Wang Hai-Ling, Ma Xiong-Feng, Peng Jin-Mei, Zhu Zhong-Hong, Li Bo, Zou Hua-Hong, Liang Fu-Pei
State Key Laboratory for Chemistry and Molecular Engineering of Medicinal Resources , School of Chemistry & Pharmacy of Guangxi Normal University , Guilin 541004 , P. R. China.
College of Chemistry and Pharmaceutical Engineering , Nanyang Normal University , Nanyang 473061 , P. R. China.
Inorg Chem. 2019 Jul 15;58(14):9169-9174. doi: 10.1021/acs.inorgchem.9b00760. Epub 2019 Jun 26.
High-nuclear lanthanide clusters are generally formed by the rapid accumulation of simple building units. Thus, tracking and observing the stepwise assembly process, which is vital for understanding the assembly mechanism, are extremely difficult. Herein, the decanuclear nanocluster [Dy(L)(μ-NO)(OAc)(HOAc)]·8HO (, HL = ()-3-((3-ethoxy-2-hydroxybenzylidene)amino)propane-1,2-diol) was obtained from the reaction of Dy(NO)·6HO, Dy(OAc)·6HO, 3-ethoxy-2-hydroxybenzaldehyde (L), and 3-amino-1,2-propanediol (L). The reaction process was further tracked by time-dependent high-resolution electrospray ionization mass spectrometry, and seven reaction intermediate fragments were screened. A stepwise assembly mechanism was observed based on these fragments, that is, L → Dy1 → Dy2 → Dy3 → Dy4 → Dy5 → Dy6 → Dy10. This study is the first to discover a stepwise assembly mechanism during the formation of high-nuclear lanthanide clusters (cluster nucleus > 3). Magnetic studies have shown the multiple relaxation behavior of .
