Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition
Through nuclear magnetic relaxation and pH-metry, the details of the complexation of gadolinium(III) ions with citric acid (H<sub>4</sub>L) in water and aqueous solutions of cationic polyelectrolytes are established. It is shown that the presence of poly(ethylene imine) (PEI) in solution...
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MDPI AG
2021
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oai:doaj.org-article:22a0c8d8c0644ca093bfc2921857197e2021-11-11T17:04:31ZDesign of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition10.3390/ijms2221115901422-00671661-6596https://doaj.org/article/22a0c8d8c0644ca093bfc2921857197e2021-10-01T00:00:00Zhttps://www.mdpi.com/1422-0067/22/21/11590https://doaj.org/toc/1661-6596https://doaj.org/toc/1422-0067Through nuclear magnetic relaxation and pH-metry, the details of the complexation of gadolinium(III) ions with citric acid (H<sub>4</sub>L) in water and aqueous solutions of cationic polyelectrolytes are established. It is shown that the presence of poly(ethylene imine) (PEI) in solution affects magnetic relaxation behavior of gadolinium(III) complexes with citric acid (Cit) to a greater extent than polydiallyldimethylammonium chloride (PDDC). A large increase in relaxivity (up to 50 mM<sup>−1</sup>s<sup>−1</sup>) in the broad pH range (4–8) is revealed for the gadolinium(III)–citric acid–PEI system, which is particularly strong in the case of PEI with the molecular weight of 25 and 60 kDa. In weakly acidic medium (pH 3–7), the presence of PEI results in the formation of two tris-ligand associates [Gd(H<sub>2</sub>L)<sub>3</sub>]<sup>3</sup><sup>−</sup> and [Gd(H<sub>2</sub>L)<sub>2</sub>(HL)]<sup>4</sup><sup>−</sup>, which do not exist in aqueous medium. In weakly alkaline medium (pH 7–10), formation of ternary complexes Gd(III)–Cit–PEI with the Gd(III)–to–Cit ratio of 1:2 is evidenced. Using transmission electron microscopy (TEM) and dynamic light scattering techniques (DLS), the formation of the particles with the size of 50–100 nm possessing narrow molecular-mass distribution (PDI 0.08) is determined in the solution containing associate of PEI with tris-ligand complex [Gd(H<sub>2</sub>L)<sub>2</sub>(HL)]<sup>4</sup><sup>−</sup>.Evgenia BurilovaAlexander SolodovJulia ShayimovaJulia ZhuravlevaDarya ShurtakovaVladimir EvtjuginElena ZhiltsovaLucia ZakharovaRuslan KashapovRustem AmirovMDPI AGarticlegadolinium(III)NMR-relaxationpolyelectrolytes solutionscitrate complexesTEMBiology (General)QH301-705.5ChemistryQD1-999ENInternational Journal of Molecular Sciences, Vol 22, Iss 11590, p 11590 (2021) |
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gadolinium(III) NMR-relaxation polyelectrolytes solutions citrate complexes TEM Biology (General) QH301-705.5 Chemistry QD1-999 |
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gadolinium(III) NMR-relaxation polyelectrolytes solutions citrate complexes TEM Biology (General) QH301-705.5 Chemistry QD1-999 Evgenia Burilova Alexander Solodov Julia Shayimova Julia Zhuravleva Darya Shurtakova Vladimir Evtjugin Elena Zhiltsova Lucia Zakharova Ruslan Kashapov Rustem Amirov Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| description |
Through nuclear magnetic relaxation and pH-metry, the details of the complexation of gadolinium(III) ions with citric acid (H<sub>4</sub>L) in water and aqueous solutions of cationic polyelectrolytes are established. It is shown that the presence of poly(ethylene imine) (PEI) in solution affects magnetic relaxation behavior of gadolinium(III) complexes with citric acid (Cit) to a greater extent than polydiallyldimethylammonium chloride (PDDC). A large increase in relaxivity (up to 50 mM<sup>−1</sup>s<sup>−1</sup>) in the broad pH range (4–8) is revealed for the gadolinium(III)–citric acid–PEI system, which is particularly strong in the case of PEI with the molecular weight of 25 and 60 kDa. In weakly acidic medium (pH 3–7), the presence of PEI results in the formation of two tris-ligand associates [Gd(H<sub>2</sub>L)<sub>3</sub>]<sup>3</sup><sup>−</sup> and [Gd(H<sub>2</sub>L)<sub>2</sub>(HL)]<sup>4</sup><sup>−</sup>, which do not exist in aqueous medium. In weakly alkaline medium (pH 7–10), formation of ternary complexes Gd(III)–Cit–PEI with the Gd(III)–to–Cit ratio of 1:2 is evidenced. Using transmission electron microscopy (TEM) and dynamic light scattering techniques (DLS), the formation of the particles with the size of 50–100 nm possessing narrow molecular-mass distribution (PDI 0.08) is determined in the solution containing associate of PEI with tris-ligand complex [Gd(H<sub>2</sub>L)<sub>2</sub>(HL)]<sup>4</sup><sup>−</sup>. |
| format |
article |
| author |
Evgenia Burilova Alexander Solodov Julia Shayimova Julia Zhuravleva Darya Shurtakova Vladimir Evtjugin Elena Zhiltsova Lucia Zakharova Ruslan Kashapov Rustem Amirov |
| author_facet |
Evgenia Burilova Alexander Solodov Julia Shayimova Julia Zhuravleva Darya Shurtakova Vladimir Evtjugin Elena Zhiltsova Lucia Zakharova Ruslan Kashapov Rustem Amirov |
| author_sort |
Evgenia Burilova |
| title |
Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| title_short |
Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| title_full |
Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| title_fullStr |
Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| title_full_unstemmed |
Design of High-Relaxivity Polyelectrolyte Nanocapsules Based on Citrate Complexes of Gadolinium(III) of Unusual Composition |
| title_sort |
design of high-relaxivity polyelectrolyte nanocapsules based on citrate complexes of gadolinium(iii) of unusual composition |
| publisher |
MDPI AG |
| publishDate |
2021 |
| url |
https://doaj.org/article/22a0c8d8c0644ca093bfc2921857197e |
| work_keys_str_mv |
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