Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts
Iron cations are essential for the high activity of nickel and cobalt‐based (oxy)hydroxides for the oxygen evolution reaction, but the role of iron in the catalytic mechanism remains under active investigation. Operando X‐ray absorption spectroscopy and density functional theory calculations are use...
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| Veröffentlicht in: | Angewandte Chemie 2018-09, Vol.130 (39), p.13022-13026 |
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| creator | Enman, Lisa J. Stevens, Michaela Burke Dahan, Meir Haim Nellist, Michael R. Toroker, Maytal Caspary Boettcher, Shannon W. |
| description | Iron cations are essential for the high activity of nickel and cobalt‐based (oxy)hydroxides for the oxygen evolution reaction, but the role of iron in the catalytic mechanism remains under active investigation. Operando X‐ray absorption spectroscopy and density functional theory calculations are used to demonstrate partial Fe oxidation and a shortening of the Fe−O bond length during oxygen evolution on Co(Fe)OxHy. Cobalt oxidation during oxygen evolution is only observed in the absence of iron. These results demonstrate a different mechanism for water oxidation in the presence and absence of iron and support the hypothesis that oxidized iron species are involved in water‐oxidation catalysis on Co(Fe)OxHy.
Fe‐haltige Co‐ und Ni‐(Oxy)Hydroxide katalysieren die schnellste bekannte Wasseroxidation unter alkalischen Bedingungen, der Wirkmechanismus von Fe wird allerdings noch untersucht. Hier wird gezeigt, dass die Sauerstoffentwicklung mit einer Oxidation der Fe‐Kationen und einer Verkürzung der Fe‐O‐Bindungen einhergeht. Übereinstimmend mit DFT‐Rechnungen weisen diese Resultate auf Fe‐basierte aktive Zentren hin. |
| doi_str_mv | 10.1002/ange.201808818 |
| format | Article |
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Fe‐haltige Co‐ und Ni‐(Oxy)Hydroxide katalysieren die schnellste bekannte Wasseroxidation unter alkalischen Bedingungen, der Wirkmechanismus von Fe wird allerdings noch untersucht. Hier wird gezeigt, dass die Sauerstoffentwicklung mit einer Oxidation der Fe‐Kationen und einer Verkürzung der Fe‐O‐Bindungen einhergeht. Übereinstimmend mit DFT‐Rechnungen weisen diese Resultate auf Fe‐basierte aktive Zentren hin.</description><identifier>ISSN: 0044-8249</identifier><identifier>EISSN: 1521-3757</identifier><identifier>DOI: 10.1002/ange.201808818</identifier><language>eng</language><publisher>Weinheim: Wiley Subscription Services, Inc</publisher><subject>Absorption spectroscopy ; Catalysis ; Cations ; Chemistry ; Cobalt ; Density functional theory ; Electrocatalysts ; Elektrokatalysatoren ; Evolution ; Heterogene Katalyse ; Hydroxides ; Iron ; Nickel ; Oxidation ; Oxygen ; Oxygen evolution reactions ; Röntgen-Absorptionsspektroskopie ; Sauerstoffentwicklung ; Spectroscopy ; Spectrum analysis ; Wasserelektrolyse</subject><ispartof>Angewandte Chemie, 2018-09, Vol.130 (39), p.13022-13026</ispartof><rights>2018 Wiley‐VCH Verlag GmbH & Co. KGaA, Weinheim</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-c2298-4f209614f442ccd54d32abb775de511bb80f51f2a60771b80482cd2bd6ddc1c93</citedby><cites>FETCH-LOGICAL-c2298-4f209614f442ccd54d32abb775de511bb80f51f2a60771b80482cd2bd6ddc1c93</cites><orcidid>0000-0001-8971-9123 ; 0000-0003-1449-2977 ; 0000000314492977 ; 0000000189719123</orcidid></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://onlinelibrary.wiley.com/doi/pdf/10.1002%2Fange.201808818$$EPDF$$P50$$Gwiley$$H</linktopdf><linktohtml>$$Uhttps://onlinelibrary.wiley.com/doi/full/10.1002%2Fange.201808818$$EHTML$$P50$$Gwiley$$H</linktohtml><link.rule.ids>230,314,776,780,881,1411,27901,27902,45550,45551</link.rule.ids><backlink>$$Uhttps://www.osti.gov/biblio/1468491$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Enman, Lisa J.</creatorcontrib><creatorcontrib>Stevens, Michaela Burke</creatorcontrib><creatorcontrib>Dahan, Meir Haim</creatorcontrib><creatorcontrib>Nellist, Michael R.</creatorcontrib><creatorcontrib>Toroker, Maytal Caspary</creatorcontrib><creatorcontrib>Boettcher, Shannon W.</creatorcontrib><title>Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts</title><title>Angewandte Chemie</title><description>Iron cations are essential for the high activity of nickel and cobalt‐based (oxy)hydroxides for the oxygen evolution reaction, but the role of iron in the catalytic mechanism remains under active investigation. Operando X‐ray absorption spectroscopy and density functional theory calculations are used to demonstrate partial Fe oxidation and a shortening of the Fe−O bond length during oxygen evolution on Co(Fe)OxHy. Cobalt oxidation during oxygen evolution is only observed in the absence of iron. These results demonstrate a different mechanism for water oxidation in the presence and absence of iron and support the hypothesis that oxidized iron species are involved in water‐oxidation catalysis on Co(Fe)OxHy.
Fe‐haltige Co‐ und Ni‐(Oxy)Hydroxide katalysieren die schnellste bekannte Wasseroxidation unter alkalischen Bedingungen, der Wirkmechanismus von Fe wird allerdings noch untersucht. Hier wird gezeigt, dass die Sauerstoffentwicklung mit einer Oxidation der Fe‐Kationen und einer Verkürzung der Fe‐O‐Bindungen einhergeht. Übereinstimmend mit DFT‐Rechnungen weisen diese Resultate auf Fe‐basierte aktive Zentren hin.</description><subject>Absorption spectroscopy</subject><subject>Catalysis</subject><subject>Cations</subject><subject>Chemistry</subject><subject>Cobalt</subject><subject>Density functional theory</subject><subject>Electrocatalysts</subject><subject>Elektrokatalysatoren</subject><subject>Evolution</subject><subject>Heterogene Katalyse</subject><subject>Hydroxides</subject><subject>Iron</subject><subject>Nickel</subject><subject>Oxidation</subject><subject>Oxygen</subject><subject>Oxygen evolution reactions</subject><subject>Röntgen-Absorptionsspektroskopie</subject><subject>Sauerstoffentwicklung</subject><subject>Spectroscopy</subject><subject>Spectrum analysis</subject><subject>Wasserelektrolyse</subject><issn>0044-8249</issn><issn>1521-3757</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2018</creationdate><recordtype>article</recordtype><recordid>eNqFkc1OAyEUhYnRxPqzdU10o4upQJkZZtk0tTYxNvEncUcYYOyYEUag1tn5CEbf0CcRW6NLN9zA_c7h5h4ADjDqY4TIqTD3uk8QZogxzDZAD6cEJ4M8zTdBDyFKE0ZosQ12vH9ACGUkL3rgfdZqJ4yy8O7z9e1KdHBYeuvaUFsDr1stg7Ne2raD13O79HDq4vvspVZiRUw9HFkjF85pE-CyDvPY7O61geNn2yxWTG0iU4omfL5-rOTHETmZd8rZ6KPhuFn9IkUQTeeD3wNblWi83v-pu-D2bHwzOk8uZpPpaHiRSEIKltCKoCLDtKKUSKlSqgZElGWep0qnGJclQ1WKKyIylOc43igjUpFSZUpJLIvBLjhc-1ofau5lHbScS2tMHIdjmjFa4AgdraHW2aeF9oE_2IUzcS5OcFw0QvGMVH9Nybgt73TFW1c_CtdxjPh3OPw7HP4bThQUa8GybnT3D82Hl5Pxn_YLREaXtA</recordid><startdate>20180924</startdate><enddate>20180924</enddate><creator>Enman, Lisa J.</creator><creator>Stevens, Michaela Burke</creator><creator>Dahan, Meir Haim</creator><creator>Nellist, Michael R.</creator><creator>Toroker, Maytal Caspary</creator><creator>Boettcher, Shannon W.</creator><general>Wiley Subscription Services, Inc</general><general>Wiley Blackwell (John Wiley & Sons)</general><scope>AAYXX</scope><scope>CITATION</scope><scope>7SR</scope><scope>7U5</scope><scope>8BQ</scope><scope>8FD</scope><scope>JG9</scope><scope>L7M</scope><scope>OTOTI</scope><orcidid>https://orcid.org/0000-0001-8971-9123</orcidid><orcidid>https://orcid.org/0000-0003-1449-2977</orcidid><orcidid>https://orcid.org/0000000314492977</orcidid><orcidid>https://orcid.org/0000000189719123</orcidid></search><sort><creationdate>20180924</creationdate><title>Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts</title><author>Enman, Lisa J. ; Stevens, Michaela Burke ; Dahan, Meir Haim ; Nellist, Michael R. ; Toroker, Maytal Caspary ; Boettcher, Shannon W.</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-c2298-4f209614f442ccd54d32abb775de511bb80f51f2a60771b80482cd2bd6ddc1c93</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2018</creationdate><topic>Absorption spectroscopy</topic><topic>Catalysis</topic><topic>Cations</topic><topic>Chemistry</topic><topic>Cobalt</topic><topic>Density functional theory</topic><topic>Electrocatalysts</topic><topic>Elektrokatalysatoren</topic><topic>Evolution</topic><topic>Heterogene Katalyse</topic><topic>Hydroxides</topic><topic>Iron</topic><topic>Nickel</topic><topic>Oxidation</topic><topic>Oxygen</topic><topic>Oxygen evolution reactions</topic><topic>Röntgen-Absorptionsspektroskopie</topic><topic>Sauerstoffentwicklung</topic><topic>Spectroscopy</topic><topic>Spectrum analysis</topic><topic>Wasserelektrolyse</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Enman, Lisa J.</creatorcontrib><creatorcontrib>Stevens, Michaela Burke</creatorcontrib><creatorcontrib>Dahan, Meir Haim</creatorcontrib><creatorcontrib>Nellist, Michael R.</creatorcontrib><creatorcontrib>Toroker, Maytal Caspary</creatorcontrib><creatorcontrib>Boettcher, Shannon W.</creatorcontrib><collection>CrossRef</collection><collection>Engineered Materials Abstracts</collection><collection>Solid State and Superconductivity Abstracts</collection><collection>METADEX</collection><collection>Technology Research Database</collection><collection>Materials Research Database</collection><collection>Advanced Technologies Database with Aerospace</collection><collection>OSTI.GOV</collection><jtitle>Angewandte Chemie</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Enman, Lisa J.</au><au>Stevens, Michaela Burke</au><au>Dahan, Meir Haim</au><au>Nellist, Michael R.</au><au>Toroker, Maytal Caspary</au><au>Boettcher, Shannon W.</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts</atitle><jtitle>Angewandte Chemie</jtitle><date>2018-09-24</date><risdate>2018</risdate><volume>130</volume><issue>39</issue><spage>13022</spage><epage>13026</epage><pages>13022-13026</pages><issn>0044-8249</issn><eissn>1521-3757</eissn><abstract>Iron cations are essential for the high activity of nickel and cobalt‐based (oxy)hydroxides for the oxygen evolution reaction, but the role of iron in the catalytic mechanism remains under active investigation. Operando X‐ray absorption spectroscopy and density functional theory calculations are used to demonstrate partial Fe oxidation and a shortening of the Fe−O bond length during oxygen evolution on Co(Fe)OxHy. Cobalt oxidation during oxygen evolution is only observed in the absence of iron. These results demonstrate a different mechanism for water oxidation in the presence and absence of iron and support the hypothesis that oxidized iron species are involved in water‐oxidation catalysis on Co(Fe)OxHy.
Fe‐haltige Co‐ und Ni‐(Oxy)Hydroxide katalysieren die schnellste bekannte Wasseroxidation unter alkalischen Bedingungen, der Wirkmechanismus von Fe wird allerdings noch untersucht. Hier wird gezeigt, dass die Sauerstoffentwicklung mit einer Oxidation der Fe‐Kationen und einer Verkürzung der Fe‐O‐Bindungen einhergeht. Übereinstimmend mit DFT‐Rechnungen weisen diese Resultate auf Fe‐basierte aktive Zentren hin.</abstract><cop>Weinheim</cop><pub>Wiley Subscription Services, Inc</pub><doi>10.1002/ange.201808818</doi><tpages>5</tpages><orcidid>https://orcid.org/0000-0001-8971-9123</orcidid><orcidid>https://orcid.org/0000-0003-1449-2977</orcidid><orcidid>https://orcid.org/0000000314492977</orcidid><orcidid>https://orcid.org/0000000189719123</orcidid><oa>free_for_read</oa></addata></record> |
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| source | Wiley Online Library Journals Frontfile Complete |
| subjects | Absorption spectroscopy Catalysis Cations Chemistry Cobalt Density functional theory Electrocatalysts Elektrokatalysatoren Evolution Heterogene Katalyse Hydroxides Iron Nickel Oxidation Oxygen Oxygen evolution reactions Röntgen-Absorptionsspektroskopie Sauerstoffentwicklung Spectroscopy Spectrum analysis Wasserelektrolyse |
| title | Operando X‐Ray Absorption Spectroscopy Shows Iron Oxidation Is Concurrent with Oxygen Evolution in Cobalt–Iron (Oxy)hydroxide Electrocatalysts |
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