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@ARTICLE{Cui:201604,
author = {Cui, Chunhua and Gan, Lin and Heggen, Marc and Rudi, Stefan
and Strasser, Peter},
title = {{C}ompositional segregation in shaped {P}t alloy
nanoparticles and their structural behaviour during
electrocatalysis},
journal = {Nature materials},
volume = {12},
number = {8},
issn = {1476-4660},
address = {Basingstoke},
publisher = {Nature Publishing Group},
reportid = {FZJ-2015-03898},
pages = {765 - 771},
year = {2013},
abstract = {Shape-selective monometallic nanocatalysts offer activity
benefits based on structural sensitivity and high surface
area. In bimetallic nanoalloys with well-defined shape,
site-dependent metal surface segregation additionally
affects the catalytic activity and stability. However,
segregation on shaped alloy nanocatalysts and their
atomic-scale evolution is largely unexplored. Exemplified by
three octahedral PtxNi1−x alloy nanoparticle
electrocatalysts with unique activity for the oxygen
reduction reaction at fuel cell cathodes, we reveal an
unexpected compositional segregation structure across the
{111} facets using aberration-corrected scanning
transmission electron microscopy and electron energy-loss
spectroscopy. In contrast to theoretical predictions, the
pristine PtxNi1−x nano-octahedra feature a Pt-rich frame
along their edges and corners, whereas their Ni atoms are
preferentially segregated in their {111} facet region. We
follow their morphological and compositional evolution in
electrochemical environments and correlate this with their
exceptional catalytic activity. The octahedra preferentially
leach in their facet centres and evolve into ‘concave
octahedra’. More generally, the segregation and leaching
mechanisms revealed here highlight the complexity with which
shape-selective nanoalloys form and evolve under reactive
conditions},
cin = {PGI-5},
ddc = {610},
cid = {I:(DE-Juel1)PGI-5-20110106},
pnm = {424 - Exploratory materials and phenomena (POF2-424)},
pid = {G:(DE-HGF)POF2-424},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000322119100025},
doi = {10.1038/nmat3668},
url = {https://juser.fz-juelich.de/record/201604},
}