Nanoscale molecular materials obtained from building-block methods have flourished in recent years and have stimulated further efforts to more challenging systems. Employing building blocks to assemble atomically precise giant clusters is one of the most striking fields but is quite challenging. Here, we report the synthesis of two giant lanthanide-transition metal clusters, Ln₆₈Ni₉₀ and Ln₇₆Ni₈₈, by combining the identification of building blocks through data analysis, the determination of their formation conditions by high-resolution mass spectrometry, and the design of new structures based on topological analysis. Compared with established one-pot methods, synthesizing the building blocks separately provides extra evolution chances for the building blocks and facilitates efficient synthesis. In particular, this study focused on challenging giant heterometallic systems, and the clusters set a new nuclearity record. These results demonstrate the design-driven synthesis of hydroxide clusters from their building blocks and might advance the directed synthesis of giant clusters.

近年来，通过构建模块方法获得的纳米级分子材料蓬勃发展，并刺激了对更具挑战性的系统的进一步努力。使用构建基块来组装原子精确的巨型星团是最引人注目的领域之一，但是却极具挑战性。在这里，我们报告了两个巨型镧系元素过渡金属簇Ln ₆₈ Ni ₉₀和Ln ₇₆ Ni ₈₈的合成，结合了通过数据分析识别积木，通过高分辨率质谱确定其形成条件以及基于拓扑分析设计新结构的方法。与已建立的一锅法相比，分别合成构件为构件提供了更多的进化机会，并促进了有效的合成。尤其是，这项研究的重点是具有挑战性的巨型异金属系统，并且这些团簇创造了新的核记录。这些结果证明了设计驱动的氢氧化物簇团簇的合成，可能会促进巨型簇团的定向合成。