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000878638 0247_ $$2doi$$a10.1021/acs.nanolett.9b02116
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000878638 1001_ $$0P:(DE-HGF)0$$aDionigi, F.$$b0
000878638 245__ $$aControlling Near-Surface Ni Composition in Octahedral PtNi(Mo) Nanoparticles by Mo Doping for a Highly Active Oxygen Reduction Reaction Catalyst
000878638 260__ $$aWashington, DC$$bACS Publ.$$c2019
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000878638 520__ $$aWe report and study the translation of exceptionally high catalytic oxygen electroreduction activities of molybdenum-doped octahedrally shaped PtNi(Mo) nanoparticles from conventional thin-film rotating disk electrode screenings (3.43 ± 0.35 A mgPt–1 at 0.9 VRHE) to membrane electrode assembly (MEA)-based single fuel cell tests with sustained Pt mass activities of 0.45 A mgPt–1 at 0.9 Vcell, one of the highest ever reported performances for advanced shaped Pt alloys in real devices. Scanning transmission electron microscopy with energy dispersive X-ray analysis (STEM-EDX) reveals that Mo preferentially occupies the Pt-rich edges and vertices of the element-anisotropic octahedral PtNi particles. Furthermore, by combining in situ 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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000878638 536__ $$0G:(GEPRIS)257727131$$aDFG project 257727131 - Nanoskalige Pt Legierungselektrokatalysatoren mit definierter Morphologie: Synthese, Electrochemische Analyse, und ex-situ/in-situ Transmissionselektronenmikroskopische (TEM) Studien (257727131)$$c257727131$$x1
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000878638 7001_ $$0P:(DE-HGF)0$$aWeber, C. Cesar$$b1
000878638 7001_ $$0P:(DE-HGF)0$$aPrimbs, M.$$b2
000878638 7001_ $$0P:(DE-Juel1)161464$$aGocyla, M.$$b3
000878638 7001_ $$0P:(DE-HGF)0$$aBonastre, A. Martinez$$b4
000878638 7001_ $$0P:(DE-HGF)0$$aSpöri, C.$$b5
000878638 7001_ $$0P:(DE-HGF)0$$aSchmies, H.$$b6
000878638 7001_ $$0P:(DE-HGF)0$$aHornberger, E.$$b7
000878638 7001_ $$0P:(DE-Juel1)159484$$aKühl, S.$$b8
000878638 7001_ $$0P:(DE-HGF)0$$aDrnec, J.$$b9
000878638 7001_ $$0P:(DE-Juel1)130695$$aHeggen, M.$$b10
000878638 7001_ $$0P:(DE-HGF)0$$aSharman, J.$$b11
000878638 7001_ $$0P:(DE-HGF)0$$aDunin-Borkowski, R. Edward$$b12
000878638 7001_ $$00000-0002-3884-436X$$aStrasser, P.$$b13$$eCorresponding author
000878638 773__ $$0PERI:(DE-600)2048866-X$$a10.1021/acs.nanolett.9b02116$$gVol. 19, no. 10, p. 6876 - 6885$$n10$$p6876 - 6885$$tNano letters$$v19$$x1530-6992$$y2019
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