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@ARTICLE{Klemeyer:636202,
author = {Klemeyer, Lars and Caddeo, Francesco and Gröne, Tjark L.
R. and Harouna-Mayer, Sani Y. and Jessen, Brian and Zito,
Cecilia A. and Kopula Kesavan, Jagadesh and Dippel,
Ann-Christin and Igoa Saldana, Fernando and Mathon, Olivier
and Glatzel, Pieter and Koziej, Dorota},
title = {{S}patially {R}esolved {I}n {S}itu {X}-ray {A}bsorption
{S}pectroscopy {S}tudies of {Z}n{S} {N}anoparticle
{S}ynthesis at the {W}ater–{T}oluene {I}nterface},
journal = {ACS nano},
volume = {19},
number = {28},
issn = {1936-0851},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PUBDB-2025-03627},
pages = {25710 - 25719},
year = {2025},
abstract = {Two-phase synthesis is a well-established approach for
achieving precise control of the nanoparticle properties.
However, studying and understanding chemical transformations
in such a spatially heterogeneous system is challenging. In
this work, we introduce a two-phase synthesis route for ZnS
nanoparticles (ZnS NPs) at the water–toluene interface. By
employing spatially resolved in situ high-energy resolution
fluorescence-detected X-ray absorption spectroscopy
(HERFD-XAS) combined with density functional theory (DFT)
calculations, we track the diffusion of Zn$^{2+}$ species at
the interface, identify key reaction intermediates, and
monitor the nucleation and growth of ZnS NPs within the
toluene phase. We propose the formation of a
[Zn(H$_2$O)$_6$]$^{2+}$ complex upon dissolving Zn(Ac)$_2$
in water and the diffusion of Zn$^{2+}$ ions from water to
toluene driven by the formation of an octahedral
[Zn(OA)$_6$]$^{2+}$ complex (OA = oleylamine). Furthermore,
by complementing HERFD-XAS with total X-ray scattering
analysis, we show the formation of an intermediate
tetrahedral [Zn(SR)4]$^{2+}$ complex at 60 °C and its
successive transformation to noncrystalline ZnS nuclei at 80
°C and crystalline ZnS NPs starting at 100 °C. Thus, we
demonstrate how in situ X-ray spectroscopy can elucidate the
coordination and diffusion of Zn$^{2+}$ ions, and, in
combination with X-ray scattering studies, identify the
emergence of atomic and electronic structures during the
two-phase synthesis of ZnS nanoparticles.},
cin = {DOOR ; HAS-User / FS-PETRA-D},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PETRA-D-20210408},
pnm = {632 - Materials – Quantum, Complex and Functional
Materials (POF4-632) / 6G3 - PETRA III (DESY) (POF4-6G3) /
LINCHPIN - A platform to LINk between CHemistry and PhysIcs
of colloidal Nanomaterials (818941) / AIM, DFG project
G:(GEPRIS)390715994 - EXC 2056: CUI: Advanced Imaging of
Matter (390715994) / GRK 2536 - GRK 2536: Hybridstrukturen
auf der Nanometerskala: Chemische Konzepte zur Herstellung
heterogener Nanostrukturen mit anisotropen
Materialeigenschaften (NANOHYBRID) (408076438)},
pid = {G:(DE-HGF)POF4-632 / G:(DE-HGF)POF4-6G3 /
G:(EU-Grant)818941 / G:(GEPRIS)390715994 /
G:(GEPRIS)408076438},
experiment = {EXP:(DE-H253)P-P21.1-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:40627349},
doi = {10.1021/acsnano.5c02875},
url = {https://bib-pubdb1.desy.de/record/636202},
}