The First Series of Heterometallic Ln III ‐V IV Complexes Based on Substituted Malonic Acid Anions: Synthesis, Structure and Magnetic Properties
The reaction of VOSO 4 with K 2 cbdc (cbdc 2– is cyclobutane‐1,1‐dicarboxylate anion) and Ln(NO 3 ) 3 (Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Y, Er, Tm, Yb, Lu) yielded 17 novel heterometallic Ln III ‐V IV compounds comprising stable bis‐chelate units {V IV O(cbdc) 2 (H 2 O)}. Three structural...
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| Published in | European journal of inorganic chemistry Vol. 2018; no. 47; pp. 5075 - 5090 |
|---|---|
| Main Authors | , , , , , , , , , , , |
| Format | Journal Article |
| Language | English |
| Published |
19.12.2018
|
| Online Access | Get full text |
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| Abstract | The reaction of VOSO
4
with K
2
cbdc (cbdc
2–
is cyclobutane‐1,1‐dicarboxylate anion) and Ln(NO
3
)
3
(Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Y, Er, Tm, Yb, Lu) yielded 17 novel heterometallic Ln
III
‐V
IV
compounds comprising stable bis‐chelate units {V
IV
O(cbdc)
2
(H
2
O)}. Three structural types of compounds are formed depending on the nature of the rare‐earth metal: 1D polymers {[Ln(VO)(cbdc)
2
(H
2
O)
7
]
·
0.5[VO(cbdc)
2
]}
n
(structural type I) [Ln = La (
1
), Ce (
2
)], 3D polymers {[KLn(VO)
2
(cbdc)
4
(H
2
O)
9
]
·
3.5H
2
O}
n
(structural type II) [Ln = La (
3
), Ce (
4
), Pr (
5
), Nd (
6
), Sm (
7
), Eu (
8
), Gd (
9
), Tb (
10
), Dy (
11
), Ho (
12
)] comprising trinuclear units {LnV
2
}, and octanuclear complexes {[KLn(VO)
2
(cbdc)
4
(H
2
O)
11
]
·
2H
2
O}
2
(structural type III) [Ln = Y (
13
), Er (
14
), Tm (
15
), Yb (
16
), Lu (
17
)] containing dinuclear units {LnV}. Magnetic properties were investigated for all isolated compounds. The Gd
III
‐V
IV
compound has ferromagnetic and antiferromagnetic exchange interactions between isotropic V
IV
and Gd
III
ions. Calculations using the DFT method at the UB3LYP/6‐31G(d,p)/SDD level of theory were performed in order to explain the different nature of exchange interactions in two Gd
III
‐V
IV
pairs. The Yb
III
‐V
IV
complex displays single‐molecule magnet properties; the effective energy barrier was estimated at Δ
E
eff
/k
B
= 26 K. The magnetic properties of Ln
III
‐V
IV
compounds with heavy lanthanide ions (Ln
III
= Er, Tm, Yb) were rationalized in terms of crystal‐field calculations for Ln
III
ions. |
|---|---|
| AbstractList | The reaction of VOSO
4
with K
2
cbdc (cbdc
2–
is cyclobutane‐1,1‐dicarboxylate anion) and Ln(NO
3
)
3
(Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Y, Er, Tm, Yb, Lu) yielded 17 novel heterometallic Ln
III
‐V
IV
compounds comprising stable bis‐chelate units {V
IV
O(cbdc)
2
(H
2
O)}. Three structural types of compounds are formed depending on the nature of the rare‐earth metal: 1D polymers {[Ln(VO)(cbdc)
2
(H
2
O)
7
]
·
0.5[VO(cbdc)
2
]}
n
(structural type I) [Ln = La (
1
), Ce (
2
)], 3D polymers {[KLn(VO)
2
(cbdc)
4
(H
2
O)
9
]
·
3.5H
2
O}
n
(structural type II) [Ln = La (
3
), Ce (
4
), Pr (
5
), Nd (
6
), Sm (
7
), Eu (
8
), Gd (
9
), Tb (
10
), Dy (
11
), Ho (
12
)] comprising trinuclear units {LnV
2
}, and octanuclear complexes {[KLn(VO)
2
(cbdc)
4
(H
2
O)
11
]
·
2H
2
O}
2
(structural type III) [Ln = Y (
13
), Er (
14
), Tm (
15
), Yb (
16
), Lu (
17
)] containing dinuclear units {LnV}. Magnetic properties were investigated for all isolated compounds. The Gd
III
‐V
IV
compound has ferromagnetic and antiferromagnetic exchange interactions between isotropic V
IV
and Gd
III
ions. Calculations using the DFT method at the UB3LYP/6‐31G(d,p)/SDD level of theory were performed in order to explain the different nature of exchange interactions in two Gd
III
‐V
IV
pairs. The Yb
III
‐V
IV
complex displays single‐molecule magnet properties; the effective energy barrier was estimated at Δ
E
eff
/k
B
= 26 K. The magnetic properties of Ln
III
‐V
IV
compounds with heavy lanthanide ions (Ln
III
= Er, Tm, Yb) were rationalized in terms of crystal‐field calculations for Ln
III
ions. |
| Author | Bogomyakov, Artem S. Minin, Vadim V. Mironov, Vladimir S. Sidorov, Alexey A. Kiskin, Mikhail A. Efimov, Nikolay N. Ugolkova, Elena A. Bazhina, Evgeniya S. Korlyukov, Alexander A. Aleksandrov, Grigory G. Starikova, Alyona A. Eremenko, Igor L. |
| Author_xml | – sequence: 1 givenname: Evgeniya S. orcidid: 0000-0003-4722-0599 surname: Bazhina fullname: Bazhina, Evgeniya S. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 2 givenname: Grigory G. surname: Aleksandrov fullname: Aleksandrov, Grigory G. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 3 givenname: Mikhail A. orcidid: 0000-0002-8782-1308 surname: Kiskin fullname: Kiskin, Mikhail A. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 4 givenname: Alexander A. orcidid: 0000-0002-5600-9886 surname: Korlyukov fullname: Korlyukov, Alexander A. organization: A.N. Nesmeyanov Institute of Organoelement Compounds the Russian Academy of Sciences Vavilova St. 28 119991 Moscow Russian Federation – sequence: 5 givenname: Nikolay N. orcidid: 0000-0003-4651-7948 surname: Efimov fullname: Efimov, Nikolay N. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 6 givenname: Artem S. orcidid: 0000-0002-6918-5459 surname: Bogomyakov fullname: Bogomyakov, Artem S. organization: International Tomography Center Siberian Branch of the Russian Academy of Sciences Institutskaya St. 3a 630090 Novosibirsk Russian Federation – sequence: 7 givenname: Alyona A. orcidid: 0000-0001-5842-0559 surname: Starikova fullname: Starikova, Alyona A. organization: Institute of Physical and Organic Chemistry Southern Federal University Stachka Ave. 194/2 344090 Rostov‐on‐Don Russian Federation – sequence: 8 givenname: Vladimir S. orcidid: 0000-0001-7313-8279 surname: Mironov fullname: Mironov, Vladimir S. organization: Shubnikov Institute of Crystallography of Federal Scientific Research Centre “Crystallography and Photonics” the Russian Academy of Sciences Leninsky Ave. 59 119333 Moscow Russian Federation – sequence: 9 givenname: Elena A. orcidid: 0000-0001-8192-7200 surname: Ugolkova fullname: Ugolkova, Elena A. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 10 givenname: Vadim V. orcidid: 0000-0002-9620-6956 surname: Minin fullname: Minin, Vadim V. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 11 givenname: Alexey A. orcidid: 0000-0001-8892-2066 surname: Sidorov fullname: Sidorov, Alexey A. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation – sequence: 12 givenname: Igor L. orcidid: 0000-0001-6861-1404 surname: Eremenko fullname: Eremenko, Igor L. organization: N.S. Kurnakov Institute of General and Inorganic Chemistry the Russian Academy of Sciences Leninsky Ave. 31 119991 Moscow Russian Federation |
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| Snippet | The reaction of VOSO
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with K
2
cbdc (cbdc
2–
is cyclobutane‐1,1‐dicarboxylate anion) and Ln(NO
3
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3
(Ln = La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Y, Er, Tm,... |
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