Syntheses, Structures, Electrochemistry and Magnetic Properties of Two Trinuclear Cyanide-bridged Clusters Based on Tricyanometalate Building Block
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摘要
The reaction of tricyanometallate precursor, Bu_4N[Fe(Tp)(CN)_3] and(Bu_4N)[(pzTp)Fe(CN)_3](Tp = tris(pyrazolyl)hydroborate, pzTp = tetrakis(pyrazolyl)borate) with Ni(ClO_4).26 H_2O in the presence of the monodentate N-methylimidazole ligand afforded two new cyano-bridged heterobimetallic {Fe2 Ni} trinuclear clusters, {[Fe(Tp)(CN)_3]_2[Ni(Mim)_4]}·8 H_2O(1) and {[Fe(pzTp)(CN)_3]_2[Ni(Mim)_4]}·2 CH_3OH·2H_2O(2). The molecular structure was determined by single-crystal X-ray diffraction. In the two compounds, the FeIII ions were coordinated by three cyanide carbon atoms and three nitrogen atoms of Tp(or pzTp) anions, whereas, the NiII ions were surrounded by two cyanide nitrogen atoms and four nitrogen atoms from four monodentate N-methylimidazole ligands, and they were bridged by tricyanometalate building block to form similar {Fe2Ni} trinuclear clusters. Cyclic voltammetry(CV) measurements indicated that compound 1 exhibited two quasireversible iron-centered reduction processes at –0.71 and –0.17 V and one quasireversible nickel-centered oxidation process at 0.92 V, while compound 2 showed two quasireversible iron-centered reduction processes at –0.66 and –0.09 V and one quasireversible nickel-centered oxidation process at 0.88 V. Magnetic measurements showed that compounds 1 and 2 exhibited strong intrachain ferromagnetic interaction between the low-spin Fe~Ⅲ(S = 1/2) and high-spin Ni~Ⅱ(S = 1) ions.
The reaction of tricyanometallate precursor, Bu_4N[Fe(Tp)(CN)_3] and(Bu_4N)[(pzTp)Fe(CN)_3](Tp = tris(pyrazolyl)hydroborate, pzTp = tetrakis(pyrazolyl)borate) with Ni(ClO_4).26 H_2O in the presence of the monodentate N-methylimidazole ligand afforded two new cyano-bridged heterobimetallic {Fe2 Ni} trinuclear clusters, {[Fe(Tp)(CN)_3]_2[Ni(Mim)_4]}·8 H_2O(1) and {[Fe(pzTp)(CN)_3]_2[Ni(Mim)_4]}·2 CH_3OH·2H_2O(2). The molecular structure was determined by single-crystal X-ray diffraction. In the two compounds, the FeIII ions were coordinated by three cyanide carbon atoms and three nitrogen atoms of Tp(or pzTp) anions, whereas, the NiII ions were surrounded by two cyanide nitrogen atoms and four nitrogen atoms from four monodentate N-methylimidazole ligands, and they were bridged by tricyanometalate building block to form similar {Fe2Ni} trinuclear clusters. Cyclic voltammetry(CV) measurements indicated that compound 1 exhibited two quasireversible iron-centered reduction processes at –0.71 and –0.17 V and one quasireversible nickel-centered oxidation process at 0.92 V, while compound 2 showed two quasireversible iron-centered reduction processes at –0.66 and –0.09 V and one quasireversible nickel-centered oxidation process at 0.88 V. Magnetic measurements showed that compounds 1 and 2 exhibited strong intrachain ferromagnetic interaction between the low-spin Fe~Ⅲ(S = 1/2) and high-spin Ni~Ⅱ(S = 1) ions.
The reaction of tricyanometallate precursor, Bu_4N[Fe(Tp)(CN)_3] and(Bu_4N)[(pzTp)Fe(CN)_3](Tp = tris(pyrazolyl)hydroborate, pzTp = tetrakis(pyrazolyl)borate) with Ni(ClO_4).26 H_2O in the presence of the monodentate N-methylimidazole ligand afforded two new cyano-bridged heterobimetallic {Fe2 Ni} trinuclear clusters, {[Fe(Tp)(CN)_3]_2[Ni(Mim)_4]}·8 H_2O(1) and {[Fe(pzTp)(CN)_3]_2[Ni(Mim)_4]}·2 CH_3OH·2H_2O(2). The molecular structure was determined by single-crystal X-ray diffraction. In the two compounds, the FeIII ions were coordinated by three cyanide carbon atoms and three nitrogen atoms of Tp(or pzTp) anions, whereas, the NiII ions were surrounded by two cyanide nitrogen atoms and four nitrogen atoms from four monodentate N-methylimidazole ligands, and they were bridged by tricyanometalate building block to form similar {Fe2Ni} trinuclear clusters. Cyclic voltammetry(CV) measurements indicated that compound 1 exhibited two quasireversible iron-centered reduction processes at –0.71 and –0.17 V and one quasireversible nickel-centered oxidation process at 0.92 V, while compound 2 showed two quasireversible iron-centered reduction processes at –0.66 and –0.09 V and one quasireversible nickel-centered oxidation process at 0.88 V. Magnetic measurements showed that compounds 1 and 2 exhibited strong intrachain ferromagnetic interaction between the low-spin Fe~Ⅲ(S = 1/2) and high-spin Ni~Ⅱ(S = 1) ions.
引文
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(26)Mercurol, J.; Li, Y.; Pardo, E.; Risset, O.; Seuleiman, M.; Rousselière, H.; Lescou?zec, R.; Julve, M.[FeII LSCoIII LS]2?[FeI II LSCoII HS]2 photoinduced conversion in a cyanide-bridged heterobimetallic molecular square. Chem. Commun. 2010, 46, 8995–8997.
(27)Liu,T.;Dong,D.P.;Kanegawa,S.;Kang,S.;Sato,O.;Shiota,Y.;Yoshizawa,K.;Hayami,S.;Wu,S.;He,C.;Duan,C.Y.Reversibleelectron transfer in a linear{Fe2Co}trinuclear complex induced by thermal treatment and photoirraditaion. Angew. Chem. Int. Ed. 2012, 51, 4367–4370.
(28)Hu, J. X.; Luo, L.; Lv, X. J.; Liu, L.; Liu, Q.; Yang, Y. K.; Duan, C. Y.; Luo, Y.; Liu, T. Light-induced bidirectional metal-to-metal charge transfer in a linear Fe2Co cluster. Angew. Chem. Int. Ed. 2017, 56, 7663–7668.
(29)Nihei, M.; Ui, M.; Hoshino, N.; Oshio, H. Cyanide-bridged iron(II,III)cube with multistepped redox behavior. Inorg. Chem. 2008, 47, 6106–6108.
(30)Nihei, M.; Ui, M.; Yokota, M.; Han, L.; Maeda, A.; Kishida, H.; Okamoto, H.; Oshio, H. Two-step spin conversion in a cyanide-bridged ferrous square. Angew. Chem. Int. Ed. 2005, 44, 6484–6487.
(31)Sheldrick, G. M. Program for X-ray crystal structure solution. Acta Cryst. 2015, 71, 3-8.
(2)Liu, T.; Zheng, H.; Kang, S.; Shiota, Y.; Hayami, S.; Mito, M.; Sato, O.; Yoshizawa, K.; Kanegawa, S.; Duan, C. A light-induced spin crossover actuated single-chain magnet. Nat. Commun. 2013, 4, 2826–2832.
(3)Rinehart, J. D.; Long, J. R. Exploiting single-ion anisotropy in the design of f-element single-molecule magnets. Chem. Sci. 2011, 2, 2078–2085.
(4)Sun, H. L.; Wang, Z. M.; Gao, S. Strategies towards single-chain magnets. Coord. Chem. Rev. 2010, 254, 1081–1100.
(5)Sato, O.; Tao, J.; Zhang, Y. Z. Control of magnetic properties through external stimuli. Angew. Chem. Int. Ed. 2007, 46, 2152–2187.
(6)Weng, D. F.; Wang, Z. M.; Gao, S. Framework-structured weak ferromagnets. Chem. Soc. Rev. 2011, 40, 3157-3181.
(7)Zheng,Y.Z.;Tong,M.L.;Zhang,W.X.;Chen,X.M.Coexistenceofspinfrustrationandlong-rangemagneticorderinginatriangularCoII(μ-OH)-based two-dimensional compound. Chem. Commun. 2006, 165–167.
(8)Dong, D. P.; Liu, T.; Kanegawa, S.; Kang, S.; Sato, O.; He, C.; Duan, C. Y.Photoswitchable dynamic magnetic relaxation in a well-isolated{Fe2Co}double-zigzag chain. Angew. Chem. Int. Ed. 2012, 51, 5119-5123.
(9)Liu, T.; Zhang, Y. J.; Kanegawa, S.; Sato, O. Photoinduced metal-to-metal charge transfer toward single-chain magnet. J. Am. Chem. Soc. 2010, 132,8250–8251.
(10)Clérac,R.;Miyasaka,H.;Yamashita,M.;Coulon,C.Evidenceforsingle-chainmagnetbehaviorinaMnIIINiIIchaindesignedwithhighspin magnetic units:a route to high temperature metastable magnets. J. Am. Chem. Soc. 2002, 124, 12837–12844.
(11)Wang,S.;Ding,X.H.;Zuo,J.L.;You,X.Z.;Huang,W.Tricyanometalatemolecularchemistry:atypeofversatilebuildingblocksforthe construction of cyano-bridged molecular architectures. Coord. Chem. Rev. 2011, 255, 1713–1732.
(12)Huang,F.P.;Tian,J.L.;Li,D.D.;Chen,G.J.;Gu,W.;Yan,S.P.;Liu,X.;Liao,D.Z.;Cheng,P.Pillaredcobalt-organicframeworkwithan unprecedented(3,4,6)-connected architecture showing the coexistence of spin canting and long-range magnetic ordering. CrystEngComm. 2010, 12,395–400.
(13)Toma,L.M.;Lescou?zec,R.;Pasán,J.;Ruiz-Pérez,C.;Vaissermann,J.;Cano,J.;Carrasco,R.;Wernsdorfer,W.;Lloret,F.;Julve,M.[Fe(bpym)(CN)4]:a new building block for designing single-chain magnets. J. Am. Chem. Soc. 2006, 128, 4842–4853.
(14)Liu,T.;Zhang,Y.J.;Kanegawa,S.;Sato,O.Water-switchingofspintransitionsinducedbymetal-to-metalchargetransferinamicroporous framework. Angew. Chem. Int. Ed. 2010, 49, 8645–8648.
(15)Harris, T. D.; Bennett, M. V.; Clérac, R.; Long, J. R.[ReCl4(CN)2]2:a high magnetic anisotropy building unit giving rise to the single-chain magnets(DMF)4MReCl4(CN)2(M=Mn, Fe, Co, Ni). J. Am. Chem. Soc. 2010, 132, 3980–3988.
(16)Dong,D.P.;Zhang,Y.J.;Zheng,H.;Zhuang,P.F.;Zhao,L.;Xu,Y.;Hu,J.;Liu,T.;Duan,C.Y.Slowmagneticrelaxationinacyano-bridged ferromagnetic{FeIIINiII}alternating chain. Dalton Trans. 2013, 42, 7693–7698.
(17)Dong, D. P.; Zhang, Y. J.; Jiao, C.; Zhao, L.; Liu, T.; Liu, D.; Li, Z.; Liu, J.; Liu, D. Syntheses, structures, and magnetic properties of three new cyano-bridged heterobimetallic chains based on[Fe(Tp*)(CN)3]-. New J. Chem. 2016, 40, 8451–8458.
(18)Jiang, L.; Feng, X. L.; Lu, T. B.; Gao, S. Synthesis, structures, and magnetic properties of a series of cyano-bridged Fe-Mn bimetallic complexes.Inorg. Chem. 2006, 45, 5018–5026.
(19)Li,D.;Parkin,S.;Wang,G.;Yee,G.T.;Holmes,S.M.Synthesisandspectroscopicandmagneticcharacterizationof tris(3,5-dimethylpyrazol-1-yl)borateirontricyanidebuildingblocks,acluster,andaone-dimensionalchainofsquares.Inorg.Chem.2006,45,1951–1959.
(20)Li,D.;Clérac,R.;Roubeau,O.;Harté,E.;Mathonière,C.;Bris,R.L.;Holmes,S.M.Magneticandopticalbistabilitydrivenbythermallyand photoinduced intramolecular electron transfer in a molecular cobalt iron Prussian blue analogue. J. Am. Chem. Soc. 2008, 130, 252–258.
(21)Wen,H.R.;Wang,C.F.;Song,Y.;Gao,S.;Zuo,J.L.;You,X.Z.Synthesis,crystalstructures,andmagneticpropertiesofcyano-bridged heterobimetallic chains based on[(Tp)Fe(CN)3]–. Inorg. Chem. 2006, 45, 8942–8949.
(22)Zhang, Y.; Li, D.; Clérac, R.; Kalisz, M.; Mathonière, C.; Holmes, S. M. Reversible thermally and photoinduced electron transfer in a cyano-bridged{Fe2Co2}square complex. Angew. Chem. Int. Ed. 2010, 49, 3752–3756.
(23)Li, D.; Parkin, S.; Wang, G.; Yee, G. T.; Clérac, R.; Wernsdorfer, W.; Holmes, S. M. An S=6 cyanide-bridged octanuclear FeIII4NiII4 complex that exhibits slow relaxation of the magnetization. J. Am. Chem. Soc. 2006, 128, 4214–4215.
(24)Wu,D.;Zhang,Y.;Huang,W.;Sato,O.AnS=3cyanide-bridgedtetranuclearFeIII2NiII2squarethatexhibitsslowrelaxationofmagnetization:synthesis, structure and magnetic properties. Dalton Trans. 2010, 39, 5500–5503.
(25)Nihei, M.; Sekine, Y.; Suganami, N.; Nakazawa, K.; Nakao, A.; Nakao, H.; Murakami, Y.; Oshio, H. Controlled intramolecular electron transfers in cyanide-bridged molecular squares by chemical modifications and external stimuli. J. Am. Chem. Soc. 2011, 133, 3592–3600.
(26)Mercurol, J.; Li, Y.; Pardo, E.; Risset, O.; Seuleiman, M.; Rousselière, H.; Lescou?zec, R.; Julve, M.[FeII LSCoIII LS]2?[FeI II LSCoII HS]2 photoinduced conversion in a cyanide-bridged heterobimetallic molecular square. Chem. Commun. 2010, 46, 8995–8997.
(27)Liu,T.;Dong,D.P.;Kanegawa,S.;Kang,S.;Sato,O.;Shiota,Y.;Yoshizawa,K.;Hayami,S.;Wu,S.;He,C.;Duan,C.Y.Reversibleelectron transfer in a linear{Fe2Co}trinuclear complex induced by thermal treatment and photoirraditaion. Angew. Chem. Int. Ed. 2012, 51, 4367–4370.
(28)Hu, J. X.; Luo, L.; Lv, X. J.; Liu, L.; Liu, Q.; Yang, Y. K.; Duan, C. Y.; Luo, Y.; Liu, T. Light-induced bidirectional metal-to-metal charge transfer in a linear Fe2Co cluster. Angew. Chem. Int. Ed. 2017, 56, 7663–7668.
(29)Nihei, M.; Ui, M.; Hoshino, N.; Oshio, H. Cyanide-bridged iron(II,III)cube with multistepped redox behavior. Inorg. Chem. 2008, 47, 6106–6108.
(30)Nihei, M.; Ui, M.; Yokota, M.; Han, L.; Maeda, A.; Kishida, H.; Okamoto, H.; Oshio, H. Two-step spin conversion in a cyanide-bridged ferrous square. Angew. Chem. Int. Ed. 2005, 44, 6484–6487.
(31)Sheldrick, G. M. Program for X-ray crystal structure solution. Acta Cryst. 2015, 71, 3-8.