A Mononuclear Uranium(IV) Single-Molecule Magnet with an Azobenzene Radical Ligand

A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2.)] (2), was obtained by one‐electron reduction of azobenzene by the trivalent uranium compound [UIII{(SiMe2NPh)3‐tacn}] (1). Compound 2 was characterized by single‐crystal X‐ray diffraction and 1...

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Vydané v:Chemistry : a European journal Ročník 21; číslo 49; s. 17817 - 17826
Hlavní autori: Antunes, Maria A., Coutinho, Joana T., Santos, Isabel C., Marçalo, Joaquim, Almeida, Manuel, Baldoví, José J., Pereira, Laura C. J., Gaita-Ariño, Alejandro, Coronado, Eugenio
Médium: Journal Article
Jazyk:English
Vydavateľské údaje: Weinheim WILEY-VCH Verlag 01.12.2015
WILEY‐VCH Verlag
Wiley Subscription Services, Inc
Predmet:
azo compounds
Chemistry
Diffraction
Electrostatics
Ligands
Low temperature
Magnetic properties
Magnetization
N ligands
Radicals
Reduction
Spectrum analysis
Uranium
Uranium compounds
X-ray diffraction
N ligands
magnetic properties
uranium
radicals
azo compounds
ISSN:0947-6539, 1521-3765, 1521-3765
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Abstract A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2.)] (2), was obtained by one‐electron reduction of azobenzene by the trivalent uranium compound [UIII{(SiMe2NPh)3‐tacn}] (1). Compound 2 was characterized by single‐crystal X‐ray diffraction and 1H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single‐molecule magnet behaviour for the first time in a mononuclear UIV compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single‐ion Hamiltonian. Uranium magnet: The mononuclear UIV complex with an azobenzene radical ligand [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2)] exhibits slow relaxation of magnetization with an energy barrier of 17.6 K. This unprecedented behaviour among UIV complexes, due to the interaction of the metal ion with the paramagnetic ligand, was investigated by means of an effective electrostatic model and provides a new strategy to design single‐ion magnets with non‐Kramers ions (see figure).
AbstractList A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3-tacn}UIV(η2-N2Ph2.)] (2), was obtained by one-electron reduction of azobenzene by the trivalent uranium compound [UIII{(SiMe2NPh)3-tacn}] (1). Compound 2 was characterized by single-crystal X-ray diffraction and 1HNMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single-molecule magnet behaviour for the first time in a mononuclear UIV compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single-ion Hamiltonian.
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe sub(2)NPh) sub(3)-tacn}U super(IV)( eta super(2)-N sub(2)Ph sub(2) super(.))] (2), was obtained by one-electron reduction of azobenzene by the trivalent uranium compound [U super(III){(SiMe sub(2)NPh) sub(3)-tacn}] (1). Compound 2 was characterized by single-crystal X-ray diffraction and super(1)HNMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single-molecule magnet behaviour for the first time in a mononuclear U super(IV) compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single-ion Hamiltonian. Uranium magnet: The mononuclear U super(IV) complex with an azobenzene radical ligand [{(SiMe sub(2)NPh) sub(3)-tacn}U super(IV)( eta super(2)-N sub(2)Ph sub(2))] exhibits slow relaxation of magnetization with an energy barrier of 17.6K. This unprecedented behaviour among U super(IV) complexes, due to the interaction of the metal ion with the paramagnetic ligand, was investigated by means of an effective electrostatic model and provides a new strategy to design single-ion magnets with non-Kramers ions (see figure).
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe 2 NPh) 3 ‐tacn}U IV (η 2 ‐N 2 Ph 2 . )] ( 2 ), was obtained by one‐electron reduction of azobenzene by the trivalent uranium compound [U III {(SiMe 2 NPh) 3 ‐tacn}] ( 1 ). Compound 2 was characterized by single‐crystal X‐ray diffraction and 1 H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single‐molecule magnet behaviour for the first time in a mononuclear U IV compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single‐ion Hamiltonian.
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2 NPh)3 -tacn}U(IV) (η(2) -N2 Ph2 (.) )] (2), was obtained by one-electron reduction of azobenzene by the trivalent uranium compound [U(III) {(SiMe2 NPh)3 -tacn}] (1). Compound 2 was characterized by single-crystal X-ray diffraction and (1) H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single-molecule magnet behaviour for the first time in a mononuclear U(IV) compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single-ion Hamiltonian.A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2 NPh)3 -tacn}U(IV) (η(2) -N2 Ph2 (.) )] (2), was obtained by one-electron reduction of azobenzene by the trivalent uranium compound [U(III) {(SiMe2 NPh)3 -tacn}] (1). Compound 2 was characterized by single-crystal X-ray diffraction and (1) H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single-molecule magnet behaviour for the first time in a mononuclear U(IV) compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single-ion Hamiltonian.
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2 NPh)3 -tacn}U(IV) (η(2) -N2 Ph2 (.) )] (2), was obtained by one-electron reduction of azobenzene by the trivalent uranium compound [U(III) {(SiMe2 NPh)3 -tacn}] (1). Compound 2 was characterized by single-crystal X-ray diffraction and (1) H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single-molecule magnet behaviour for the first time in a mononuclear U(IV) compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single-ion Hamiltonian.
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2.)] (2), was obtained by one‐electron reduction of azobenzene by the trivalent uranium compound [UIII{(SiMe2NPh)3‐tacn}] (1). Compound 2 was characterized by single‐crystal X‐ray diffraction and 1H NMR, IR, and UV/Vis/NIR spectroscopy. The magnetic properties of 2 and precursor 1 were studied by static magnetization and ac susceptibility measurements, which for the former revealed single‐molecule magnet behaviour for the first time in a mononuclear UIV compound, whereas trivalent uranium compound 1 does not exhibit slow relaxation of the magnetization at low temperatures. A first approximation to the magnetic behaviour of these compounds was attempted by combining an effective electrostatic model with a phenomenological approach using the full single‐ion Hamiltonian. Uranium magnet: The mononuclear UIV complex with an azobenzene radical ligand [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2)] exhibits slow relaxation of magnetization with an energy barrier of 17.6 K. This unprecedented behaviour among UIV complexes, due to the interaction of the metal ion with the paramagnetic ligand, was investigated by means of an effective electrostatic model and provides a new strategy to design single‐ion magnets with non‐Kramers ions (see figure).
Author Antunes, Maria A.
Santos, Isabel C.
Pereira, Laura C. J.
Almeida, Manuel
Marçalo, Joaquim
Coutinho, Joana T.
Gaita-Ariño, Alejandro
Coronado, Eugenio
Baldoví, José J.
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  surname: Santos
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  surname: Marçalo
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  surname: Baldoví
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  organization: Instituto de Ciencia Molecular, Universitat de València, C/Catedrático José Beltrán 2, 46980 Paterna (Spain)
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  givenname: Laura C. J.
  surname: Pereira
  fullname: Pereira, Laura C. J.
  email: lpereira@ctn.ist.utl.pt
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  surname: Coronado
  fullname: Coronado, Eugenio
  email: eugenio.coronado@uv.es
  organization: Instituto de Ciencia Molecular, Universitat de València, C/Catedrático José Beltrán 2, 46980 Paterna (Spain)
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Issue 49
Keywords N ligands
magnetic properties
uranium
radicals
azo compounds
Language English
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PublicationSubtitle A European Journal
PublicationTitle Chemistry : a European journal
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2014 2014; 53 126
2015; 34
2013; 4
1941; 9
2013; 66
2015; 289–290
2010; 468
1999; 121
2013; 5
2014; 136
2013 2013; 52 125
2014; 20
1998 1998; 37 110
2012; 51
2014; 5
2010; 636
2006; 27
2015; 44
1986; 5
2003; 9
2013; 113
1984
2000; 122
2005; 37
2003; 125
2014; 50
2003; 42
1998; 120
2007; 26
2014; 53
2007; 129
2015; 6
2011; 2
2013; 49
2011; 40
2013; 42
1971; 25
2006
2003 2003; 42 115
2009; 131
2014; 276
2011; 3
2014; 114
2008; 361
2011; 133
2014; 43
1993; 12
2010; 49
2013; 34
2002; 124
2002; 21
2011; 51
2011; 50
2010; 132
2013; 135
1999; 32
1988; 110
2011 2011; 50 123
2008; 130
2005; 11
2006 2006; 39 39
2014; 33
2012; 41
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Snippet A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3‐tacn}UIV(η2‐N2Ph2.)] (2), was obtained by one‐electron reduction of...
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe 2 NPh) 3 ‐tacn}U IV (η 2 ‐N 2 Ph 2 . )] ( 2 ), was obtained by one‐electron...
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2 NPh)3 -tacn}U(IV) (η(2) -N2 Ph2 (.) )] (2), was obtained by one-electron...
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe2NPh)3-tacn}UIV(η2-N2Ph2.)] (2), was obtained by one-electron reduction of...
A tetravalent uranium compound with a radical azobenzene ligand, namely, [{(SiMe sub(2)NPh) sub(3)-tacn}U super(IV)( eta super(2)-N sub(2)Ph sub(2) super(.))]...
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StartPage 17817
SubjectTerms azo compounds
Chemistry
Diffraction
Electrostatics
Ligands
Low temperature
Magnetic properties
Magnetization
N ligands
Radicals
Reduction
Spectrum analysis
Uranium
Uranium compounds
X-ray diffraction
Title A Mononuclear Uranium(IV) Single-Molecule Magnet with an Azobenzene Radical Ligand
URI https://api.istex.fr/ark:/67375/WNG-5J6880VH-7/fulltext.pdf
https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fchem.201503133
https://www.ncbi.nlm.nih.gov/pubmed/26536849
https://www.proquest.com/docview/1735661480
https://www.proquest.com/docview/1736680918
https://www.proquest.com/docview/1786165982
Volume 21
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