Heterometallic 3d-4f complexes are being investigated, for some time, as being useful in molecular magnetism, particularly as single-molecule magnets (SMMs). This interest is primarily because of the possibility of an increased ligand-mediated super-exchange phenomenon between the 3d and 4f metal ions. Such an interaction, apart from bestowing a favorable ground-state spin to the complex, also assists in reducing quantum tunneling of magnetization that is widely prevalent in SMMs making them to lose magnetization. However, assembling both 3d as well as 4f ions using same ligand system is challenging and involves the design of multi-site coordination ligands with specific coordination compartments for the 3d and the 4f metal ions while at the same time allowing these disparate metal ions to be linked to each other through a bridging ligating atom. This review presents a summary of the 3d-4f complexes primarily derived from the author's work while alluding to important examples from the literature. We also provide an outlook for the future design of such complexes.

Heterometallic 3d–4f Complexes as Single‐Molecule Magnets

Two mononuclear dysprosium(III) complexes [Dy(H3NAP)2Cl2]Cl·EtOH (1) and [Dy(H3NAP)2(H2O)Cl2]Cl·−2CH3CN·MeOH·0.5H2O (2) were obtained by coordinating an in situ formed Schiff base ligand of 1,3-bis(2-hydroxynaphthalenemethyleneamino)-propan-2-ol (H3NAP) to the dysprosium(III) ion. Their Dy(III) centers are six and seven-coordinated in octahedral and pentagonal–bipyramidal coordination geometries, respectively. Their structural difference is caused by the additional coordinated water molecule in the equatorial positions of complex 2 in comparison with that of complex 1. The well designed semi-rigid ligand contributes significantly to the low coordination numbers of Dy(III) ions in the two title complexes, as well as to their structural difference. Magnetic investigations revealed that complexes 1 and 2 are both field-induced single-ion magnets (SIMs) with their effective energy barriers being 22.9(6) and 153.9(5) K, respectively. They are typical SIM examples with their performances tuned by the coordination geometries of metal ions.

Two mononuclear dysprosium(iii) complexes with their slow magnetic relaxation behaviors tuned by coordination geometry.

https://chemistry-europe.onlinelibrary.wiley.com/doi/pdf/10.1002/ejic.201901350

Pentanuclear Spirocyclic Ni4Ln Derivatives: Field Induced Slow Magnetic Relaxation in the Dysprosium and Erbium Analogues

In the past two decades, tremendous progress has been made in the field of single-molecule magnets (SMMs), which not only achieves breakthroughs in various key indicators (flipping energy barrier and hysteresis temperature), but also expands SMMs of various types (3d, 4f, 3d–4f and 5f) and different connection methods. Among the many different types of SMM mentioned above, the SMM based on the 4f metal center has made the biggest breakthrough. Introducing 3d metal ions into lanthanide complexes to form 3d–4f heterometallic complexes can promote strong magnetic exchange between multiple metal centers, resulting in magnetic properties different from 3d and 4f complexes. Therefore, the expansion of the structure and magnetic properties of 3d–4f heterometallic complexes can promote the progress in the field of SMM. In this review, we summarize the structure and magnetic properties of 3d–4f heterometallic complexes formed by different types of organic ligands.

Heterometallic 3d/4f-Metal Complexes: Structure and Magnetism

Three heterometallic dinuclear compounds, [MIIDyIII(L)(Pc)(ROH)]·ROH (R = CH3, M = Ni (1), Zn (2); R = C2H5, M = Zn (3)), were stepwise synthesized based on phthalocyanine (H2Pc) and one tripodal S...

Modulating Magnetic Property of Phthalocyanine Supported MII-DyIII (M = Ni, Zn) Heterodinuclear Complexes.

To achieve a heterometallic single-molecule magnet with novel topologies, two isostructural hexanuclear clusters [Ni4Ln2(μ3-OH)2L4(OAc)8]·H2O [Ln = Dy, 1; Y, 2] were prepared from the reactions of 1,3-diamine-2-propanol (HL) with MCl3·6H2O (M = Dy, Y) and Ni(OAc)2·4H2O in acetonitrile, in which the studies for 2 with the diamagnetic metal ion of Y(III) are just for further understanding of the magnetic properties of 1. Single-crystal X-ray diffraction measurements indicate that both heterometallic hexanuclear complexes possess an S-shaped double-pocket skeleton with the two M(III) ions separated by a chair-like Ni4O4 moiety. The temperature- and frequency-dependent alternating-current (ac) susceptibility measurements under zero dc fields revealed a single-molecule magnet for 1. Its magnetic properties can be further understood based on the magnetic analysis of 2.

Heterometallic hexanuclear Ni4M2 (M = Dy, Y) complexes: structure and single-molecule magnet for the Dy(III) derivative

The invention discloses a terbium copper hetero-metal coordination polymer with a single-chain magnet magnetic switch effect and a preparation method of the terbium copper hetero-metal coordination polymer. A chemical formula of the polymer is as follows: [Cu3Tb2(Htris)2(H2tris)2(NO3)6].2C2H5OH. The preparation method comprises the following steps: successively weighing Cu(OAc)2.H2O, Tb(NO3)3.5H2O and H3tris, and dissolving in absolute ethyl alcohol, placing an obtained mixed solution in a container, vacuumizing, sealing, reacting under a heating condition, cooling, and thus obtaining a target product. A research result shows that when free object ethanol molecules are not lost, the coordination polymer has a slow relaxation behavior; and after the free ethanol molecules are lost, the coordination polymer does not have the slow relaxation behavior at all, so that the single-chain magnet magnetic switch effect is realized by successively utilizing the obtaining and loss of the object molecules.

Terbium copper hetero-metal coordination polymer with single-chain magnet magnetic switch effect and preparation method of terbium copper hetero-metal coordination polymer

The invention discloses a linear valence-variable trinuclear Co cluster compound with double crystalline states and a preparation method of the linear valence-variable trinuclear Co cluster compound. The chemical formula is [Co 2Co L6](ClO4)2, wherein L represents a negative one-valance isopropanolamine anion. The cluster compound has two different crystalline states including a crystalline state 1 and a crystalline state 2, wherein a preparation method of the crystalline state 1 comprises steps as follows: isopropanolamine and Co(ClO4)2*6H2O are taken and dissolved in an organic solvent, a mixed solution is added to a container, the container is sealed after vacuum pumping, the mixed solution reacts under the heating condition, and a product is obtained; a preparation method of the crystalline state 2 comprises steps as follows: isopropanolamine, Co(ClO4)2*6H2O and strong alkali substances are taken and dissolved in an organic solvent, a mixed solution is added to a container, the container is sealed after vacuum pumping, the mixed solution reacts under the heating condition, and a product is obtained. The cluster compound has two different crystalline states, solid reversible transformation from a single crystal to a single crystal can be performed between the crystalline states, and the two crystalline states have different magnetic properties.

Linear valence-variable trinuclear Co cluster compound with double crystalline states and preparation method of linear valence-variable trinuclear Co cluster compound

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Heterometallic hexanuclear Ni4M2 (M = Dy, Y) complexes: structure and single-molecule magnet for the Dy(III) derivative

Terbium copper hetero-metal coordination polymer with single-chain magnet magnetic switch effect and preparation method of terbium copper hetero-metal coordination polymer

Linear valence-variable trinuclear Co cluster compound with double crystalline states and preparation method of linear valence-variable trinuclear Co cluster compound