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@ARTICLE{Linnenberg:830302,
author = {Linnenberg, Oliver and Moors, Marco and Solé-Daura, Albert
and López, Xavier and Bäumer, Christoph and Kentzinger,
Emmanuel and Pyckhout-Hintzen, Wim and Monakhov, Kirill},
title = {{M}olecular {C}haracteristics of a {M}ixed-{V}alence
{P}olyoxovanadate {{V} {IV}/{V} 18 {O} 42 } in {S}olution
and at the {L}iquid–{S}urface {I}nterface},
journal = {The journal of physical chemistry / C},
volume = {121},
number = {19},
issn = {1932-7455},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2017-03870},
pages = {10419 - 10429},
year = {2017},
abstract = {The understanding of the molecular state of vanadium-oxo
clusters (polyoxovanadates, POVs) in solution and on surface
is a key to their target application in catalysis as well as
molecular electronics and spintronics. We here report the
results of a combined experimental and computational study
of the behavior of nucleophilic polyoxoanions
[VIV10VV8O42(I)]5– charged balanced by Et4N+ in water, in
a one-phase organic solution of N,N-dimethylformamid (DMF)
or acetonitrile (MeCN), in a mixed solution of MeCN–water,
and at the hybrid liquid–surface interface. The molecular
characteristics of the compound (NEt4)5[V18O42(I)] (1) in
the given environments were studied by microspectroscopic,
electrochemical, scattering, and molecular mechanics
methods. Contrary to the situation in pure water, where we
observe great agglomeration with a number of intercalated
H2O molecules between POVs that are surrounded by the Et4N+
ions, no or only minor agglomeration of redox-active POVs in
an unprecedented cation-mediated fashion was detected in
pure DMF and MeCN, respectively. An inclusion of $1\%$ water
in the MeCN solution does not have an effect significant
enough to reinforce agglomeration; however, this leads to
the POV···POV interface characterized by the presence of
the Et4N+ ions and a small number of H2O molecules. Water
amounts of $≥5\%$ trigger the formation of higher
oligomers. The deposition of compound 1 from MeCN onto an
Au(111) surface affords nearly round-shaped particles (∼10
nm). The use of DMF instead of MeCN results in bigger,
irregularly shaped particles (∼30 nm). This change of
solvent gives rise to more extensive intermolecular
interactions between polyoxoanions and their countercations
as well as weaker binding of ion-pairing induced
agglomerates to the metallic substrate. Lower concentration
of adsorbed molecules leads to a submonolayer coverage and
an accompanied change of the POV’s redox state, whereas
their higher concentration results in a multilayer coverage
that offers the pristine mixed-valence structure of the
polyoxoanion. Our study provides first important insights
into the reactivity peculiarities of this redox-responsive
material class on a solid support.},
cin = {JCNS-2 / PGI-4 / JARA-FIT / PGI-7 / Neutronenstreuung ;
JCNS-1},
ddc = {540},
cid = {I:(DE-Juel1)JCNS-2-20110106 / I:(DE-Juel1)PGI-4-20110106 /
$I:(DE-82)080009_20140620$ / I:(DE-Juel1)PGI-7-20110106 /
I:(DE-Juel1)JCNS-1-20110106},
pnm = {144 - Controlling Collective States (POF3-144) / 524 -
Controlling Collective States (POF3-524) / 6212 - Quantum
Condensed Matter: Magnetism, Superconductivity (POF3-621) /
6213 - Materials and Processes for Energy and Transport
Technologies (POF3-621)},
pid = {G:(DE-HGF)POF3-144 / G:(DE-HGF)POF3-524 /
G:(DE-HGF)POF3-6212 / G:(DE-HGF)POF3-6213},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000402024200020},
doi = {10.1021/acs.jpcc.7b02138},
url = {https://juser.fz-juelich.de/record/830302},
}