PMID- 34114807 OWN - NLM STAT- PubMed-not-MEDLINE LR - 20210706 IS - 1520-510X (Electronic) IS - 0020-1669 (Linking) VI - 60 IP - 13 DP - 2021 Jul 5 TI - Influence of the Different Types of Auxiliary Noncarboxylate Organic Ligands on the Topologies and Magnetic Relaxation Behavior of Zn-Dy Heterometallic Single Molecule Magnets. PG - 9941-9955 LID - 10.1021/acs.inorgchem.1c01217 [doi] AB - In this work, we first synthesized a Zn-Dy complex, [Zn(6)Dy(2)(L)(6)(tea)(2)(CH(3)OH)(2)].6CH(3)OH.8H(2)O (H(2)L = N-3-methoxysalicylidene-2-amino-3-hydroxypyridine, teaH(3) = triethanolamine, 1), by employing H(2)L, anhydrous ZnCl(2), and Dy(NO(3))(3).5H(2)O reacting with auxiliary ligand teaH(3) in the mixture of CH(3)OH and DMF. When teaH(3) and the solvent CH(3)OH in the reaction system of 1 were replaced by the auxiliary ligand 2,6-pyridinedimethanol (pdmH(2)) and the solvent MeCN, another Zn-Dy complex, [Zn(4)Dy(4)(L)(6)(pdm)(2)(pdmH)(4)].10CH(3)CN.5H(2)O (2), was obtained. For 1, its crystal structure can be viewed as a dimer of two Zn(3)Dy(III) units. However, for 2, four Dy(III) form a zigzag arrangement, and each of its terminals linked two Zn(II) ions. Interestingly, although the structural topologies of 1 and 2 are different, the coordination geometries of Dy(III) in 1 and 2 are all triangular dodecahedron (TDD-8). The difference is that the continuous shape measure (CShM) values of Dy(III) in 1 are larger than the corresponding values in 2. Magnetic investigation revealed that the diluted sample 1@Y exhibits two magnetic relaxation processes, while 2 only exhibits a single relaxation process. Ab initio calculations indicated that, in the crystal lattice of 1, two complexes exhibiting slightly different CShM values of Dy(III) result in the double relaxation behavior of 1@Y. However, for 2, one of two Dy(III) fragments possesses a fast quantum tunneling of magnetization (QTM), resulting in its magnetic process presented at T < 1.8 K, so 2 exhibits single relaxation behavior. More importantly, the theoretical calculations also clearly indicated that the weak ligation at equatorial sites of Dy(III) in 1 and 2 ensure 1@Y and 2 possess SMM behavior, although the coordination geometry of Dy(III) (TDD-8) in 1 and 2 severely deviates from the ideal polyhedron and its axial symmetry is low. FAU - Wang, Hui-Sheng AU - Wang HS AUID- ORCID: 0000-0002-4502-9996 AD - School of Chemistry and Environmental Engineering, Key Laboratory of Green Chemical Process of Ministry of Education, Key Laboratory of Novel Reactor and Green Chemical Technology of Hubei Province, Wuhan Institute of Technology, Wuhan 430074, P. R. China. FAU - Zhang, Ke AU - Zhang K AD - School of Chemistry and Environmental Engineering, Key Laboratory of Green Chemical Process of Ministry of Education, Key Laboratory of Novel Reactor and Green Chemical Technology of Hubei Province, Wuhan Institute of Technology, Wuhan 430074, P. R. China. FAU - Wang, Jia AU - Wang J AD - State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210046, P. R. China. FAU - Hu, Zhao-Bo AU - Hu ZB AD - State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210046, P. R. China. FAU - Zhang, Zaichao AU - Zhang Z AD - Jiangsu Key Laboratory for the Chemistry of Low-dimensional Materials, School of Chemistry and Chemical Engineering, Huaiyin Normal University, Huai'an 210024, P. R. China. FAU - Song, You AU - Song Y AUID- ORCID: 0000-0002-0289-7830 AD - State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210046, P. R. China. FAU - Zhang, Yi-Quan AU - Zhang YQ AUID- ORCID: 0000-0003-1818-0612 AD - Jiangsu Key Laboratory for NSLSCS, School of Physical Science and Technology, Nanjing Normal University, Nanjing 210023, P. R. China. LA - eng PT - Journal Article DEP - 20210611 PL - United States TA - Inorg Chem JT - Inorganic chemistry JID - 0366543 SB - IM EDAT- 2021/06/12 06:00 MHDA- 2021/06/12 06:01 CRDT- 2021/06/11 12:11 PHST- 2021/06/12 06:00 [pubmed] PHST- 2021/06/12 06:01 [medline] PHST- 2021/06/11 12:11 [entrez] AID - 10.1021/acs.inorgchem.1c01217 [doi] PST - ppublish SO - Inorg Chem. 2021 Jul 5;60(13):9941-9955. doi: 10.1021/acs.inorgchem.1c01217. Epub 2021 Jun 11.