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| 100 | 1 | _ | |a Beermann, Vera |0 P:(DE-HGF)0 |b 0 |
| 245 | _ | _ | |a Tuning the Electrocatalytic Oxygen Reduction Reaction Activity and Stability of Shape-Controlled Pt–Ni Nanoparticles by Thermal Annealing − Elucidating the Surface Atomic Structural and Compositional Changes |
| 260 | _ | _ | |a Washington, DC |c 2017 |b American Chemical Society |
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| 520 | _ | _ | |a Shape-controlled octahedral Pt–Ni alloy nanoparticles exhibit remarkably high activities for the electroreduction of molecular oxygen (oxygen reduction reaction, ORR), which makes them fuel-cell cathode catalysts with exceptional potential. To unfold their full and optimized catalytic activity and stability, however, the nano-octahedra require post-synthesis thermal treatments, which alter the surface atomic structure and composition of the crystal facets. Here, we address and strive to elucidate the underlying surface chemical processes using a combination of ex situ analytical techniques with in situ transmission electron microscopy (TEM), in situ X-ray diffraction (XRD), and in situ electrochemical Fourier transformed infrared (FTIR) experiments. We present a robust fundamental correlation between annealing temperature and catalytic activity, where a ∼25 times higher ORR activity than for commercial Pt/C (2.7 A mgPt–1 at 0.9 VRHE) was reproducibly observed upon annealing at 300 °C. The electrochemical stability, however, peaked out at the most severe heat treatments at 500 °C. Aberration-corrected scanning transmission electron microscopy and energy-dispersive X-ray spectroscopy (EDX) in combination with in situ electrochemical CO stripping/FTIR data revealed subtle, but important, differences in the formation and chemical nature of Pt-rich and Ni-rich surface domains in the octahedral (111) facets. Estimating trends in surface chemisorption energies from in situ electrochemical CO/FTIR investigations suggested that balanced annealing generates an optimal degree of Pt surface enrichment, while the others exhibited mostly Ni-rich facets. The insights from our study are quite generally valid and aid in developing suitable post-synthesis thermal treatments for other alloy nanocatalysts as well. |
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| 700 | 1 | _ | |a Padgett, Elliot |0 0000-0001-9034-2335 |b 3 |
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| 700 | 1 | _ | |a Strasser, Peter |0 0000-0002-3884-436X |b 11 |e Corresponding author |
| 773 | _ | _ | |a 10.1021/jacs.7b06846 |g Vol. 139, no. 46, p. 16536 - 16547 |0 PERI:(DE-600)1472210-0 |n 46 |p 16536 - 16547 |t Journal of the American Chemical Society |v 139 |y 2017 |x 1520-5126 |
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