic acid; at concentrations
>
60
wt
%
, it is ethyl acetate. |
| doi_str_mv | 10.1016/j.jcat.2007.08.004 |
| format | Article |
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2O
4 and Au/TiO
2 showed that these two catalysts exhibited similar performance in the reaction. By proper selection of the reaction conditions, yields of 90–95% of acetic acid could be achieved at moderate temperatures and pressures. Based on our findings, a reaction pathway for the catalytic oxidation of ethanol via acetaldehyde to acetic acid is proposed, and the rate-determining step (RDS) in the mechanism is found to be the (possibly oxygen-assisted) dehydrogenation of ethanol to produce acetaldehyde. It also is concluded that most of the CO
2 formed as a byproduct in the reaction results from the absorbed intermediate in the dehydrogenation of ethanol to produce acetaldehyde. By varying the amount of water in the reaction mixture, the possibilities for producing ethyl acetate by the aerobic oxidation of ethanol is also studied. At low ethanol concentrations, the main product is acetic acid; at concentrations
>
60
wt
%
, it is ethyl acetate.</description><identifier>ISSN: 0021-9517</identifier><identifier>EISSN: 1090-2694</identifier><identifier>DOI: 10.1016/j.jcat.2007.08.004</identifier><identifier>CODEN: JCTLA5</identifier><language>eng</language><publisher>Amsterdam: Elsevier Inc</publisher><subject>Acetic acid ; Aerobic oxidation ; Bioethanol ; Catalysis ; Catalysts ; Chemistry ; Comparative studies ; Ethyl acetate ; Exact sciences and technology ; General and physical chemistry ; Gold ; Heterogeneous catalysis ; Oxidation ; Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><ispartof>Journal of catalysis, 2007-10, Vol.251 (2), p.332-337</ispartof><rights>2007 Elsevier Inc.</rights><rights>2007 INIST-CNRS</rights><rights>Copyright © 2007 Elsevier B.V. All rights reserved.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c460t-137dadc549491a251a316f2bd7b198c296b5150750b5a3e44a44284cfdcef53a3</citedby><cites>FETCH-LOGICAL-c460t-137dadc549491a251a316f2bd7b198c296b5150750b5a3e44a44284cfdcef53a3</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktohtml>$$Uhttps://www.sciencedirect.com/science/article/pii/S0021951707003156$$EHTML$$P50$$Gelsevier$$H</linktohtml><link.rule.ids>314,776,780,3537,27901,27902,65306</link.rule.ids><backlink>$$Uhttp://pascal-francis.inist.fr/vibad/index.php?action=getRecordDetail&idt=19163718$$DView record in Pascal Francis$$Hfree_for_read</backlink></links><search><creatorcontrib>Jørgensen, Betina</creatorcontrib><creatorcontrib>Egholm Christiansen, Sofie</creatorcontrib><creatorcontrib>Dahl Thomsen, Marie Louise</creatorcontrib><creatorcontrib>Christensen, Claus Hviid</creatorcontrib><title>Aerobic oxidation of aqueous ethanol using heterogeneous gold catalysts: Efficient routes to acetic acid and ethyl acetate</title><title>Journal of catalysis</title><description>The aerobic oxidation of aqueous ethanol to produce acetic acid and ethyl acetate was studied using heterogeneous gold catalysts. Comparing the performance of Au/MgAl
2O
4 and Au/TiO
2 showed that these two catalysts exhibited similar performance in the reaction. By proper selection of the reaction conditions, yields of 90–95% of acetic acid could be achieved at moderate temperatures and pressures. Based on our findings, a reaction pathway for the catalytic oxidation of ethanol via acetaldehyde to acetic acid is proposed, and the rate-determining step (RDS) in the mechanism is found to be the (possibly oxygen-assisted) dehydrogenation of ethanol to produce acetaldehyde. It also is concluded that most of the CO
2 formed as a byproduct in the reaction results from the absorbed intermediate in the dehydrogenation of ethanol to produce acetaldehyde. By varying the amount of water in the reaction mixture, the possibilities for producing ethyl acetate by the aerobic oxidation of ethanol is also studied. At low ethanol concentrations, the main product is acetic acid; at concentrations
>
60
wt
%
, it is ethyl acetate.</description><subject>Acetic acid</subject><subject>Aerobic oxidation</subject><subject>Bioethanol</subject><subject>Catalysis</subject><subject>Catalysts</subject><subject>Chemistry</subject><subject>Comparative studies</subject><subject>Ethyl acetate</subject><subject>Exact sciences and technology</subject><subject>General and physical chemistry</subject><subject>Gold</subject><subject>Heterogeneous catalysis</subject><subject>Oxidation</subject><subject>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</subject><issn>0021-9517</issn><issn>1090-2694</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2007</creationdate><recordtype>article</recordtype><recordid>eNp9kE1rFTEUhoMoeK3-AVdBcDnjOTPJfIibUqoWCm50Hc7k4zbDOKlJRrz-ejO9BXddBU6e876ch7G3CDUCdh_metaU6wagr2GoAcQzdkAYoWq6UTxnB4AGq1Fi_5K9SmkGQJRyOLC_lzaGyWse_nhD2YeVB8fp12bDlrjNd7SGhW_Jr0d-Z3OBj3Z9-DuGxfBSSssp5fSRXzvntbdr5jFs2SaeAydtc8km7Q2n1ex5p-VhStm-Zi8cLcm-eXwv2I_P19-vvla3377cXF3eVlp0kCtse0NGSzGKEamRSC12rplMP-E46GbsJokSegmTpNYKQUI0g9DOaOtkS-0Fe3fOvY-h3JWymsMW11KpcJRCSAF9gZozpGNIKVqn7qP_SfGkENSuWM1qV6x2xQoGVRSXpfePyZQ0LS7Sqn36vzli1_Y4FO7TmbPlzN_eRpV2U9oaH63OygT_VM0_vOaTVQ</recordid><startdate>20071025</startdate><enddate>20071025</enddate><creator>Jørgensen, Betina</creator><creator>Egholm Christiansen, Sofie</creator><creator>Dahl Thomsen, Marie Louise</creator><creator>Christensen, Claus Hviid</creator><general>Elsevier Inc</general><general>Elsevier</general><general>Elsevier BV</general><scope>IQODW</scope><scope>AAYXX</scope><scope>CITATION</scope></search><sort><creationdate>20071025</creationdate><title>Aerobic oxidation of aqueous ethanol using heterogeneous gold catalysts: Efficient routes to acetic acid and ethyl acetate</title><author>Jørgensen, Betina ; Egholm Christiansen, Sofie ; Dahl Thomsen, Marie Louise ; Christensen, Claus Hviid</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c460t-137dadc549491a251a316f2bd7b198c296b5150750b5a3e44a44284cfdcef53a3</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2007</creationdate><topic>Acetic acid</topic><topic>Aerobic oxidation</topic><topic>Bioethanol</topic><topic>Catalysis</topic><topic>Catalysts</topic><topic>Chemistry</topic><topic>Comparative studies</topic><topic>Ethyl acetate</topic><topic>Exact sciences and technology</topic><topic>General and physical chemistry</topic><topic>Gold</topic><topic>Heterogeneous catalysis</topic><topic>Oxidation</topic><topic>Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Jørgensen, Betina</creatorcontrib><creatorcontrib>Egholm Christiansen, Sofie</creatorcontrib><creatorcontrib>Dahl Thomsen, Marie Louise</creatorcontrib><creatorcontrib>Christensen, Claus Hviid</creatorcontrib><collection>Pascal-Francis</collection><collection>CrossRef</collection><jtitle>Journal of catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Jørgensen, Betina</au><au>Egholm Christiansen, Sofie</au><au>Dahl Thomsen, Marie Louise</au><au>Christensen, Claus Hviid</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Aerobic oxidation of aqueous ethanol using heterogeneous gold catalysts: Efficient routes to acetic acid and ethyl acetate</atitle><jtitle>Journal of catalysis</jtitle><date>2007-10-25</date><risdate>2007</risdate><volume>251</volume><issue>2</issue><spage>332</spage><epage>337</epage><pages>332-337</pages><issn>0021-9517</issn><eissn>1090-2694</eissn><coden>JCTLA5</coden><abstract>The aerobic oxidation of aqueous ethanol to produce acetic acid and ethyl acetate was studied using heterogeneous gold catalysts. Comparing the performance of Au/MgAl
2O
4 and Au/TiO
2 showed that these two catalysts exhibited similar performance in the reaction. By proper selection of the reaction conditions, yields of 90–95% of acetic acid could be achieved at moderate temperatures and pressures. Based on our findings, a reaction pathway for the catalytic oxidation of ethanol via acetaldehyde to acetic acid is proposed, and the rate-determining step (RDS) in the mechanism is found to be the (possibly oxygen-assisted) dehydrogenation of ethanol to produce acetaldehyde. It also is concluded that most of the CO
2 formed as a byproduct in the reaction results from the absorbed intermediate in the dehydrogenation of ethanol to produce acetaldehyde. By varying the amount of water in the reaction mixture, the possibilities for producing ethyl acetate by the aerobic oxidation of ethanol is also studied. At low ethanol concentrations, the main product is acetic acid; at concentrations
>
60
wt
%
, it is ethyl acetate.</abstract><cop>Amsterdam</cop><pub>Elsevier Inc</pub><doi>10.1016/j.jcat.2007.08.004</doi><tpages>6</tpages></addata></record> |
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| ispartof | Journal of catalysis, 2007-10, Vol.251 (2), p.332-337 |
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| language | eng |
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| source | Elsevier ScienceDirect Journals |
| subjects | Acetic acid Aerobic oxidation Bioethanol Catalysis Catalysts Chemistry Comparative studies Ethyl acetate Exact sciences and technology General and physical chemistry Gold Heterogeneous catalysis Oxidation Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry |
| title | Aerobic oxidation of aqueous ethanol using heterogeneous gold catalysts: Efficient routes to acetic acid and ethyl acetate |
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