10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd3+ Ions

Konstantin A. Brylev; Bulat S. Akhmadeev; Julia G. Elistratova; Irek R. Nizameev; Aidar T. Gubaidullin; Kirill V. Kholin; Ilya V. Kashnik; Noboru Kitamura; Sung Jin Kim; Yuri V. Mironov; Asiya R. Mustafina

doi:10.1021/acs.inorgchem.9b02346

^10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd³⁺ Ions

Konstantin A. Brylev, Bulat S. Akhmadeev, Julia G. Elistratova, Irek R. Nizameev, Aidar T. Gubaidullin, Kirill V. Kholin, Ilya V. Kashnik, Noboru Kitamura, Sung Jin Kim, Yuri V. Mironov, Asiya R. Mustafina

Chemistry & Nanoscience

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Abstract

New octahedral rhenium cluster complexes [{Re₆Q₈}(SO₃)₆]^10- (Q = S or Se) were synthesized starting from [{Re₆Q₈}(H₂O)₄(OH)₂]·12H₂O. The complexes were crystallized as sodium salts and characterized by X-ray single-crystal diffraction and elemental analyses, IR, UV/vis and luminescence spectroscopies. Magnetic relaxation data demonstrate the complex formation of the cluster units with gadolinium ions. The analysis of the magnetic relaxation rates measured at various Gd:cluster ratios and different concentrations revealed the conversion of the aggregates (Gd_x[{Re₆Se₈}(SO₃)₆]_y)^n- into a nanoparticulate form even at x = 1 and y ≥ 1. Thus, the self-assembly of the cluster units into the nanoparticles is greatly facilitated by counterion binding with sodium cations. The concentration conditions were optimized for the formation and hydrophilization of Na_xGd_y[{Re₆Q₈}(SO₃)₆]-based colloids with the magnetic relaxivity values of r₁₍₂₎ = 21.0(24.1) and r₁₍₂₎ = 25.9(29.8) mM^-1 s^-1 for the {Re₆S₈}²⁺ and {Re₆Se₈}²⁺ derivatives, respectively.

Original language	English
Pages (from-to)	15889-15897
Number of pages	9
Journal	Inorganic Chemistry
Volume	58
Issue number	23
DOIs	https://doi.org/10.1021/acs.inorgchem.9b02346
State	Published - 2 Dec 2019

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Brylev, K. A., Akhmadeev, B. S., Elistratova, J. G., Nizameev, I. R., Gubaidullin, A. T., Kholin, K. V., Kashnik, I. V., Kitamura, N., Kim, S. J., Mironov, Y. V., & Mustafina, A. R. (2019). ^10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd³⁺ Ions. Inorganic Chemistry, 58(23), 15889-15897. https://doi.org/10.1021/acs.inorgchem.9b02346

@article{46df9f194e2846baafd00b2c9a388735,

title = "10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd3+ Ions",

abstract = "New octahedral rhenium cluster complexes [{Re6Q8}(SO3)6]10- (Q = S or Se) were synthesized starting from [{Re6Q8}(H2O)4(OH)2]·12H2O. The complexes were crystallized as sodium salts and characterized by X-ray single-crystal diffraction and elemental analyses, IR, UV/vis and luminescence spectroscopies. Magnetic relaxation data demonstrate the complex formation of the cluster units with gadolinium ions. The analysis of the magnetic relaxation rates measured at various Gd:cluster ratios and different concentrations revealed the conversion of the aggregates (Gdx[{Re6Se8}(SO3)6]y)n- into a nanoparticulate form even at x = 1 and y ≥ 1. Thus, the self-assembly of the cluster units into the nanoparticles is greatly facilitated by counterion binding with sodium cations. The concentration conditions were optimized for the formation and hydrophilization of NaxGdy[{Re6Q8}(SO3)6]-based colloids with the magnetic relaxivity values of r1(2) = 21.0(24.1) and r1(2) = 25.9(29.8) mM-1 s-1 for the {Re6S8}2+ and {Re6Se8}2+ derivatives, respectively.",

author = "Brylev, {Konstantin A.} and Akhmadeev, {Bulat S.} and Elistratova, {Julia G.} and Nizameev, {Irek R.} and Gubaidullin, {Aidar T.} and Kholin, {Kirill V.} and Kashnik, {Ilya V.} and Noboru Kitamura and Kim, {Sung Jin} and Mironov, {Yuri V.} and Mustafina, {Asiya R.}",

note = "Funding Information: We acknowledge the Russian Science Foundation for financial support. In particular, K.A.B., I.V.K. and Y.V.M. express thanks for Grant RSF No. 19-73-20196, while B.S.A., J.G.E., I.R.N., A.T.G., and A.R.M. are indebted to Grant RSF No. 17-13-01013. Also, K.A.B. thanks the Brain Pool Program of the Korean Federation of Science and Technology Societies (KOFST) funded by the Ministry of Science, ICT and Future Planning (151-S-1-3-1190). Some experimental measurements were performed in “Center for Optical and Laser Materials Research” (St. Petersburg State University, St. Petersburg, Russian Federation). Publisher Copyright: {\textcopyright} 2019 American Chemical Society.",

year = "2019",

month = dec,

day = "2",

doi = "10.1021/acs.inorgchem.9b02346",

language = "English",

volume = "58",

pages = "15889--15897",

journal = "Inorganic Chemistry",

issn = "0020-1669",

publisher = "American Chemical Society",

number = "23",

}

Brylev, KA, Akhmadeev, BS, Elistratova, JG, Nizameev, IR, Gubaidullin, AT, Kholin, KV, Kashnik, IV, Kitamura, N, Kim, SJ, Mironov, YV & Mustafina, AR 2019, '^10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd³⁺ Ions', Inorganic Chemistry, vol. 58, no. 23, pp. 15889-15897. https://doi.org/10.1021/acs.inorgchem.9b02346

^10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd³⁺ Ions. / Brylev, Konstantin A.; Akhmadeev, Bulat S.; Elistratova, Julia G. et al.
In: Inorganic Chemistry, Vol. 58, No. 23, 02.12.2019, p. 15889-15897.

Research output: Contribution to journal › Article › peer-review

TY - JOUR

T1 - 10- (Q = S or Se)

T2 - Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd3+ Ions

AU - Brylev, Konstantin A.

AU - Akhmadeev, Bulat S.

AU - Elistratova, Julia G.

AU - Nizameev, Irek R.

AU - Gubaidullin, Aidar T.

AU - Kholin, Kirill V.

AU - Kashnik, Ilya V.

AU - Kitamura, Noboru

AU - Kim, Sung Jin

AU - Mironov, Yuri V.

AU - Mustafina, Asiya R.

N1 - Funding Information: We acknowledge the Russian Science Foundation for financial support. In particular, K.A.B., I.V.K. and Y.V.M. express thanks for Grant RSF No. 19-73-20196, while B.S.A., J.G.E., I.R.N., A.T.G., and A.R.M. are indebted to Grant RSF No. 17-13-01013. Also, K.A.B. thanks the Brain Pool Program of the Korean Federation of Science and Technology Societies (KOFST) funded by the Ministry of Science, ICT and Future Planning (151-S-1-3-1190). Some experimental measurements were performed in “Center for Optical and Laser Materials Research” (St. Petersburg State University, St. Petersburg, Russian Federation). Publisher Copyright: © 2019 American Chemical Society.

PY - 2019/12/2

Y1 - 2019/12/2

N2 - New octahedral rhenium cluster complexes [{Re6Q8}(SO3)6]10- (Q = S or Se) were synthesized starting from [{Re6Q8}(H2O)4(OH)2]·12H2O. The complexes were crystallized as sodium salts and characterized by X-ray single-crystal diffraction and elemental analyses, IR, UV/vis and luminescence spectroscopies. Magnetic relaxation data demonstrate the complex formation of the cluster units with gadolinium ions. The analysis of the magnetic relaxation rates measured at various Gd:cluster ratios and different concentrations revealed the conversion of the aggregates (Gdx[{Re6Se8}(SO3)6]y)n- into a nanoparticulate form even at x = 1 and y ≥ 1. Thus, the self-assembly of the cluster units into the nanoparticles is greatly facilitated by counterion binding with sodium cations. The concentration conditions were optimized for the formation and hydrophilization of NaxGdy[{Re6Q8}(SO3)6]-based colloids with the magnetic relaxivity values of r1(2) = 21.0(24.1) and r1(2) = 25.9(29.8) mM-1 s-1 for the {Re6S8}2+ and {Re6Se8}2+ derivatives, respectively.

AB - New octahedral rhenium cluster complexes [{Re6Q8}(SO3)6]10- (Q = S or Se) were synthesized starting from [{Re6Q8}(H2O)4(OH)2]·12H2O. The complexes were crystallized as sodium salts and characterized by X-ray single-crystal diffraction and elemental analyses, IR, UV/vis and luminescence spectroscopies. Magnetic relaxation data demonstrate the complex formation of the cluster units with gadolinium ions. The analysis of the magnetic relaxation rates measured at various Gd:cluster ratios and different concentrations revealed the conversion of the aggregates (Gdx[{Re6Se8}(SO3)6]y)n- into a nanoparticulate form even at x = 1 and y ≥ 1. Thus, the self-assembly of the cluster units into the nanoparticles is greatly facilitated by counterion binding with sodium cations. The concentration conditions were optimized for the formation and hydrophilization of NaxGdy[{Re6Q8}(SO3)6]-based colloids with the magnetic relaxivity values of r1(2) = 21.0(24.1) and r1(2) = 25.9(29.8) mM-1 s-1 for the {Re6S8}2+ and {Re6Se8}2+ derivatives, respectively.

UR - http://www.scopus.com/inward/record.url?scp=85075456534&partnerID=8YFLogxK

U2 - 10.1021/acs.inorgchem.9b02346

DO - 10.1021/acs.inorgchem.9b02346

M3 - Article

C2 - 31746193

AN - SCOPUS:85075456534

SN - 0020-1669

VL - 58

SP - 15889

EP - 15897

JO - Inorganic Chemistry

JF - Inorganic Chemistry

IS - 23

ER -

10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd3+ Ions

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^10- (Q = S or Se): Facile Synthesis and Properties of the Most Highly Charged Octahedral Cluster Complexes and High Magnetic Relaxivity of Their Colloids with Gd³⁺ Ions