Electrodeposited ultrafine TaOx/CB catalysts for PEFC cathode application: Their oxygen reduction reaction kinetics

Handle URI:
http://hdl.handle.net/10754/563891
Title:
Electrodeposited ultrafine TaOx/CB catalysts for PEFC cathode application: Their oxygen reduction reaction kinetics
Authors:
Seo, Jeongsuk; Anjum, Dalaver H.; Takanabe, Kazuhiro ( 0000-0001-5374-9451 ) ; Kubota, Jun; Domen, Kazunari
Abstract:
Ultrafine TaOx nanoparticles were electrodeposited on carbon black (CB) powder in a nonaqueous Ta complex solution at room temperature, and the resultant TaOx/CB catalysts were assessed as oxygen reduction reaction (ORR) electrocatalysts for polymer electrolyte fuel cell (PEFC) cathodes. The Ta electrodeposition process was scaled up using a newly designed working electrode containing a CB dense layer, without introducing any binder such as the ionomer Nafion in the electrode for electrodeposition. The electrodeposited TaOx/CB powders were removed from the deposition electrode and subsequent H2 treatment at varying temperatures between 523 and 1073 K was attempted to increase the ORR performance. The TaOx/CB samples were characterized by SEM, STEM, XPS, and EELS measurements. XPS and EELS results indicated the reduced nature of the Ta species caused by the high-temperature treatment in H2, while STEM images clearly revealed that the TaOx particles aggregated as the treatment temperature increased. When the TaOx/CB catalyst, which was treated at 873 K for 2 h, was deposited on a glassy carbon substrate with Nafion ionomer, it resulted in the highest activity among the samples investigated, giving an onset potential of 0.95 VRHE at -2 μA cm-2 in a 0.1 M H2SO4 solution. Moreover, the long-term stability test with 10,000 cycles of the voltammetry only led to a 6% loss in the ORR currents, demonstrating the high stability of the TaOx/CB catalysts. Kinetic analysis by R(R)DE indicated that the four-electron transfer pathway in the ORR process was dominant for this TaOx/CB catalyst, and Tafel plots showed a slope corresponding to a one-electron reaction for the rate-determining step.
KAUST Department:
Advanced Nanofabrication, Imaging and Characterization Core Lab; KAUST Catalysis Center (KCC); Physical Sciences and Engineering (PSE) Division; Chemical Science Program; Core Labs; Catalysis for Energy Conversion (CatEC)
Publisher:
Elsevier BV
Journal:
Electrochimica Acta
Issue Date:
Dec-2014
DOI:
10.1016/j.electacta.2014.10.073
Type:
Article
ISSN:
00134686
Sponsors:
This work was supported in part by the "Elements Strategy Initiative to Form Core Research Center" (since 2012) of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. This work was also funded by the international exchange program of the A3 Foresight Program of the Japan Society for the Promotion of Science (JSPS). One of the authors, Seo would like to express her gratitude for the support of the Global Centers of Excellence (GCOE) Program of JSPS for her work at the University of Tokyo.
Appears in Collections:
Articles; Advanced Nanofabrication, Imaging and Characterization Core Lab; Physical Sciences and Engineering (PSE) Division; Chemical Science Program; KAUST Catalysis Center (KCC)

Full metadata record

DC FieldValue Language
dc.contributor.authorSeo, Jeongsuken
dc.contributor.authorAnjum, Dalaver H.en
dc.contributor.authorTakanabe, Kazuhiroen
dc.contributor.authorKubota, Junen
dc.contributor.authorDomen, Kazunarien
dc.date.accessioned2015-08-03T12:18:33Zen
dc.date.available2015-08-03T12:18:33Zen
dc.date.issued2014-12en
dc.identifier.issn00134686en
dc.identifier.doi10.1016/j.electacta.2014.10.073en
dc.identifier.urihttp://hdl.handle.net/10754/563891en
dc.description.abstractUltrafine TaOx nanoparticles were electrodeposited on carbon black (CB) powder in a nonaqueous Ta complex solution at room temperature, and the resultant TaOx/CB catalysts were assessed as oxygen reduction reaction (ORR) electrocatalysts for polymer electrolyte fuel cell (PEFC) cathodes. The Ta electrodeposition process was scaled up using a newly designed working electrode containing a CB dense layer, without introducing any binder such as the ionomer Nafion in the electrode for electrodeposition. The electrodeposited TaOx/CB powders were removed from the deposition electrode and subsequent H2 treatment at varying temperatures between 523 and 1073 K was attempted to increase the ORR performance. The TaOx/CB samples were characterized by SEM, STEM, XPS, and EELS measurements. XPS and EELS results indicated the reduced nature of the Ta species caused by the high-temperature treatment in H2, while STEM images clearly revealed that the TaOx particles aggregated as the treatment temperature increased. When the TaOx/CB catalyst, which was treated at 873 K for 2 h, was deposited on a glassy carbon substrate with Nafion ionomer, it resulted in the highest activity among the samples investigated, giving an onset potential of 0.95 VRHE at -2 μA cm-2 in a 0.1 M H2SO4 solution. Moreover, the long-term stability test with 10,000 cycles of the voltammetry only led to a 6% loss in the ORR currents, demonstrating the high stability of the TaOx/CB catalysts. Kinetic analysis by R(R)DE indicated that the four-electron transfer pathway in the ORR process was dominant for this TaOx/CB catalyst, and Tafel plots showed a slope corresponding to a one-electron reaction for the rate-determining step.en
dc.description.sponsorshipThis work was supported in part by the "Elements Strategy Initiative to Form Core Research Center" (since 2012) of the Ministry of Education, Culture, Sports, Science and Technology (MEXT), Japan. This work was also funded by the international exchange program of the A3 Foresight Program of the Japan Society for the Promotion of Science (JSPS). One of the authors, Seo would like to express her gratitude for the support of the Global Centers of Excellence (GCOE) Program of JSPS for her work at the University of Tokyo.en
dc.publisherElsevier BVen
dc.subject4- or 2-electron transfer pathwayen
dc.subjectElectrodepositionen
dc.subjectNon-noble-metal catalystsen
dc.subjectORRen
dc.subjectORR kineticsen
dc.subjectPEFCsen
dc.subjectTaOx nanoparticlesen
dc.titleElectrodeposited ultrafine TaOx/CB catalysts for PEFC cathode application: Their oxygen reduction reaction kineticsen
dc.typeArticleen
dc.contributor.departmentAdvanced Nanofabrication, Imaging and Characterization Core Laben
dc.contributor.departmentKAUST Catalysis Center (KCC)en
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.contributor.departmentChemical Science Programen
dc.contributor.departmentCore Labsen
dc.contributor.departmentCatalysis for Energy Conversion (CatEC)en
dc.identifier.journalElectrochimica Actaen
dc.contributor.institutionDepartment of Chemical System Engineering, University of Tokyo, 7-3-1 HongoBunkyo-ku, Tokyo, Japanen
dc.contributor.institutionElements Strategy Initiative for Catalysts and Batteries (ESICB), Kyoto UniversityKatsura, Kyoto, Japanen
kaust.authorAnjum, Dalaver H.en
kaust.authorTakanabe, Kazuhiroen
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