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Anion-directed assembly of lanthanide coordination polymers with SMMs properties based on a dihydrazone ligand

  • Lina Zhang , Peigao Duan , Yang Liu , Jingxian Sun , Dan Zhao EMAIL logo and Chenxia Du EMAIL logo
Published/Copyright: August 25, 2017

Abstract

Four new Ln(III)-based coordination polymers (CPs), [Eu(HL)Cl2(DMF)2]·(H2L) (1), [Dy(HL)Cl2(DMF)2]·(H2L) (2), [Er(HL)Cl2(DMF)(CH3OH)]·(DMF) (3) and [Yb(HL)Cl2(DMF)(H2O)]·(DMF) (4) (H2L=2,6-bis[(3-methoxysalicylidene)hydrazinocarbonyl]pyridine) have been synthesized through the reaction of Ln(III) chloride and H2L by using the vapour diffusion method. Interestingly, Cl as a template agent plays a vital role in the formation of the target complexes. Single-crystal X-ray diffraction studies indicate that 1 and 2 are isostructural and crystallize in triclinic space group P1̅, while complexes 3 and 4 are isostructural and crystallize in monoclinic space group C2/c. Variable temperature magnetization measurement (χMTT) demonstrates possible antiferromagnetic interactions in complex 2. Alternating-current (ac) susceptibility measurement furthermore indicated frequency dependence for both the in-phase (χ′) and out-of-phase (χ″) components in 2, suggesting that there is a slow relaxation behavior of the magnetization, which is typical of single-molecule magnets (SMMs). This is the first time that Ln(III) CPs based on such a dihydrazone ligand has been reported so far.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (21371154), the Key Scientific Research Project of Henan Province (16A150052), Science and Technology Research Project of Henan Province (172102210281) and Dr. Funds of Henan Polytechnic University (B2016-47).

References

[1] B. Moulton, M. J. Zaworotko, From molecules to crystal engineering: supramolecular isomerism and polymorphism in network solids. Chem. Rev.2001, 101, 1629.10.1021/cr9900432Search in Google Scholar PubMed

[2] C. Pettinari, A. Tăbăcaru, S. Galli, Coordination polymers and metal-organic frameworks based on poly(pyrazole)-containing ligands. Coord. Chem. Rev.2016, 307, 1.10.1016/j.ccr.2015.08.005Search in Google Scholar

[3] X. J. Zhang, W. J. Wang, Z. J. Hu, G. Wang, K. Uvdal, Coordination polymers for energy transfer: preparations, properties, sensing applications, and perspectives. Coord. Chem. Rev.2015, 284, 206.10.1016/j.ccr.2014.10.006Search in Google Scholar

[4] Z. X. Zhou, X. Z. Yan, T. R. Cook, M. L. Saha, P. J. Stang, Engineering functionalization in a supramolecular polymer: hierarchical self-organization of triply orthogonal non-covalent interactions on a supramolecular coordination complex platform. J. Am. Chem. Soc.2016, 138, 806.10.1021/jacs.5b12986Search in Google Scholar PubMed

[5] M. Wang, Y. R. Zheng, K. Ghosh, P. J. Stang, Metallosupramolecular tetragonal prisms via multicomponent coordination-driven template-free self-assembly. J. Am. Chem. Soc.2010, 132, 6282.10.1021/ja100889hSearch in Google Scholar PubMed PubMed Central

[6] R. L. E. Furlan, S. Otto, J. K. M. Sanders, Supramolecular templating in thermodynamically controlled synthesis. Proc. Sanders Natl. Acad. Sci.2002, 99, 4801.10.1073/pnas.022643699Search in Google Scholar PubMed PubMed Central

[7] C. S. Campos-Fernández, B. L. Schottel, H. T. Chifotides, J. K. Bera, J. Bacsa, J. M. Koomen, D. H. Russell, K. R. Dunbar, Anion template effect on the self-assembly and interconversion of metallacyclophanes. J. Am. Chem. Soc.2005, 127, 12909.10.1021/ja052108qSearch in Google Scholar PubMed

[8] P. Diaz, D. M. P. Mingos, R. Vilar, A. J. P. White, D. J. Williams, Anion-templated synthesis of metallacages as a means for the colorimetric detection of chlorides. Inorg. Chem.2004, 43, 7597.10.1021/ic049508jSearch in Google Scholar PubMed

[9] Y. B. Dong, H. X. Xu, J. P. Ma, R. Q. Huang, Silver(I) coordination polymers based on a nano-sized bent bis(3-acetylenylphenyl-(4-cyanophenyl))oxadiazole ligand: the role of ligand isomerism and the templating effect of polyatomic anions and solvent intermediates. Inorg. Chem.2006, 45, 3325.10.1021/ic052158wSearch in Google Scholar PubMed

[10] L. Yi, X. Yang, T. B. Lu, P. Cheng, Self-assembly of right-handed helical infinite chain, one- and two-dimensional coordination polymers tuned via anions. Cryst. Growth Des.2005, 5, 1215.10.1021/cg049587+Search in Google Scholar

[11] K. J. Wei, J. Ni, Y. Z. Liu, Q.-L. Liu, Self-assembly of silver(I) coordination polymers from AgX (X=BF4, ClO4, CF3COO, and SO3CF3) and a rigid bent 3,6-dicyano-9-phenylcarbazole ligand: the templating effect of anions. Eur. J. Inorg. Chem.2007, 24, 3868.10.1002/ejic.200601259Search in Google Scholar

[12] Q. Chen, M. H. Zeng, L. Q. Wei, M. Kurmoo, A multifaceted cage cluster, [CoII6O12⊃X] (X=Cl or F): halide template effect and frustrated magnetism. Chem. Mater.2010, 22, 4328.10.1021/cm1014459Search in Google Scholar

[13] P. H. Lin, T. J. Burchell, L. Ungur, L. F. Chibotaru, W. Wernsdorfer, M. Murugesu, A polynuclear lanthanide single-molecule magnet with a record anisotropic barrier. Angew. Chem. Int. Ed.2009, 48, 9489.10.1002/anie.200903199Search in Google Scholar

[14] Y. N. Guo, X. H. Chen, S. F. Xue, J. K. Tang, Molecular assembly and magnetic dynamics of two novel Dy6 and Dy8 aggregates. Inorg. Chem.2012, 51, 4035.10.1021/ic202170zSearch in Google Scholar

[15] R. S. Vadavi, R. V. Shenoy, D. S. Badiger, K. B. Gudasi, L. G. Devi, M. Nethaji, Crystal structure of nonadentate tricompartmental ligand derived from pyridine-2,6-dicarboxylic acid: spectroscopic, electrochemical and thermal investigations of its transition metal(II) complexes. Spectrochim. Acta A2011, 79, 348.10.1016/j.saa.2011.03.011Search in Google Scholar

[16] G. M. Sheldrick, SHELXS-97, Program for Crystal Structure Solution, University of Göttingen, Göttingen, Germany, 1997.Search in Google Scholar

[17] G. M. Sheldrick, SHELXL-97, Program for Crystal Structure Refinement, University of Göttingen, Göttingen, Germany, 1997.Search in Google Scholar

[18] V. B. Rana, S. K. Sahni, S. K. Sangal, Oxovanadium(IV) complexes of potential pentadentate ligands. J. Inorg. Nucl. Chem.1979, 41, 1498.10.1016/0022-1902(79)80223-7Search in Google Scholar

[19] T. F. Zafiropoulos, J. C. Plakatouras, S. P. Perlepes, Preparation and properties of lanthanide(III) salts with N-(2-pyridyl)pyridine-2′-carboxamide. Polyhedron1991, 10, 2405.10.1016/S0277-5387(00)86202-6Search in Google Scholar

[20] X. Chen, S. Zhan, C. Hu, Q. Meng, Y. Liu, Synthesis, electrochemical and magnetic properties of Cu3 complexes of a series of new compartmental trinucleating ligands H4L. J. Chem. Soc. Dalton Trans.1997, 2, 245.10.1039/a603850fSearch in Google Scholar

[21] J. L. Liu, Y. C. Chen, Y. Z. Zheng, W.-Q. Lin, L. Ungur, W. Wernsdorfer, L. F. Chibotaru, M.-L. Tong, Switching the anisotropy barrier of a single-ion magnet by symmetry change from quasi-D5h to quasi-Oh. Chem. Sci.2013, 4, 3310.10.1039/c3sc50843aSearch in Google Scholar

[22] T. Han, W. Shi, Z. Niu, B. Na, P. Cheng, Magnetic blocking from exchange interactions: slow relaxation of the magnetization and hysteresis loop observed in a dysprosium-nitronyl nitroxide chain compound with an antiferromagnetic ground state. Chem. Eur. J.2013, 19, 994.10.1002/chem.201202708Search in Google Scholar PubMed

[23] L. N. Zhang, C. Zhang, B. Zhang, C. X. Du, H. Hou, Two series of pH-dependent lanthanide complexes showing solvent-induced single crystal to single crystal transformation, sorption and luminescence properties. CrystEngComm2015, 17, 2837.10.1039/C5CE00263JSearch in Google Scholar

[24] J. B. Peng, Q.-C. Zhang, X.-J. Kong, Z. P. Zheng, Y.-P. Ren, L. S. Long, R.-B. Huang, L.-S. Zheng, Z. Zheng, High-nuclearity 3d–4f clusters as enhanced magnetic coolers and molecular magnets. J. Am. Chem. Soc.2012, 134, 3314.10.1021/ja209752zSearch in Google Scholar PubMed

[25] J. L. Liu, Y. C. Chen, M. L. Tong, Recent advances in the design of magnetic molecules for use as cryogenic magnetic coolants. Coord. Chem. Rev.2014, 281, 26.10.1016/j.ccr.2014.08.013Search in Google Scholar

[26] S. Y. Lin, W. Wernsdorfer, L. Ungur, A. K. Powell, Y.-N. Guo, J. Tang, L. Zhao, L. F. Chibotaru, H.-J. Zhang, Coupling Dy3 triangles to maximize the toroidal moment. Angew. Chem. Int. Ed.2012, 51, 12767.10.1002/anie.201206602Search in Google Scholar PubMed

[27] X. J. Zhang, V. Vieru, X. Feng, J.-L. Liu, Z. Zhang, B. Na, W. Shi, B.-W. Wang, A. K. Powell, L. F. Chibotaru, S. Gao, P. Cheng, J. R. Long, Influence of guest exchange on the magnetization dynamics of dilanthanide single-molecule-magnet nodes within a metal–organic framework. Angew. Chem. Int. Ed.2015, 54, 9861.10.1002/anie.201503636Search in Google Scholar PubMed

[28] J. Tang, I. Hewitt, N. T. Madhu, G. Chastanet, W. Wernsdorfer, C. E. Anson, C. Benelli, R. Sessoli, A. K. Powell, Dysprosium triangles showing single-molecule magnet behavior of thermally excited spin states. Angew. Chem. Int. Ed.2006, 45, 1729.10.1002/anie.200503564Search in Google Scholar PubMed

[29] P. H. Lin, W. B. Sun, M. F. Yu, G.-M. Li, P.-F. Yan, M. Murugesu, An unsymmetrical coordination environment leading to two slow relaxation modes in a Dy2 single-molecule magnet. Chem. Commun.2011, 47, 10993.10.1039/c1cc14223bSearch in Google Scholar PubMed

[30] Y. Wang, X. Li, T. W. Wang, Y. Song, X.-Z. You, Slow relaxation processes and single-ion magnetic behaviors in dysprosium-containing complexes. Inorg. Chem.2010, 49, 969.10.1021/ic901720aSearch in Google Scholar PubMed

[31] J. Bartolomé, G. Filoti, V. Kuncser, G. Schinteie, V. Mereacre, C. E. Anson, A. K. Powell, D. Prodius, C. Turta, Magnetostructural correlations in the tetranuclear series of {Fe3LnO2} butterfly core clusters: magnetic and Mössbauer spectroscopic study. Phys. Rev. B.2009, 80, 14430.10.1103/PhysRevB.80.014430Search in Google Scholar

[32] D. I. Alexandropoulos, A. Fournet, L. C. Silva, A. M. Mowson, V. Bekiari, G. Christou, T. C. Stamatatos, Fluorescent naphthalene diols as bridging ligands in LnIII cluster chemistry: synthetic, structural, magnetic, and photophysical characterization of LnIII8 “christmas stars”. Inorg. Chem.2014, 53, 5420.10.1021/ic500806nSearch in Google Scholar PubMed

[33] P. F. Shi, Z. Chen, G. Xiong, B. Shen, J.-Z. Sun, P. Cheng, B. Zhao, Structures, luminescence, and magnetic properties of several three-dimensional lanthanide–organic frameworks comprising 4-carboxyphenoxy acetic acid. Cryst. Growth Des.2012, 12, 5203.10.1021/cg300277mSearch in Google Scholar

[34] F. Habib, J. Long, P. H. Lin, I. Korobkov, L. Ungur, W. Wernsdorfer, L. F. Chibotaru, M. Murugesu, Supramolecular architectures for controlling slow magnetic relaxation in field-induced single-molecule magnets. Chem. Sci.2012, 3, 2158.10.1039/c2sc01029aSearch in Google Scholar

[35] L. N. Zhang, S. T. Lu, C. Zhang, C. Du, H. Hou, Highly pH-dependent synthesis of two novel three-dimensional dysprosium complexes with interesting magnetic and luminescence properties. CrystEngComm2015, 17, 846.10.1039/C4CE02023ESearch in Google Scholar

[36] N. Ishikawa, M. Sugita, T. Ishikawa, S-y. Koshihara, Y. Kaizu, Lanthanide double-decker complexes functioning as magnets at the single-molecular level. J. Am. Chem. Soc.2003, 125, 8694.10.1021/ja029629nSearch in Google Scholar PubMed

[37] J. D. Rinehart, M. Fang, W. J. Evans, J. R. Long, Strong exchange and magnetic blocking in N23-radical-bridged lanthanide complexes. Nat. Chem.2011, 3, 538.10.1038/nchem.1063Search in Google Scholar PubMed

[38] F. Habib, M. Murugesu, Lessons learned from dinuclear lanthanide nano-magnets. Chem. Soc. Rev.2013, 42, 3278.10.1039/c2cs35361jSearch in Google Scholar PubMed

[39] L. Jia, Q. Chen, Y. S. Meng, H.-L. Sun, S. Gao, Elucidation of slow magnetic relaxation in a ferromagnetic 1D dysprosium chain through magnetic dilution. Chem. Commun.2014, 50, 6052.10.1039/c4cc01368aSearch in Google Scholar PubMed

[40] S. D. Jiang, B. W. Wang, G. Su, Z.-M. Wang, S. Gao, A mononuclear dysprosium complex featuring single-molecule-magnet behavior. Angew. Chem. Int. Ed.2010, 49, 7448.10.1002/anie.201004027Search in Google Scholar PubMed

[41] Y. Bi, Y. N. Guo, L. Zhao, Y. Guo, S.-Y. Lin, S.-D. Jiang, J. Tang, B.-W. Wang, S. Gao, Capping ligand perturbed slow magnetic relaxation in dysprosium single-ion magnets. Chem. Eur. J.2011, 17, 124.10.1002/chem.201101838Search in Google Scholar PubMed


Supplemental Material:

The online version of this article offers supplementary material (https://doi.org/10.1515/zkri-2017-2076).


Received: 2017-5-21
Accepted: 2017-8-2
Published Online: 2017-8-25
Published in Print: 2018-1-26

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