Supportless, Bismuth-Modified Palladium Nanotubes with Improved Activity and Stability for Formic Acid Oxidation
Palladium nanotubes (PdNTs) were synthesized by templated vapor deposition and investigated for formic acid electrooxidation. Annealed PdNTs are 2.4 times more active (2.19 mA/cm2) than commercial carbon-supported palladium (0.91 mA/cm2) at 0.3 V vs RHE. Bismuth modification improved nanotube perfor...
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| Veröffentlicht in: | ACS catalysis 2015-09, Vol.5 (9), p.5154-5163 |
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| container_title | ACS catalysis |
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| creator | Atkinson, Robert W St. John, Samuel Dyck, Ondrej Unocic, Kinga A Unocic, Raymond R Burke, Colten S Cisco, Joshua W Rice, Cynthia A Zawodzinski, Thomas A Papandrew, Alexander B |
| description | Palladium nanotubes (PdNTs) were synthesized by templated vapor deposition and investigated for formic acid electrooxidation. Annealed PdNTs are 2.4 times more active (2.19 mA/cm2) than commercial carbon-supported palladium (0.91 mA/cm2) at 0.3 V vs RHE. Bismuth modification improved nanotube performance over 4 times (3.75 mA/cm2) vs Pd/C and nearly 2 times vs unmodified PdNTs. A surface Bi coverage of 80% results in optimal site-specific activity by drastically reducing surface-poisoning CO generation during formic acid electrooxidation. The Bi-modified PdNTs are exceptionally stable, maintaining 2 times the area-normalized current density as Pd/C after 24 h at 0.2 V vs RHE. We attribute the enhanced activity and stability of the nanotube catalysts to the presence of highly coordinated surfaces, mimicking a flat polycrystal while retaining high surface area geometry. |
| doi_str_mv | 10.1021/acscatal.5b01239 |
| format | Article |
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(ANL), Argonne, IL (United States). Advanced Photon Source (APS)</creatorcontrib><description>Palladium nanotubes (PdNTs) were synthesized by templated vapor deposition and investigated for formic acid electrooxidation. Annealed PdNTs are 2.4 times more active (2.19 mA/cm2) than commercial carbon-supported palladium (0.91 mA/cm2) at 0.3 V vs RHE. Bismuth modification improved nanotube performance over 4 times (3.75 mA/cm2) vs Pd/C and nearly 2 times vs unmodified PdNTs. A surface Bi coverage of 80% results in optimal site-specific activity by drastically reducing surface-poisoning CO generation during formic acid electrooxidation. The Bi-modified PdNTs are exceptionally stable, maintaining 2 times the area-normalized current density as Pd/C after 24 h at 0.2 V vs RHE. We attribute the enhanced activity and stability of the nanotube catalysts to the presence of highly coordinated surfaces, mimicking a flat polycrystal while retaining high surface area geometry.</description><identifier>ISSN: 2155-5435</identifier><identifier>EISSN: 2155-5435</identifier><identifier>DOI: 10.1021/acscatal.5b01239</identifier><language>eng</language><publisher>United States: American Chemical Society</publisher><subject>anodic alumina ; bismuth adatom ; chemical vapor deposition ; formic acid oxidation ; INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY ; palladium nanotube ; templated synthesis</subject><ispartof>ACS catalysis, 2015-09, Vol.5 (9), p.5154-5163</ispartof><rights>Copyright © 2015 American Chemical Society</rights><lds50>peer_reviewed</lds50><oa>free_for_read</oa><woscitedreferencessubscribed>false</woscitedreferencessubscribed><citedby>FETCH-LOGICAL-a2649-ed046d7359a19c104c04bd71c7e8b5a4d3e56151e03d251e4d40c6367db10da83</citedby><cites>FETCH-LOGICAL-a2649-ed046d7359a19c104c04bd71c7e8b5a4d3e56151e03d251e4d40c6367db10da83</cites></display><links><openurl>$$Topenurl_article</openurl><openurlfulltext>$$Topenurlfull_article</openurlfulltext><thumbnail>$$Tsyndetics_thumb_exl</thumbnail><linktopdf>$$Uhttps://pubs.acs.org/doi/pdf/10.1021/acscatal.5b01239$$EPDF$$P50$$Gacs$$H</linktopdf><linktohtml>$$Uhttps://pubs.acs.org/doi/10.1021/acscatal.5b01239$$EHTML$$P50$$Gacs$$H</linktohtml><link.rule.ids>230,314,776,780,881,2752,27055,27903,27904,56716,56766</link.rule.ids><backlink>$$Uhttps://www.osti.gov/servlets/purl/1236883$$D View this record in Osti.gov$$Hfree_for_read</backlink></links><search><creatorcontrib>Atkinson, Robert W</creatorcontrib><creatorcontrib>St. John, Samuel</creatorcontrib><creatorcontrib>Dyck, Ondrej</creatorcontrib><creatorcontrib>Unocic, Kinga A</creatorcontrib><creatorcontrib>Unocic, Raymond R</creatorcontrib><creatorcontrib>Burke, Colten S</creatorcontrib><creatorcontrib>Cisco, Joshua W</creatorcontrib><creatorcontrib>Rice, Cynthia A</creatorcontrib><creatorcontrib>Zawodzinski, Thomas A</creatorcontrib><creatorcontrib>Papandrew, Alexander B</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)</creatorcontrib><title>Supportless, Bismuth-Modified Palladium Nanotubes with Improved Activity and Stability for Formic Acid Oxidation</title><title>ACS catalysis</title><addtitle>ACS Catal</addtitle><description>Palladium nanotubes (PdNTs) were synthesized by templated vapor deposition and investigated for formic acid electrooxidation. Annealed PdNTs are 2.4 times more active (2.19 mA/cm2) than commercial carbon-supported palladium (0.91 mA/cm2) at 0.3 V vs RHE. Bismuth modification improved nanotube performance over 4 times (3.75 mA/cm2) vs Pd/C and nearly 2 times vs unmodified PdNTs. A surface Bi coverage of 80% results in optimal site-specific activity by drastically reducing surface-poisoning CO generation during formic acid electrooxidation. The Bi-modified PdNTs are exceptionally stable, maintaining 2 times the area-normalized current density as Pd/C after 24 h at 0.2 V vs RHE. We attribute the enhanced activity and stability of the nanotube catalysts to the presence of highly coordinated surfaces, mimicking a flat polycrystal while retaining high surface area geometry.</description><subject>anodic alumina</subject><subject>bismuth adatom</subject><subject>chemical vapor deposition</subject><subject>formic acid oxidation</subject><subject>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</subject><subject>palladium nanotube</subject><subject>templated synthesis</subject><issn>2155-5435</issn><issn>2155-5435</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2015</creationdate><recordtype>article</recordtype><recordid>eNp1kM1LAzEQxYMoWGrvHoPnriabZD-OtVgtVCtUzyGbZGnK7mZJstX-96a0ghfn8maY3xuYB8AtRvcYpfhBSC9FEM09qxBOSXkBRilmLGGUsMs__TWYeL9DsSjLihyNQL8Z-t660Gjvp_DR-HYI2-TVKlMbreC7aBqhzNDCN9HZMFTawy8TtnDZ9s7uIzGTwexNOEDRKbgJojLNcaqtgwvrWiMjYRRcfxslgrHdDbiqReP15Kxj8Ll4-pi_JKv183I-WyUizWiZaIVopnLCSoFLiRGViFYqxzLXRcUEVUSzDDOsEVFpFKookhnJclVhpERBxuDudNf6YLiXJmi5lbbrtAw8ZpQVBYkQOkHSWe-drnnvTCvcgWPEj8ny32T5OdlomZ4sccN3dnBd_OJ__AfdtX2H</recordid><startdate>20150904</startdate><enddate>20150904</enddate><creator>Atkinson, Robert W</creator><creator>St. John, Samuel</creator><creator>Dyck, Ondrej</creator><creator>Unocic, Kinga A</creator><creator>Unocic, Raymond R</creator><creator>Burke, Colten S</creator><creator>Cisco, Joshua W</creator><creator>Rice, Cynthia A</creator><creator>Zawodzinski, Thomas A</creator><creator>Papandrew, Alexander B</creator><general>American Chemical Society</general><general>American Chemical Society (ACS)</general><scope>AAYXX</scope><scope>CITATION</scope><scope>OIOZB</scope><scope>OTOTI</scope></search><sort><creationdate>20150904</creationdate><title>Supportless, Bismuth-Modified Palladium Nanotubes with Improved Activity and Stability for Formic Acid Oxidation</title><author>Atkinson, Robert W ; St. John, Samuel ; Dyck, Ondrej ; Unocic, Kinga A ; Unocic, Raymond R ; Burke, Colten S ; Cisco, Joshua W ; Rice, Cynthia A ; Zawodzinski, Thomas A ; Papandrew, Alexander B</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a2649-ed046d7359a19c104c04bd71c7e8b5a4d3e56151e03d251e4d40c6367db10da83</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2015</creationdate><topic>anodic alumina</topic><topic>bismuth adatom</topic><topic>chemical vapor deposition</topic><topic>formic acid oxidation</topic><topic>INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY</topic><topic>palladium nanotube</topic><topic>templated synthesis</topic><toplevel>peer_reviewed</toplevel><toplevel>online_resources</toplevel><creatorcontrib>Atkinson, Robert W</creatorcontrib><creatorcontrib>St. John, Samuel</creatorcontrib><creatorcontrib>Dyck, Ondrej</creatorcontrib><creatorcontrib>Unocic, Kinga A</creatorcontrib><creatorcontrib>Unocic, Raymond R</creatorcontrib><creatorcontrib>Burke, Colten S</creatorcontrib><creatorcontrib>Cisco, Joshua W</creatorcontrib><creatorcontrib>Rice, Cynthia A</creatorcontrib><creatorcontrib>Zawodzinski, Thomas A</creatorcontrib><creatorcontrib>Papandrew, Alexander B</creatorcontrib><creatorcontrib>Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)</creatorcontrib><collection>CrossRef</collection><collection>OSTI.GOV - Hybrid</collection><collection>OSTI.GOV</collection><jtitle>ACS catalysis</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Atkinson, Robert W</au><au>St. John, Samuel</au><au>Dyck, Ondrej</au><au>Unocic, Kinga A</au><au>Unocic, Raymond R</au><au>Burke, Colten S</au><au>Cisco, Joshua W</au><au>Rice, Cynthia A</au><au>Zawodzinski, Thomas A</au><au>Papandrew, Alexander B</au><aucorp>Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)</aucorp><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Supportless, Bismuth-Modified Palladium Nanotubes with Improved Activity and Stability for Formic Acid Oxidation</atitle><jtitle>ACS catalysis</jtitle><addtitle>ACS Catal</addtitle><date>2015-09-04</date><risdate>2015</risdate><volume>5</volume><issue>9</issue><spage>5154</spage><epage>5163</epage><pages>5154-5163</pages><issn>2155-5435</issn><eissn>2155-5435</eissn><abstract>Palladium nanotubes (PdNTs) were synthesized by templated vapor deposition and investigated for formic acid electrooxidation. Annealed PdNTs are 2.4 times more active (2.19 mA/cm2) than commercial carbon-supported palladium (0.91 mA/cm2) at 0.3 V vs RHE. Bismuth modification improved nanotube performance over 4 times (3.75 mA/cm2) vs Pd/C and nearly 2 times vs unmodified PdNTs. A surface Bi coverage of 80% results in optimal site-specific activity by drastically reducing surface-poisoning CO generation during formic acid electrooxidation. The Bi-modified PdNTs are exceptionally stable, maintaining 2 times the area-normalized current density as Pd/C after 24 h at 0.2 V vs RHE. We attribute the enhanced activity and stability of the nanotube catalysts to the presence of highly coordinated surfaces, mimicking a flat polycrystal while retaining high surface area geometry.</abstract><cop>United States</cop><pub>American Chemical Society</pub><doi>10.1021/acscatal.5b01239</doi><tpages>10</tpages><oa>free_for_read</oa></addata></record> |
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| subjects | anodic alumina bismuth adatom chemical vapor deposition formic acid oxidation INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY palladium nanotube templated synthesis |
| title | Supportless, Bismuth-Modified Palladium Nanotubes with Improved Activity and Stability for Formic Acid Oxidation |
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