In this paper, we report the synthesis of surface-engineered multifunctional Eu:GdO triangular nanoplates with small size and uniform shape via a high-temperature solvothermal technique. Surface engineering has been performed by a one-step polyacrylate coating, followed by controlled conjugation chemistry. This creates the desired number of surface functional groups that can be used to attach folic acid as a targeting ligand on the nanoparticle surface. To specifically deliver the drug molecules in the nucleus, the folate density on the nanoparticle surface has been kept low. We have also modified the drug molecules with terminal double bond and ester linkage for the easy conjugation of nanoparticles. The nanoparticle surface was further modified with free thiols to specifically attach the modified drug molecules with a pH-responsive feature. High drug loading has been encountered for both hydrophilic drug daunorubicin (∼69% loading) and hydrophobic drug curcumin (∼75% loading) with excellent pH-responsive drug release. These nanoparticles have also been used as imaging probes in fluorescence imaging. Some preliminary experiments to evaluate their application in magnetic resonance imaging have also been explored. A detailed fluorescence imaging study has confirmed the efficient delivery of drugs to the nuclei of cancer cells with a high cytotoxic effect. Synthesized surface-engineered nanomaterials having small hydrodynamic size, excellent colloidal stability, and high drug-loading capacity, along with targeted and pH-responsive delivery of dual drugs to the cancer cells, will be potential nanobiomaterials for various biomedical applications.
A water-soluble hexadentate ligand
H4bedik was reproduced
and employed to synthesize the corresponding mononegative [FeIIIbedik]− complex core. In the complex formation
process, NaOH, KOH, and Ca(OH)2 bases were used in order
to have the corresponding cations as the counterpart of the mononegative
complex core. Thus, formed complexes were designated as complex 1·H2O, Na+ ion as the countercation;
complex 2, K+ ion as the countercation; and
complex 3·H2O, 1/2 Ca2+ ion
as the countercation. Complexes were characterized by IR and mass
spectrometric techniques. Additionally, the complexes were structurally
characterized by single crystal X-ray diffraction analysis. In complex 1·H2O, where the Na+ ion was present
as a countercation, a two-dimensional (2D) zigzag layer structure
was formed along the bc plane. The two adjacent layers
were parallel to each other and propagated along the same direction,
and the adjacent layers were connected to each other by H-bonding.
Thus, a three-dimensional (3D) network was found. A K+ ion-containing
complex 2 formed a one-dimensional (1D) linear network
that propagated along the b axis. H-bonding driven
3D layers were also found in complex 2. Akin to complex 1·H2O, complex 3·H2O also formed a 2D layers structure; however, the structure was planar
and not zigzag as observed in complex 1·H2O. In complex 3·H2O, two adjacent parallel
layers were propagated along two opposite directions. Thermogravimetric
analyses indicated that the stability of the complexes and the [FeIIIbedik]− complex core depended on the nature
of the countercation. Longitudinal (r
1) and transverse relaxivity (r
2) measurements
of aqueous solutions of the complexes have been performed. The value
was cation-dependent and thus emphasized different interactions between
[FeIIIbedik]− units in the presence of
different cations.
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