Effective Reversible Potentials and Onset Potentials for O2 Electroreduction on Transition Metal Electrodes: Theoretical Analysis
Results from a comprehensive approach to predicting and explaining activities of 13 transition metal cathode materials toward oxygen electroreduction are presented. Effective reversible potentials for four-electron reduction were calculated based on exergonic O–O bond scission for OOH and O2 on Pt(1...
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Veröffentlicht in: | Journal of physical chemistry. C 2013-01, Vol.117 (1), p.41-48 |
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description | Results from a comprehensive approach to predicting and explaining activities of 13 transition metal cathode materials toward oxygen electroreduction are presented. Effective reversible potentials for four-electron reduction were calculated based on exergonic O–O bond scission for OOH and O2 on Pt(111), Pt monolayer skins on Pd(111), Pt3Cu(111), Ir(111), Pt3Ni(111), Pt3Co(111), Au(111), Rh(111), Pt3Fe(111), Ru(0001), Ag(111), Pt3Ti(111), and, finally, on pure Au(111). All values based on the OOH(ads) route were several hundred millivolts less than the 1.23 V standard value for the four-electron reduction. Although the route where O2 dissociates was calculated to have higher values for their effective reversible potentials, predicted activation energies were also high, precluding this possibility in most cases. Comparison of predicted effective reversible potentials, which spanned a range of 0.3 V and measured reduction onset potentials, which according to the literature span a narrower ∼0.1 V range, suggests the possibility that higher activation energies will for some materials reduce the measured onset potentials to values less than the effective reversible potentials. Assignments based on the energy scaling model to the left- or right-hand sides of volcano-shaped activity plots at 900 mV vs O and OH adsorption bond strengths were found to be correct when the former was used. It was found for all 13 materials that the Gibbs adsorption bond strengths of OOH are at least 0.9 eV less than the ideal value of 1.35 eV, and an important goal is to reduce this gap through the discovery of new catalysts. When this is accomplished, it will be possible to construct volcano plots using current densities measured at electrode potentials approaching 1.23 V. |
doi_str_mv | 10.1021/jp307367m |
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Effective reversible potentials for four-electron reduction were calculated based on exergonic O–O bond scission for OOH and O2 on Pt(111), Pt monolayer skins on Pd(111), Pt3Cu(111), Ir(111), Pt3Ni(111), Pt3Co(111), Au(111), Rh(111), Pt3Fe(111), Ru(0001), Ag(111), Pt3Ti(111), and, finally, on pure Au(111). All values based on the OOH(ads) route were several hundred millivolts less than the 1.23 V standard value for the four-electron reduction. Although the route where O2 dissociates was calculated to have higher values for their effective reversible potentials, predicted activation energies were also high, precluding this possibility in most cases. Comparison of predicted effective reversible potentials, which spanned a range of 0.3 V and measured reduction onset potentials, which according to the literature span a narrower ∼0.1 V range, suggests the possibility that higher activation energies will for some materials reduce the measured onset potentials to values less than the effective reversible potentials. Assignments based on the energy scaling model to the left- or right-hand sides of volcano-shaped activity plots at 900 mV vs O and OH adsorption bond strengths were found to be correct when the former was used. It was found for all 13 materials that the Gibbs adsorption bond strengths of OOH are at least 0.9 eV less than the ideal value of 1.35 eV, and an important goal is to reduce this gap through the discovery of new catalysts. When this is accomplished, it will be possible to construct volcano plots using current densities measured at electrode potentials approaching 1.23 V.</description><identifier>ISSN: 1932-7447</identifier><identifier>EISSN: 1932-7455</identifier><identifier>DOI: 10.1021/jp307367m</identifier><language>eng</language><publisher>Columbus, OH: American Chemical Society</publisher><subject>Catalytic methods ; Condensed matter: structure, mechanical and thermal properties ; Cross-disciplinary physics: materials science; rheology ; Exact sciences and technology ; Materials science ; Methods of nanofabrication ; Physics ; Solid surfaces and solid-solid interfaces ; Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)</subject><ispartof>Journal of physical chemistry. 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C</title><addtitle>J. Phys. Chem. C</addtitle><description>Results from a comprehensive approach to predicting and explaining activities of 13 transition metal cathode materials toward oxygen electroreduction are presented. Effective reversible potentials for four-electron reduction were calculated based on exergonic O–O bond scission for OOH and O2 on Pt(111), Pt monolayer skins on Pd(111), Pt3Cu(111), Ir(111), Pt3Ni(111), Pt3Co(111), Au(111), Rh(111), Pt3Fe(111), Ru(0001), Ag(111), Pt3Ti(111), and, finally, on pure Au(111). All values based on the OOH(ads) route were several hundred millivolts less than the 1.23 V standard value for the four-electron reduction. Although the route where O2 dissociates was calculated to have higher values for their effective reversible potentials, predicted activation energies were also high, precluding this possibility in most cases. Comparison of predicted effective reversible potentials, which spanned a range of 0.3 V and measured reduction onset potentials, which according to the literature span a narrower ∼0.1 V range, suggests the possibility that higher activation energies will for some materials reduce the measured onset potentials to values less than the effective reversible potentials. Assignments based on the energy scaling model to the left- or right-hand sides of volcano-shaped activity plots at 900 mV vs O and OH adsorption bond strengths were found to be correct when the former was used. It was found for all 13 materials that the Gibbs adsorption bond strengths of OOH are at least 0.9 eV less than the ideal value of 1.35 eV, and an important goal is to reduce this gap through the discovery of new catalysts. When this is accomplished, it will be possible to construct volcano plots using current densities measured at electrode potentials approaching 1.23 V.</description><subject>Catalytic methods</subject><subject>Condensed matter: structure, mechanical and thermal properties</subject><subject>Cross-disciplinary physics: materials science; rheology</subject><subject>Exact sciences and technology</subject><subject>Materials science</subject><subject>Methods of nanofabrication</subject><subject>Physics</subject><subject>Solid surfaces and solid-solid interfaces</subject><subject>Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)</subject><issn>1932-7447</issn><issn>1932-7455</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2013</creationdate><recordtype>article</recordtype><recordid>eNpNUE1LAzEQDaJgrR78B7l4XJ18bVhvpdQPqFSknpfsZoIp292SpIUe_efGryoMzMzjzZvHI-SSwTUDzm5WGwFalHp9REasErzQUqnjwyz1KTmLcQWgBDAxIu8z57BNfof0BXcYom86pM9Dwj5500VqeksXfcT0H3RDoAtOZ10-DUNAu80SQ09zLYPpo__anjCZ7pdkMd7S5RtmdvJtxie96fbRx3Ny4rImXvz0MXm9my2nD8V8cf84ncwLwwSkQoNVXJdtKVirtTZlZW2DTcNBGVdaKSsnkTEA6RrGVVNxrlijOFTCOgcgxuTqW3djYv7vss_Wx3oT_NqEfc01aC2k_OOZNtarYRuyz1gzqD_zrQ_5ig-0XW8B</recordid><startdate>20130110</startdate><enddate>20130110</enddate><creator>Anderson, Alfred B</creator><creator>Jinnouchi, Ryosuke</creator><creator>Uddin, Jamal</creator><general>American Chemical Society</general><scope>IQODW</scope></search><sort><creationdate>20130110</creationdate><title>Effective Reversible Potentials and Onset Potentials for O2 Electroreduction on Transition Metal Electrodes: Theoretical Analysis</title><author>Anderson, Alfred B ; Jinnouchi, Ryosuke ; Uddin, Jamal</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a130t-70d5276c631c777a69ddbebb205af6d449f4e11004fb125b92251b52093dff003</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2013</creationdate><topic>Catalytic methods</topic><topic>Condensed matter: structure, mechanical and thermal properties</topic><topic>Cross-disciplinary physics: materials science; rheology</topic><topic>Exact sciences and technology</topic><topic>Materials science</topic><topic>Methods of nanofabrication</topic><topic>Physics</topic><topic>Solid surfaces and solid-solid interfaces</topic><topic>Surfaces and interfaces; thin films and whiskers (structure and nonelectronic properties)</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Anderson, Alfred B</creatorcontrib><creatorcontrib>Jinnouchi, Ryosuke</creatorcontrib><creatorcontrib>Uddin, Jamal</creatorcontrib><collection>Pascal-Francis</collection><jtitle>Journal of physical chemistry. C</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Anderson, Alfred B</au><au>Jinnouchi, Ryosuke</au><au>Uddin, Jamal</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Effective Reversible Potentials and Onset Potentials for O2 Electroreduction on Transition Metal Electrodes: Theoretical Analysis</atitle><jtitle>Journal of physical chemistry. C</jtitle><addtitle>J. Phys. Chem. C</addtitle><date>2013-01-10</date><risdate>2013</risdate><volume>117</volume><issue>1</issue><spage>41</spage><epage>48</epage><pages>41-48</pages><issn>1932-7447</issn><eissn>1932-7455</eissn><abstract>Results from a comprehensive approach to predicting and explaining activities of 13 transition metal cathode materials toward oxygen electroreduction are presented. Effective reversible potentials for four-electron reduction were calculated based on exergonic O–O bond scission for OOH and O2 on Pt(111), Pt monolayer skins on Pd(111), Pt3Cu(111), Ir(111), Pt3Ni(111), Pt3Co(111), Au(111), Rh(111), Pt3Fe(111), Ru(0001), Ag(111), Pt3Ti(111), and, finally, on pure Au(111). All values based on the OOH(ads) route were several hundred millivolts less than the 1.23 V standard value for the four-electron reduction. Although the route where O2 dissociates was calculated to have higher values for their effective reversible potentials, predicted activation energies were also high, precluding this possibility in most cases. Comparison of predicted effective reversible potentials, which spanned a range of 0.3 V and measured reduction onset potentials, which according to the literature span a narrower ∼0.1 V range, suggests the possibility that higher activation energies will for some materials reduce the measured onset potentials to values less than the effective reversible potentials. Assignments based on the energy scaling model to the left- or right-hand sides of volcano-shaped activity plots at 900 mV vs O and OH adsorption bond strengths were found to be correct when the former was used. It was found for all 13 materials that the Gibbs adsorption bond strengths of OOH are at least 0.9 eV less than the ideal value of 1.35 eV, and an important goal is to reduce this gap through the discovery of new catalysts. When this is accomplished, it will be possible to construct volcano plots using current densities measured at electrode potentials approaching 1.23 V.</abstract><cop>Columbus, OH</cop><pub>American Chemical Society</pub><doi>10.1021/jp307367m</doi><tpages>8</tpages></addata></record> |
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subjects | Catalytic methods Condensed matter: structure, mechanical and thermal properties Cross-disciplinary physics: materials science rheology Exact sciences and technology Materials science Methods of nanofabrication Physics Solid surfaces and solid-solid interfaces Surfaces and interfaces thin films and whiskers (structure and nonelectronic properties) |
title | Effective Reversible Potentials and Onset Potentials for O2 Electroreduction on Transition Metal Electrodes: Theoretical Analysis |
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