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New Progress in the Field of Spherical Lanthanide Cluster Assembly and Magnetic Exchange “Fingerprints” by a Team Led by Prof. Yan-Zhen Zheng
Hits:    Update:2017/11/3 08:21:33


The creation of a perfect hollow nanoscopic sphere of metal centres is clearly an unrealisable synthetic challenge. It is however an inspirational challenge, from the viewpoint of chemical architecture and also as finite molecular species may provide unique microscopic insight into the origin and onset of phenomena such as topological spin-frustration effects found in infinite 2D and 3D systems.
Recently, under the guidance of Professor Yan-Zhen Zheng in Xi'an Jiaotong University, postgraduate students Lei Qin and Guo-Jun Zhou successfully synthesized four spherical Gd(III)-based clusters and two intermediates based on the controlled hydrolysis methods in solution chemistry and solvothermal reactions. The core structures of the four spherical clusters have high symmetry, and their size increases from 1.2 nm to 2.0 nm with the increase of the nuclearity. The topological analysis indicates that these four spherical clusters are constructed by triangle, square, pentagon and hexagon secondary building units through vertex-, edge- and face-sharing modes. Structural analysis reveals the Gd20 cage resembles a dodecahedron; the vertices of the Gd32 polyhedron exactly reveal symmetry Oh; Gd50 displays an unprecedented polyhedron in which an icosidodecahedron Gd30 core is encapsulated by an outer Gd20 dodecahedral shell with approximate Ih symmetry; and the Gd60 shows a truncated octahedron geometry. Experimental and theoretical magnetic studies show that this series produces the expected antiferromagnetic interaction that can be modelled based on classical spins at the Gd sites. From the magnetization analyses we can roughly correlate the derivative bands to the Gd-O-Gd angles with the equation J = 0.0072φ−0.85245 (cm−1). Moreover, the different systems are correlated to distinct magnetization differential curve. Such a magneto-structural correlation may be used as “fingerprints” to identify these cages.
This work was collaborated with Prof. C. Schrö der (Bielefeld University, Germany), Prof. H. Nojiri (Tohoku University) and Prof. R. E. P. Winpenny (University of Manchester) and supported by the key international joint project of NSFC (Grant No. 21620102002 ), “National 1000 Young Talents” program, Wuhan National High Magnetic Field Center (2015KF06), the Cyrus Chung Ying Tang Foundation and Fundamental Research Funds for the Central University. The related paper was published in the international authoritative journal Journal of the American Chemical Society ( IF = 13.86), entitled as “ Topological Self-Assembly of Highly-Symmetric Lanthanide Clusters: A Magnetic Study of Exchange-Coupling Fingerprints in Giant Gadolinium(III) Cages ”.Link: http://pubs.acs.org/doi/10.1021/jacs.7b09996
Prof. Yan-Zhen Zheng is the vice dean of Frontier Institute of Science and Technology (FIST), Young Top-Notch Talent (A level), Young Scholars of the Cyrus Chung Ying Tang. Research interests: coordination chemistry, organometallics, functional metal clusters, molecular magnets, molecular conductors, magnetoelectric coupling, photoelectric effect, etc. Students from relevant departments and majors are strongly welcomed for further contact.           

Center for Applied Chemical Research (CACR) link:http://fist.xjtu.edu.cn/center/CACR/

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