NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2
The synthesis and characterization of the first catalytic manganese N‐heterocyclic carbene complexes are reported: MnBr(N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine)(CO)3 and MnBr(N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two‐electron...
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| Veröffentlicht in: | Angewandte Chemie International Edition 2014-05, Vol.53 (20), p.5152-5155 |
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| creator | Agarwal, Jay Shaw, Travis W. Stanton III, Charles J. Majetich, George F. Bocarsly, Andrew B. Schaefer III, Henry F. |
| description | The synthesis and characterization of the first catalytic manganese N‐heterocyclic carbene complexes are reported: MnBr(N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine)(CO)3 and MnBr(N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center, as observed with preparative scale electrolysis and verified with 13CO2. The two‐electron reduction of these species occurs at a single potential, rather than in two sequential steps separated by hundreds of millivolts, as is the case for previously reported MnBr(2,2′‐bipyridine)(CO)3. Catalytic current enhancement is observed at voltages similar to MnBr(2,2′‐bipyridine)(CO)3.
Catalytic manganese N‐heterocyclic carbene complexes have been synthesized and characterized: [MnBrL(CO)3] (see scheme; L=N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine or N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine). Both species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center at a single potential, as observed with preparative scale electrolysis and verified with 13CO2. |
| doi_str_mv | 10.1002/anie.201311099 |
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Catalytic manganese N‐heterocyclic carbene complexes have been synthesized and characterized: [MnBrL(CO)3] (see scheme; L=N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine or N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine). Both species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center at a single potential, as observed with preparative scale electrolysis and verified with 13CO2.</description><edition>International ed. in English</edition><identifier>ISSN: 1433-7851</identifier><identifier>EISSN: 1521-3773</identifier><identifier>DOI: 10.1002/anie.201311099</identifier><identifier>PMID: 24700649</identifier><identifier>CODEN: ACIEAY</identifier><language>eng</language><publisher>Weinheim: WILEY-VCH Verlag</publisher><subject>Carbon dioxide ; Carbon monoxide ; catalysis ; Chemical reduction ; Chemical synthesis ; Electrocatalysts ; electrochemistry ; Electrolysis ; Electrons ; Manganese ; N-heterocyclic carbenes ; New species</subject><ispartof>Angewandte Chemie International Edition, 2014-05, Vol.53 (20), p.5152-5155</ispartof><rights>2014 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.</rights><rights>2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim</rights><rights>Copyright Wiley Subscription Services, Inc. May 2014</rights><lds50>peer_reviewed</lds50><woscitedreferencessubscribed>false</woscitedreferencessubscribed></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fanie.201311099$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fanie.201311099$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>314,780,784,1417,27924,27925,45574,45575</link.rule.ids><backlink>$$Uhttps://www.ncbi.nlm.nih.gov/pubmed/24700649$$D View this record in MEDLINE/PubMed$$Hfree_for_read</backlink></links><search><creatorcontrib>Agarwal, Jay</creatorcontrib><creatorcontrib>Shaw, Travis W.</creatorcontrib><creatorcontrib>Stanton III, Charles J.</creatorcontrib><creatorcontrib>Majetich, George F.</creatorcontrib><creatorcontrib>Bocarsly, Andrew B.</creatorcontrib><creatorcontrib>Schaefer III, Henry F.</creatorcontrib><title>NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2</title><title>Angewandte Chemie International Edition</title><addtitle>Angew. Chem. Int. Ed</addtitle><description>The synthesis and characterization of the first catalytic manganese N‐heterocyclic carbene complexes are reported: MnBr(N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine)(CO)3 and MnBr(N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center, as observed with preparative scale electrolysis and verified with 13CO2. The two‐electron reduction of these species occurs at a single potential, rather than in two sequential steps separated by hundreds of millivolts, as is the case for previously reported MnBr(2,2′‐bipyridine)(CO)3. Catalytic current enhancement is observed at voltages similar to MnBr(2,2′‐bipyridine)(CO)3.
Catalytic manganese N‐heterocyclic carbene complexes have been synthesized and characterized: [MnBrL(CO)3] (see scheme; L=N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine or N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine). Both species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center at a single potential, as observed with preparative scale electrolysis and verified with 13CO2.</description><subject>Carbon dioxide</subject><subject>Carbon monoxide</subject><subject>catalysis</subject><subject>Chemical reduction</subject><subject>Chemical synthesis</subject><subject>Electrocatalysts</subject><subject>electrochemistry</subject><subject>Electrolysis</subject><subject>Electrons</subject><subject>Manganese</subject><subject>N-heterocyclic carbenes</subject><subject>New species</subject><issn>1433-7851</issn><issn>1521-3773</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2014</creationdate><recordtype>article</recordtype><recordid>eNp9kTtPwzAUhS0EgvJYGVEkFhgCfsbxiKJCK0ErShESi-W4NyWQJiVOBP33OGrpwMDka93vXB2dg9ApwVcEY3ptyhyuKCaMEKzUDuoRQUnIpGS7fuaMhTIW5AAdOvfu-TjG0T46oFxiHHHVQ5PRIAmTqmxMXublPHgw5dyU4OBieBn0C7BNXVnTmGLlGhdkVR00bxBMv6pwsyyDCcxa2-R-qrIgGdNjtJeZwsHJ5j1Cz7f9aTII78d3w-TmPpxzEaswiyxOMwKZJYJBlIFIMUkVMMqV5CmF1EY8Sq3MpLFsZlJD4pgDcCDAuFXsCF2s7y7r6rMF1-hF7iwUhfdftU77JBjHVFLi0fM_6HvV1qV3p6mIsPCHVfwf1aUae1uio842VJsuYKaXdb4w9Ur_ZuoBtQa-8gJW2z3BumtMd43pbWP6ZjTsb39eG661uWvge6s19YeOJJNCv4zu9PTpdTCZPI40YT8rDZcI</recordid><startdate>20140512</startdate><enddate>20140512</enddate><creator>Agarwal, Jay</creator><creator>Shaw, Travis W.</creator><creator>Stanton III, Charles J.</creator><creator>Majetich, George F.</creator><creator>Bocarsly, Andrew B.</creator><creator>Schaefer III, Henry F.</creator><general>WILEY-VCH Verlag</general><general>WILEY‐VCH Verlag</general><general>Wiley Subscription Services, Inc</general><scope>BSCLL</scope><scope>NPM</scope><scope>7TM</scope><scope>K9.</scope><scope>7X8</scope></search><sort><creationdate>20140512</creationdate><title>NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2</title><author>Agarwal, Jay ; Shaw, Travis W. ; Stanton III, Charles J. ; Majetich, George F. ; Bocarsly, Andrew B. ; Schaefer III, Henry F.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-g4589-f6c0bf1efc153e6fe5b01b9e324974b2ebc646bc7f7ac3daba1884ee4e1e34c93</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2014</creationdate><topic>Carbon dioxide</topic><topic>Carbon monoxide</topic><topic>catalysis</topic><topic>Chemical reduction</topic><topic>Chemical synthesis</topic><topic>Electrocatalysts</topic><topic>electrochemistry</topic><topic>Electrolysis</topic><topic>Electrons</topic><topic>Manganese</topic><topic>N-heterocyclic carbenes</topic><topic>New species</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Agarwal, Jay</creatorcontrib><creatorcontrib>Shaw, Travis W.</creatorcontrib><creatorcontrib>Stanton III, Charles J.</creatorcontrib><creatorcontrib>Majetich, George F.</creatorcontrib><creatorcontrib>Bocarsly, Andrew B.</creatorcontrib><creatorcontrib>Schaefer III, Henry F.</creatorcontrib><collection>Istex</collection><collection>PubMed</collection><collection>Nucleic Acids Abstracts</collection><collection>ProQuest Health & Medical Complete (Alumni)</collection><collection>MEDLINE - Academic</collection><jtitle>Angewandte Chemie International Edition</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Agarwal, Jay</au><au>Shaw, Travis W.</au><au>Stanton III, Charles J.</au><au>Majetich, George F.</au><au>Bocarsly, Andrew B.</au><au>Schaefer III, Henry F.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2</atitle><jtitle>Angewandte Chemie International Edition</jtitle><addtitle>Angew. Chem. Int. Ed</addtitle><date>2014-05-12</date><risdate>2014</risdate><volume>53</volume><issue>20</issue><spage>5152</spage><epage>5155</epage><pages>5152-5155</pages><issn>1433-7851</issn><eissn>1521-3773</eissn><coden>ACIEAY</coden><abstract>The synthesis and characterization of the first catalytic manganese N‐heterocyclic carbene complexes are reported: MnBr(N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine)(CO)3 and MnBr(N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine)(CO)3. Both new species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center, as observed with preparative scale electrolysis and verified with 13CO2. The two‐electron reduction of these species occurs at a single potential, rather than in two sequential steps separated by hundreds of millivolts, as is the case for previously reported MnBr(2,2′‐bipyridine)(CO)3. Catalytic current enhancement is observed at voltages similar to MnBr(2,2′‐bipyridine)(CO)3.
Catalytic manganese N‐heterocyclic carbene complexes have been synthesized and characterized: [MnBrL(CO)3] (see scheme; L=N‐methyl‐N′‐2‐pyridylbenzimidazol‐2‐ylidine or N‐methyl‐N′‐2‐pyridylimidazol‐2‐ylidine). Both species mediate the reduction of CO2 to CO following two‐electron reduction of the MnI center at a single potential, as observed with preparative scale electrolysis and verified with 13CO2.</abstract><cop>Weinheim</cop><pub>WILEY-VCH Verlag</pub><pmid>24700649</pmid><doi>10.1002/anie.201311099</doi><tpages>4</tpages><edition>International ed. in English</edition></addata></record> |
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| subjects | Carbon dioxide Carbon monoxide catalysis Chemical reduction Chemical synthesis Electrocatalysts electrochemistry Electrolysis Electrons Manganese N-heterocyclic carbenes New species |
| title | NHC-Containing Manganese(I) Electrocatalysts for the Two-Electron Reduction of CO2 |
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