Enhancing the Performance of Shape-Controlled Octahedral Rhodium-Doped PtNi Nanoalloys inside Hydrogen–Air Fuel Cell Cathodes Using a Rational Design of Catalysts, Supports, and LayeringClick to copy article linkArticle link copied!
- Lujin PanLujin PanTechnische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Lujin Pan
- Alice ParnièreAlice ParnièreICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, FranceMore by Alice Parnière
- Olivia DunseathOlivia DunseathJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomMore by Olivia Dunseath
- Dash FongallandDash FongallandJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomMore by Dash Fongalland
- Guillermo NicolauGuillermo NicolauJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomMore by Guillermo Nicolau
- C. Cesar WeberC. Cesar WeberTechnische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by C. Cesar Weber
- Jiasheng LuJiasheng LuTechnische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Jiasheng Lu
- Malte KlingenhofMalte KlingenhofTechnische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Malte Klingenhof
- Aleks ArinchteinAleks ArinchteinTechnische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Aleks Arinchtein
- Hyung-Suk OhHyung-Suk OhClean Energy Research Center, Korea Institute of Science and Technology, 02792 Seoul, Republic of KoreaMore by Hyung-Suk Oh
- Pierre-Yves BlanchardPierre-Yves BlanchardICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, FranceMore by Pierre-Yves Blanchard
- Sara CavaliereSara CavaliereICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, FranceInstitut Universitaire de France (IUF), 1 rue Descartes, 75231 Paris cedex 05, FranceMore by Sara Cavaliere
- Marc HeggenMarc HeggenErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyMore by Marc Heggen
- Rafal E. Dunin-BorkowskiRafal E. Dunin-BorkowskiErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyMore by Rafal E. Dunin-Borkowski
- Alex Martinez BonastreAlex Martinez BonastreJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomMore by Alex Martinez Bonastre
- Fabio Dionigi*Fabio Dionigi*Email: [email protected]Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Fabio Dionigi
- Jonathan SharmanJonathan SharmanJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomMore by Jonathan Sharman
- Deborah JonesDeborah JonesICGM, Univ. Montpellier, CNRS, ENSCM, 34095 Montpellier cedex 5, FranceMore by Deborah Jones
- Peter Strasser*Peter Strasser*Email: [email protected]Technische Universität Berlin, Straße des 17. Juni 124, 10623 Berlin, GermanyMore by Peter Strasser
Abstract

Octahedral PtNi alloy nanoparticles show a very high catalytic activity for the oxygen reduction reaction. However, their integration into membrane electrode assemblies (MEAs) is challenging, resulting in low fuel cell performance. We report the application of three strategies that are promising to improve the MEA-based fuel cell performance of octahedral PtNi alloy nanoparticles: (1) Rh surface doping to stabilize the morphology, (2) high Pt weight percentage loading on carbon to decrease the catalyst layer thickness (at parity of geometric-area-normalized Pt loading), and (3) N-functionalized carbon supports to more homogeneously distribute the ionomer. The surface chemistry of the Rh dopants is analyzed by in situ X-ray absorption spectroscopy (XAS) under applied potentials in a liquid half-cell. The Rh dopants are present at the catalyst surface with a local coordination to oxygen atoms as in Rh oxide and show potential dependent changes in the oxidation states. A rotating disk electrode (RDE) screening showed advantages in using Ketjen Black EC300J instead of carbon Vulcan XC72R to accommodate high Pt weight percentage loading (∼30 Pt wt %). Finally, a Rh-doped PtNi nanoparticle catalyst was grown on 3% nitrogen-doped Ketjen Black and tested in a MEA-based single cell after being annealed and acid washed. The results showed modest mass activity (MA), 0.35 A mgPt–1 at 0.9 V, but significantly high performance at high current density for octahedral PtNi nanoparticles, 1500 mA cm–2 at 0.6 V, to our knowledge the highest to date for this class of catalysts. Despite this achievement, the full potential of N doping could not be utilized, with samples showing negligible differences with respect to undoped carbon in both high- and low-humidity MEA testing. Even though no enhancement of mass transport at high current density by better distribution of the ionomer on the N-doped carbon was seen in MEA, this could be due to the diffusion of Ni cations, affecting ionomer interaction and overwhelming the effect of nitrogen species on the support.
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