摘要:SummaryThe metallic central magnetic axes in high-nucleation clusters with complex structural connections tend to be disorganized and cancel each other out. Therefore, high-nucleation clusters cannot easily exhibit single-molecule magnets (SMMs) behaviors. Herein, we select a triple-core building block (Dy3K2,1) and use linked diamagnetic alkali metal to form an open, spherical, high-nucleation cluster Dy12Na6(3) with SMM behavior. Furthermore, by changing the reaction conditions, Dy6K2(2) formed by linking two Dy3by K(I) is obtained. High-resolution electrospray mass spectrometry of clusters1–3effectively captures the building block Dy3, and clusters1and3and Dy3have high stability even with the increase in ion source energy. To the best of our knowledge, this is the first time that an SMM based on a high-nucleation cluster has been obtained by connecting magnetic primitives via diamagnetic metal ions. Dy12K6is currently the highest nuclear ns-4fheterometallic SMM.Graphical abstractDisplay OmittedHighlights•We synthesized ns-4fcluster-based SMM by using diamagnetic alkali metal connection•Clusters1–3are rare examples of ns-4fheterometallic clusters•Dy12K6is currently the highest nuclear ns-4fheterometallic SMM•HRESI-MS is used to explore the formation of ns-4fhigh-nucleation clustersNanotechnology; Applied sciences; Materials science