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@ARTICLE{Hua:885716,
author = {Hua, Fan and Folke, Jan Markus and Liu, Zigeng and
Girgsdies, Frank and Imlau, Robert and Ruland, Holger and
Heumann, Saskia and Granwehr, Josef and Eichel, Rüdiger-A.
and Schlögl, Robert and Huang, Xing and Frei, Elias},
title = {{U}ltrathin 2{D} {F}e-{N}anosheets {S}tabilized by 2{D}
{M}esoporous {S}ilica: {S}ynthesis and {A}pplication in
{A}mmonia {S}ynthesis},
journal = {ACS applied materials $\&$ interfaces},
volume = {13},
number = {25},
issn = {1944-8252},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2020-04028},
pages = {30187 - 30197},
year = {2021},
abstract = {Developing high-performance Fe-based ammonia catalysts
through simple and cost-efficient methods has received an
increased level of attention. Herein, we report for the
first time, the synthesis of two-dimensional (2D) FeOOH
nanoflakes encapsulated by mesoporous SiO2 (mSiO2) via a
simple solution-based method for ammonia synthesis. Due to
the sticking of the mSiO2 coating layers and the limited
spaces in between, the Fe after reduction retains the 2D
morphology, showing high resistance against the sintering in
the harsh Haber–Bosch process. Compared to supported Fe
particles dispersed on mSiO2 spheres, the coated catalyst
shows a significantly improved catalytic activity by $50\%$
at 425 °C. Thermal desorption spectroscopy (TDS) reveals
the existence of a higher density of reactive sites for N2
activation in the 2D Fe catalyst, which is possibly coupled
to a larger density of surface defect sites (kinks, steps,
point defects) that are generally considered as active
centers in ammonia synthesis. Besides the structural impact
of the coating on the 2D Fe, the electronic one is
elucidated by partially substituting Si with Al in the
coating, confirmed by 29Si and 27Al magic-angle spinning
nuclear magnetic resonance (MAS NMR). An increased apparent
activation energy (Ea) of the Al-containing catalyst
evidences an influence on the nature of the active site. The
herein-developed stable 2D Fe nanostructures can serve as an
example of a 2D material applied in catalysis, offering the
chance of a rational catalyst design based on a stepwise
introduction of various promoters, in the coating and on the
metal, maintaining the spatial control of the active
centers.},
cin = {IEK-9},
ddc = {600},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {1223 - Batteries in Application (POF4-122)},
pid = {G:(DE-HGF)POF4-1223},
typ = {PUB:(DE-HGF)16},
pubmed = {34129331},
UT = {WOS:000670430100091},
doi = {10.1021/acsami.1c06771},
url = {https://juser.fz-juelich.de/record/885716},
}