% IMPORTANT: The following is UTF-8 encoded. This means that in the presence % of non-ASCII characters, it will not work with BibTeX 0.99 or older. % Instead, you should use an up-to-date BibTeX implementation like “bibtex8” or % “biber”. @ARTICLE{Beermann:842560, author = {Beermann, Vera and Gocyla, Martin and Kühl, Stefanie and Padgett, Elliot and Schmies, Henrike and Goerlin, Mikaela and Erini, Nina and Shviro, Meital and Heggen, Marc and Dunin-Borkowski, Rafal and Muller, David A. and Strasser, Peter}, title = {{T}uning the {E}lectrocatalytic {O}xygen {R}eduction {R}eaction {A}ctivity and {S}tability of {S}hape-{C}ontrolled {P}t–{N}i {N}anoparticles by {T}hermal {A}nnealing − {E}lucidating the {S}urface {A}tomic {S}tructural and {C}ompositional {C}hanges}, journal = {Journal of the American Chemical Society}, volume = {139}, number = {46}, issn = {1520-5126}, address = {Washington, DC}, publisher = {American Chemical Society}, reportid = {FZJ-2018-00779}, pages = {16536 - 16547}, year = {2017}, abstract = {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.}, cin = {ER-C-1 / PGI-5 / IEK-3}, ddc = {540}, cid = {I:(DE-Juel1)ER-C-1-20170209 / I:(DE-Juel1)PGI-5-20110106 / I:(DE-Juel1)IEK-3-20101013}, pnm = {143 - Controlling Configuration-Based Phenomena (POF3-143)}, pid = {G:(DE-HGF)POF3-143}, typ = {PUB:(DE-HGF)16}, pubmed = {pmid:29019692}, UT = {WOS:000416496400025}, doi = {10.1021/jacs.7b06846}, url = {https://juser.fz-juelich.de/record/842560}, }