Electrocatalytic Reduction of CO 2 to Acetic Acid by a Molecular Manganese Corrole Complex
The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthe...
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Veröffentlicht in: | Angewandte Chemie International Edition 2020-06, Vol.59 (26), p.10527-10534 |
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creator | De, Ratnadip Gonglach, Sabrina Paul, Shounik Haas, Michael Sreejith, S S Gerschel, Philipp Apfel, Ulf-Peter Vuong, Thanh Huyen Rabeah, Jabor Roy, Soumyajit Schöfberger, Wolfgang |
description | The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular Mn
-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO
. Electrochemical reduction of Mn
leads to an electroactive Mn
species, which binds CO
and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO
to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h
, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the Mn
-corrole center. |
doi_str_mv | 10.1002/anie.202000601 |
format | Article |
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-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO
. Electrochemical reduction of Mn
leads to an electroactive Mn
species, which binds CO
and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO
to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h
, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the Mn
-corrole center.</description><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.202000601</identifier><identifier>PMID: 32281187</identifier><language>eng</language><publisher>Germany</publisher><ispartof>Angewandte Chemie International Edition, 2020-06, Vol.59 (26), p.10527-10534</ispartof><rights>2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c1077-7d131e7b36a7ca3d62a99d408d105b8de74945e3d99066c66562fed95782c2813</citedby><cites>FETCH-LOGICAL-c1077-7d131e7b36a7ca3d62a99d408d105b8de74945e3d99066c66562fed95782c2813</cites><orcidid>0000-0002-8055-8906</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><link.rule.ids>314,776,780,27901,27902</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/32281187$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>De, Ratnadip</creatorcontrib><creatorcontrib>Gonglach, Sabrina</creatorcontrib><creatorcontrib>Paul, Shounik</creatorcontrib><creatorcontrib>Haas, Michael</creatorcontrib><creatorcontrib>Sreejith, S S</creatorcontrib><creatorcontrib>Gerschel, Philipp</creatorcontrib><creatorcontrib>Apfel, Ulf-Peter</creatorcontrib><creatorcontrib>Vuong, Thanh Huyen</creatorcontrib><creatorcontrib>Rabeah, Jabor</creatorcontrib><creatorcontrib>Roy, Soumyajit</creatorcontrib><creatorcontrib>Schöfberger, Wolfgang</creatorcontrib><title>Electrocatalytic Reduction of CO 2 to Acetic Acid by a Molecular Manganese Corrole Complex</title><title>Angewandte Chemie International Edition</title><addtitle>Angew Chem Int Ed Engl</addtitle><description>The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular Mn
-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO
. Electrochemical reduction of Mn
leads to an electroactive Mn
species, which binds CO
and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO
to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h
, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the Mn
-corrole center.</description><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2020</creationdate><recordtype>article</recordtype><recordid>eNo9kF9LwzAUxYMobk5ffZR8gdabpE3Sx1HmH9gYiL74UtLkVipdM9IO3Lc3Zbqnc7n3nAvnR8g9g5QB8EfTt5hy4AAggV2QOcs5S4RS4jLOmRCJ0jmbkZth-I5-rUFek5ngXDOm1Zx8rjq0Y_DWjKY7jq2lb-gOdmx9T31Dyy3ldPR0aXG6LW3raH2khm58zB06E-jG9F-mxwFp6UOI66i7fYc_t-SqMd2Ad3-6IB9Pq_fyJVlvn1_L5TqxDJRKlGOCoaqFNMoa4SQ3ReEy0I5BXmuHKiuyHIUrCpDSSplL3qArcqW5jTXEgqSnvzb4YQjYVPvQ7kw4VgyqCVI1QarOkGLg4RTYH-odurP9n4r4Bf-5YTc</recordid><startdate>20200622</startdate><enddate>20200622</enddate><creator>De, Ratnadip</creator><creator>Gonglach, Sabrina</creator><creator>Paul, Shounik</creator><creator>Haas, Michael</creator><creator>Sreejith, S S</creator><creator>Gerschel, Philipp</creator><creator>Apfel, Ulf-Peter</creator><creator>Vuong, Thanh Huyen</creator><creator>Rabeah, Jabor</creator><creator>Roy, Soumyajit</creator><creator>Schöfberger, Wolfgang</creator><scope>NPM</scope><scope>AAYXX</scope><scope>CITATION</scope><orcidid>https://orcid.org/0000-0002-8055-8906</orcidid></search><sort><creationdate>20200622</creationdate><title>Electrocatalytic Reduction of CO 2 to Acetic Acid by a Molecular Manganese Corrole Complex</title><author>De, Ratnadip ; Gonglach, Sabrina ; Paul, Shounik ; Haas, Michael ; Sreejith, S S ; Gerschel, Philipp ; Apfel, Ulf-Peter ; Vuong, Thanh Huyen ; Rabeah, Jabor ; Roy, Soumyajit ; Schöfberger, Wolfgang</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c1077-7d131e7b36a7ca3d62a99d408d105b8de74945e3d99066c66562fed95782c2813</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2020</creationdate><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>De, Ratnadip</creatorcontrib><creatorcontrib>Gonglach, Sabrina</creatorcontrib><creatorcontrib>Paul, Shounik</creatorcontrib><creatorcontrib>Haas, Michael</creatorcontrib><creatorcontrib>Sreejith, S S</creatorcontrib><creatorcontrib>Gerschel, Philipp</creatorcontrib><creatorcontrib>Apfel, Ulf-Peter</creatorcontrib><creatorcontrib>Vuong, Thanh Huyen</creatorcontrib><creatorcontrib>Rabeah, Jabor</creatorcontrib><creatorcontrib>Roy, Soumyajit</creatorcontrib><creatorcontrib>Schöfberger, Wolfgang</creatorcontrib><collection>PubMed</collection><collection>CrossRef</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>De, Ratnadip</au><au>Gonglach, Sabrina</au><au>Paul, Shounik</au><au>Haas, Michael</au><au>Sreejith, S S</au><au>Gerschel, Philipp</au><au>Apfel, Ulf-Peter</au><au>Vuong, Thanh Huyen</au><au>Rabeah, Jabor</au><au>Roy, Soumyajit</au><au>Schöfberger, Wolfgang</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Electrocatalytic Reduction of CO 2 to Acetic Acid by a Molecular Manganese Corrole Complex</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew Chem Int Ed Engl</addtitle><date>2020-06-22</date><risdate>2020</risdate><volume>59</volume><issue>26</issue><spage>10527</spage><epage>10534</epage><pages>10527-10534</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><abstract>The controlled electrochemical reduction of carbon dioxide to value added chemicals is an important strategy in terms of renewable energy technologies. Therefore, the development of efficient and stable catalysts in an aqueous environment is of great importance. In this context, we focused on synthesizing and studying a molecular Mn
-corrole complex, which is modified on the three meso-positions with polyethylene glycol moieties for direct and selective production of acetic acid from CO
. Electrochemical reduction of Mn
leads to an electroactive Mn
species, which binds CO
and stabilizes the reduced intermediates. This catalyst allows to electrochemically reduce CO
to acetic acid in a moderate acidic aqueous medium (pH 6) with a selectivity of 63 % and a turn over frequency (TOF) of 8.25 h
, when immobilized on a carbon paper (CP) electrode. In terms of high selectivity towards acetate, we propose the formation and reduction of an oxalate type intermediate, stabilized at the Mn
-corrole center.</abstract><cop>Germany</cop><pmid>32281187</pmid><doi>10.1002/anie.202000601</doi><tpages>8</tpages><orcidid>https://orcid.org/0000-0002-8055-8906</orcidid></addata></record> |
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source | Wiley Online Library Journals Frontfile Complete |
title | Electrocatalytic Reduction of CO 2 to Acetic Acid by a Molecular Manganese Corrole Complex |
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