Structure impact in antenna effect of novel upper rim substituted tetra-1,3-diketone calix[4]arenes on Tb(III) green and Yb(III) NIR-luminescence

Zairov, Rustem; Shamsutdinova, Nataliya; Podyachev, Sergey N.; Sudakova, Svetlana N.; Gimazetdinova, Gulnaz Sh.; Ризванов, И. Х.; Syakaev, Victor V.; Babaev, Vasily M.; Amirov, R. R.; Mustafina, Asiya R.

doi:10.1016/j.tet.2016.03.068

Cited by 31 publications

(24 citation statements)

References 40 publications

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“…1) according to the procedure described in the experimental section. According to our previous reports, the complex formation of 1 with both Gd(III)43 and Tb(III)44 occurs in 1:1 stoichiometry in alkaline DMF solutions. Our previous report43 on the synthesis of PSS-stabilized Gd- 1 colloids demonstrated the ability of keeping the full amount of Gd- 1 complex within NP shell, thanks to the poor solubility of the complex, experimentally confirmed by luminescence measurements of the supernatant solutions in the synthesis of PSS-stabilized Tb- 1 colloids.…”

Section: Resultsmentioning

confidence: 51%

“…1,3-Diketones have been reported as a very promising antenna-ligands for the Ln(III)-centered emission464748. The luminescent properties of Tb- 1 have recently been discussed44.…”

Section: Resultsmentioning

confidence: 99%

“…For more details see ref. 44. TEM image of dried PSS-coated Gd- 1 colloids ( g ), higher resolution TEM image of the same colloids ( h ), and schematic illustration of PSS-coated Gd- 1/ Tb- 1 nanoparticle and interactions on its core surface with water molecules and UV light ( i ).…”

Section: Figurementioning

confidence: 99%

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High performance magneto-fluorescent nanoparticles assembled from terbium and gadolinium 1,3-diketones

Zairov

Mustafina

Shamsutdinova

et al. 2017

Sci Rep

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Polyelectrolyte-coated nanoparticles consisting of terbium and gadolinium complexes with calix[4]arene tetra-diketone ligand were first synthesized. The antenna effect of the ligand on Tb(III) green luminescence and the presence of water molecules in the coordination sphere of Gd(III) bring strong luminescent and magnetic performance to the core-shell nanoparticles. The size and the core-shell morphology of the colloids were studied using transmission electron microscopy and dynamic light scattering. The correlation between photophysical and magnetic properties of the nanoparticles and their core composition was highlighted. The core composition was optimized for the longitudinal relaxivity to be greater than that of the commercial magnetic resonance imaging (MRI) contrast agents together with high level of Tb(III)-centered luminescence. The tuning of both magnetic and luminescent output of nanoparticles is obtained via the simple variation of lanthanide chelates concentrations in the initial synthetic solution. The exposure of the pheochromocytoma 12 (PC 12) tumor cells and periphery human blood lymphocytes to nanoparticles results in negligible effect on cell viability, decreased platelet aggregation and bright coloring, indicating the nanoparticles as promising candidates for dual magneto-fluorescent bioimaging.

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Section: Resultsmentioning

confidence: 51%

“…1,3-Diketones have been reported as a very promising antenna-ligands for the Ln(III)-centered emission464748. The luminescent properties of Tb- 1 have recently been discussed44.…”

Section: Resultsmentioning

confidence: 99%

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High performance magneto-fluorescent nanoparticles assembled from terbium and gadolinium 1,3-diketones

Zairov

Mustafina

Shamsutdinova

et al. 2017

Sci Rep

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“…The spectrophotometry data analyzed by Job plotting (See Figure S1 in ESI) reveal 1:1 complex formation for ligands 1 and 3 with Gd(III) in DMF solutions under alkalization by triethylamine, while both 1:2 and 1:1 complexes are interfering in case of ligand 2 . [37] Structural modelling of complexes indicates that the complex formation occurs via bis‐chelating of lanthanide ions with two neighbouring di‐ketonate‐groups of ligands 1–3 under alkalization by trimethylamine . The ligands and their lanthanide complexes are soluble in DMF and DMSO, but insoluble in water.…”

Section: Resultsmentioning

confidence: 64%

Polyelectrolyte-Stabilized Nanotemplates Based on Gd(III) Complexes with Macrocyclic Tetra-1,3-diketones as a Positive MR Contrast Agents

et al. 2016

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The work presents for the first time aqueous colloids prepared from Gd(III) complexes with 1,3-diketone derivatives as promising candidates for positive MR contrast agents (CA). The obtained colloids are based on reprecipitation of water insoluble Gd(III) complexes from organic to aqueous phases with further stabilization via layer-by-layer deposition of oppositely charged polyelectrolytes. A complex of experimental techniques reveals amorphous 3-6 nm sized Gd(III)-based hard templates encapsulated into soft polyelectrolyte capsules. Magnetic field and coating effects on T 1 -and T 2 -relaxivities for colloids with mono-, bi-and tri-layer polyelectrolyte deposition onto Gd(III)-based templates are revealed. The relaxivities of the mono-layered colloids are greater than those of commercial mononuclear Gd (III) CA. Water molecular correlation times in aqueous solutions of novel Gd(III)-based nanoparticles were calculated. T 1 -and T 2weighted MRI data show strong positive contrast.

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“…1a ) 28 and Na[Gd· 2 ] (Fig. 1b ) 27 complexes with different hydration numbers were chosen as the basis of the synthesis of the PSS-stabilized aqueous colloids. The hydration number (q) for [Gd(TTA) 3 · 1 ] is assumed to be one.…”

Section: Resultsmentioning

confidence: 99%

Hydration number: crucial role in nuclear magnetic relaxivity of Gd(III) chelate-based nanoparticles

Zairov

Khakimullina

Podyachev

et al. 2017

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Today, nanostructure-based contrast agents (CA) are emerging in the field of magnetic resonance imaging (MRI). Their sensitivity is reported as greatly improved in comparison to commercially used chelate-based ones. The present work is aimed at revealing the factors governing the efficiency of longitudinal magnetic relaxivity (r1) in aqueous colloids of core-shell Gd(III)-based nanoparticles. We report for the first time on hydration number (q) of gadolinium(III) as a substantial factor in controlling r1 values of polyelectrolyte-stabilized nanoparticles built from water insoluble complexes of Gd(III). The use of specific complex structure enables to reveal the impact of the inner-sphere hydration number on both r1 values for the Gd(III)-based nanoparticles and the photophysical properties of their luminescent Tb(III) and Eu(III) counterparts. The low hydration of TTA-based Gd(III) complexes (q ≈ 1) agrees well with the poor relaxivity values (r1 = 2.82 mM−1s−1 and r2 = 3.95 mM−1s−1), while these values tend to increase substantially (r1 = 12.41 mM−1s−1, r2 = 14.36 mM−1s−1) for aqueous Gd(III)-based colloids, when macrocyclic 1,3-diketonate is applied as the ligand (q ≈ 3). The regularities obtained in this work are fundamental in understanding the efficiency of MRI probes in the fast growing field of nanoparticulate contrast agents.

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Structure impact in antenna effect of novel upper rim substituted tetra-1,3-diketone calix[4]arenes on Tb(III) green and Yb(III) NIR-luminescence

Cited by 31 publications

References 40 publications

High performance magneto-fluorescent nanoparticles assembled from terbium and gadolinium 1,3-diketones

High performance magneto-fluorescent nanoparticles assembled from terbium and gadolinium 1,3-diketones

Polyelectrolyte-Stabilized Nanotemplates Based on Gd(III) Complexes with Macrocyclic Tetra-1,3-diketones as a Positive MR Contrast Agents

Hydration number: crucial role in nuclear magnetic relaxivity of Gd(III) chelate-based nanoparticles

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