ic8b00472_si_001.pdf (2.39 MB)
Noncovalent Grafting of a DyIII2 Single-Molecule Magnet onto Chemically Modified Multiwalled Carbon Nanotubes
journal contribution
posted on 2018-05-18, 18:40 authored by Vassilis Tangoulis, Nikolia Lalioti, John Parthenios, Nikos Boukos, Ondřej Malina, Jiří Tuček, Radek ZbořilWhile synthetic methods
for the grafting of nanoparticles or photoactive molecules onto carbon
nanotubes (CNTs) have been developed in the last years, a very limited
number of reports have appeared on the grafting of single-molecule
magnets (SMMs) onto CNTs. There are many potential causes, mainly
focused on the fact that the attachment of molecules on surfaces remains
not trivial and their magnetic properties are significantly affected
upon attachment. Nevertheless, implementation of this particular type
of hybrid material in demanding fields such as spintronic devices
makes of utmost importance the investigation of new synthetic protocols
for effective grafting. In this paper, we demonstrate a new experimental
protocol for the noncovalent grafting of DyIII2 SMM, [Dy2(NO3)2(saph)2(DMF)4], where H2saph = N-salicylidene-o-aminophenol and DMF = N,N-dimethylformamide, onto the surface of functionalized multiwalled
CNTs (MWCNTs). We present a simple wet chemical method, followed by
an extensive washing protocol, where the cross-referencing of data
from high-resolution transmission electron microscopy combined with
electron energy loss spectroscopy, conventional magnetic measurements
(direct and alternating current), X-ray photoelectron spectroscopy,
and Raman spectroscopy was used to investigate the physical properties,
chemical nature, and overall magnetic behavior of the resulting hybrids.
A key point to the whole synthesis involves the functionalization
of MWCNTs with carboxylic groups, which proved to be a powerful strategy
for enhancing the ability to process MWCNTs and facilitating the preparation
of hybrid composites. While in the majority of analogous hybrid materials
the raw carbon material (multiwalled or single-walled nanotubes) is
heavily treated to minimize the contribution of contaminant traces
of magnetic nanoparticles with important effects on their electronic
properties, this method can lead easily to elimination of the largest
part of the impurities and provide an effective way to investigate/discriminate
the magnetic contribution of the SMM molecules.
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Keywords
nanoparticlecarbon materialchemical natureDMFChemically Modified Multiwalled Carbon Nanotubessingle-walled nanotubesRaman spectroscopycarbon nanotubesNoncovalent GraftingDy III 2 SMMcarboxylic groupscontributionchemical methodDy 2functionalized multiwalled CNTsDy III 2 Single-Molecule Magnetphotoactive moleculestransmission electron microscopyspintronic devicessurfacecontaminant tracesSMM moleculesattachmentprocess MWCNTssingle-molecule magnetsH 2 saphelectron energy loss spectroscopy
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