Substitution Effects Regulate the Formation of Butterfly-Shaped Tetranuclear Dy(III) Cluster and Dy-Based Hydrogen-Bonded Helix Frameworks: Structure and Magnetic Properties
The generation of two types of complexes with different topological connections and completely different structural types merely via the substitution effect is extremely rare, especially for −CH3 and −C2H5 substituents with similar physical and chemical properties. Herein, we used 3-methoxysalicylal...
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Published in | Inorganic chemistry Vol. 59; no. 16; pp. 11640 - 11650 |
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Main Authors | , , , , , , |
Format | Journal Article |
Language | English |
Published |
American Chemical Society
17.08.2020
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Abstract | The generation of two types of complexes with different topological connections and completely different structural types merely via the substitution effect is extremely rare, especially for −CH3 and −C2H5 substituents with similar physical and chemical properties. Herein, we used 3-methoxysalicylaldehyde, 1,2-cyclohexanediamine, and Dy(NO3)3·6H2O to react under solvothermal conditions (CH3OH:CH3CN = 1:1) at 80 °C to obtain the butterfly-shaped tetranuclear DyIII cluster [Dy4(L 1 )4(μ3-O)2(NO3)2] (Dy 4 , H2 L 1 = 6,6′-((1E,1′E)-(cyclohexane-1,3-diylbis(azanylylidene))bis(methanylylidene))bis(2-methoxyphenol)). The ligand H2 L 1 was obtained by the Schiff base in situ reaction of 3-methoxysalicylaldehyde and 1,2-cyclohexanediamine. In the Dy 4 structure, (L 1 )2– has two different coordination modes: μ2-η1:η2:η1:η1 and μ4-η1:η2:η1:η1:η2:η1. The four DyIII ions are in two coordination environments: N2O6 (Dy1) and O9 (Dy2). The magnetic testing of cluster Dy 4 without the addition of an external field revealed that it exhibited a clear frequency-dependent behavior. We changed 3-methoxysalicylaldehyde to 3-ethoxysalicylaldehyde and obtained one case of a hydrogen-bonded helix framework, [DyL 2 (NO3)3] n ·2CH3CN (Dy-HHFs, H2 L 2 = 6,6′-((1E,1′E)-(cyclohexane-1,3-diylbis(azanylylidene))bis(methanylylidene))bis(2-ethoxyphenol)), under the same reaction conditions. The ligand H2 L 2 was formed by the Schiff base in situ reaction of 3-ethoxysalicylaldehyde and 1,2-cyclohexanediamine. All DyIII ions in the Dy-HHFs structure are in the same coordination environment (O9). The twisted S-shaped (L 2 )2– ligand is linked by a Dy(III) ion to form a spiral chain. The spiral chain is one of the independent units that is interconnected to form Dy-HHFs through three strong hydrogen-bonding interactions. Magnetic studies show that Dy-HHFs exhibits single-ion-magnet behavior (U eff = 68.59 K and τ0 = 1.10 × 10–7 s, 0 Oe DC field; U eff = 131.5 K and τ0 = 1.22 × 10–7 s, 800 Oe DC field). Ab initio calculations were performed to interpret the dynamic magnetic performance of Dy-HHFs, and a satisfactory consistency between theory and experiment exists. |
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AbstractList | The generation of two types of complexes with different topological connections and completely different structural types merely via the substitution effect is extremely rare, especially for −CH3 and −C2H5 substituents with similar physical and chemical properties. Herein, we used 3-methoxysalicylaldehyde, 1,2-cyclohexanediamine, and Dy(NO3)3·6H2O to react under solvothermal conditions (CH3OH:CH3CN = 1:1) at 80 °C to obtain the butterfly-shaped tetranuclear DyIII cluster [Dy4(L 1 )4(μ3-O)2(NO3)2] (Dy 4 , H2 L 1 = 6,6′-((1E,1′E)-(cyclohexane-1,3-diylbis(azanylylidene))bis(methanylylidene))bis(2-methoxyphenol)). The ligand H2 L 1 was obtained by the Schiff base in situ reaction of 3-methoxysalicylaldehyde and 1,2-cyclohexanediamine. In the Dy 4 structure, (L 1 )2– has two different coordination modes: μ2-η1:η2:η1:η1 and μ4-η1:η2:η1:η1:η2:η1. The four DyIII ions are in two coordination environments: N2O6 (Dy1) and O9 (Dy2). The magnetic testing of cluster Dy 4 without the addition of an external field revealed that it exhibited a clear frequency-dependent behavior. We changed 3-methoxysalicylaldehyde to 3-ethoxysalicylaldehyde and obtained one case of a hydrogen-bonded helix framework, [DyL 2 (NO3)3] n ·2CH3CN (Dy-HHFs, H2 L 2 = 6,6′-((1E,1′E)-(cyclohexane-1,3-diylbis(azanylylidene))bis(methanylylidene))bis(2-ethoxyphenol)), under the same reaction conditions. The ligand H2 L 2 was formed by the Schiff base in situ reaction of 3-ethoxysalicylaldehyde and 1,2-cyclohexanediamine. All DyIII ions in the Dy-HHFs structure are in the same coordination environment (O9). The twisted S-shaped (L 2 )2– ligand is linked by a Dy(III) ion to form a spiral chain. The spiral chain is one of the independent units that is interconnected to form Dy-HHFs through three strong hydrogen-bonding interactions. Magnetic studies show that Dy-HHFs exhibits single-ion-magnet behavior (U eff = 68.59 K and τ0 = 1.10 × 10–7 s, 0 Oe DC field; U eff = 131.5 K and τ0 = 1.22 × 10–7 s, 800 Oe DC field). Ab initio calculations were performed to interpret the dynamic magnetic performance of Dy-HHFs, and a satisfactory consistency between theory and experiment exists. |
Author | Wang, Hui-Feng Liang, Fu-Pei Zhu, Zhong-Hong Zou, Hua-Hong Yu, Shui Yin, Bing Wang, Hai-Ling |
AuthorAffiliation | Guilin University of Technology Guangxi Key Laboratory of Electrochemical and Magnetochemical Functional Materials, College of Chemistry and Bioengineering Northwest University State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry and Materials Science |
AuthorAffiliation_xml | – name: Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry and Materials Science – name: Guangxi Key Laboratory of Electrochemical and Magnetochemical Functional Materials, College of Chemistry and Bioengineering – name: Northwest University – name: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – name: Guilin University of Technology |
Author_xml | – sequence: 1 givenname: Zhong-Hong surname: Zhu fullname: Zhu, Zhong-Hong email: 18317725515@163.com organization: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – sequence: 2 givenname: Hui-Feng surname: Wang fullname: Wang, Hui-Feng organization: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – sequence: 3 givenname: Shui surname: Yu fullname: Yu, Shui organization: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – sequence: 4 givenname: Hua-Hong orcidid: 0000-0003-1968-4855 surname: Zou fullname: Zou, Hua-Hong email: gxnuchem@foxmail.com organization: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – sequence: 5 givenname: Hai-Ling surname: Wang fullname: Wang, Hai-Ling organization: State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources, Collaborative Innovation Center for Guangxi Ethnic Medicine, School of Chemistry and Pharmaceutical Science – sequence: 6 givenname: Bing orcidid: 0000-0001-8668-9504 surname: Yin fullname: Yin, Bing email: rayinyin@nwu.edu.cn organization: Northwest University – sequence: 7 givenname: Fu-Pei surname: Liang fullname: Liang, Fu-Pei email: fliangoffice@yahoo.com organization: Guilin University of Technology |
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Title | Substitution Effects Regulate the Formation of Butterfly-Shaped Tetranuclear Dy(III) Cluster and Dy-Based Hydrogen-Bonded Helix Frameworks: Structure and Magnetic Properties |
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