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Controlling Near-Surface Ni Composition in Octahedral PtNi(Mo) Nanoparticles by Mo Doping for a Highly Active Oxygen Reduction Reaction Catalyst

Fabio DionigiThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyCarl Cesar WeberThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyMathias PrimbsThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyMartin GocylaErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyAlex Martinez BonastreJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomCamillo SpöriThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyHenrike SchmiesThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyElisabeth HornbergerThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyStefanie KühlThe Electrochemical Energy, Catalysis, and Materials Science Laboratory, Department of Chemistry, Chemical Engineering Division, Technical University Berlin, 10623 Berlin, GermanyJakub DrnecEuropean Synchrotron Radiation Facility, ID 31 Beamline, BP 220, Cedex F-38043 Grenoble, FranceMarc HeggenErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyJonathan SharmanJohnson Matthey Technology Centre, Blount’s Court, Sonning Common, Reading RG4 9NH, United KingdomRafal E. Dunin‐BorkowskiErnst Ruska-Centre for Microscopy and Spectroscopy with Electrons, Forschungszentrum Jülich GmbH, 52425 Jülich, GermanyPeter StrasserErtl Center for Electrochemistry and Catalysis, Gwangju Institute of Science and Technology, Gwangju 500-712, South Korea

2019en

ABI

Annotatsiya

wide-angle X-ray spectroscopy, X-ray fluorescence, and STEM-EDX elemental mapping with electrochemical measurements, we finally succeeded to realize high Ni retention in activated PtNiMo nanoparticles even after prolonged potential-cycling stability tests. Stability losses at the anodic potential limits were mainly attributed to the loss of the octahedral particle shape. Extending the anodic potential limits of the tests to the Pt oxidation region induced detectable Ni losses and structural changes. Our study shows on an atomic level how Mo adatoms on the surface impact the Ni surface composition, which, in turn, gives rise to the exceptionally high experimental catalytic ORR reactivity and calls for strategies on how to preserve this particular surface composition to arrive at performance stabilities comparable with state-of-the-art spherical dealloyed Pt core-shell catalysts.

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DOI: 10.1021/acs.nanolett.9b02116

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