Abstract:
The study of the structures, applications, and structure-property relationships of atomically precise metal nanoclusters relies heavily on their controlled synthesis. Although great progress has been made in the controlled synthesis of Group 11 (Cu, Ag, Au) metal nanoclusters, the preparation of Pd nanoclusters remains a grand challenge. Herein, a new, simple, and versatile synthetic strategy for the controlled synthesis of Pd nanoclusters is reported with tailorable structures and functions. The synthesis strategy involves the controllable transformations of Pd4(CO)4(CH3COO)4 in air, allowing the discovery of a family of Pd nanoclusters with well-defined structure and high yield. For example, by treating the Pd4(CO)4(CH3COO)4 with 2,2-dipyridine ligands, two clusters of Pd4 and Pd10 whose metal framework describes the growth of vertex-sharing tetrahedra have been selectively isolated. Interestingly, chiral Pd4 nanoclusters can be gained by virtue of customized chiral pyridine-imine ligands, thus representing a pioneering example to shed light on the hierarchical chiral nanostructures of Pd. This synthetic methodology also tolerates a wide variety of ligands and affords phosphine-ligated Pd nanoclusters in a simple way. It is believed that the successful exploration of the synthetic strategy would simulate the research enthusiasm on both the synthesis and application of atomically precise Pd nanoclusters.
摘要:
对结构的研究,应用程序,原子精确的金属纳米团簇的结构-性质关系在很大程度上依赖于它们的受控合成。尽管在第11组(Cu,Ag,Au)金属纳米团簇,Pd纳米团簇的制备仍然是一个巨大的挑战。在这里,一个新的,简单,据报道,控制合成Pd纳米团簇的通用合成策略具有可调整的结构和功能。合成策略涉及空气中Pd4(CO)4(CH3COO)4的可控转化,允许发现具有明确结构和高产率的Pd纳米团簇家族。例如,通过用2,2-二吡啶配体处理Pd4(CO)4(CH3COO)4,已选择性地分离了两个Pd4和Pd10簇,其金属框架描述了共享顶点的四面体的生长。有趣的是,手性Pd4纳米簇可以通过定制的手性吡啶-亚胺配体,因此代表了一个开创性的例子,揭示了Pd的分层手性纳米结构。该合成方法还容许各种各样的配体,并且以简单的方式提供膦连接的Pd纳米团簇。相信合成策略的成功探索将模拟原子精确Pd纳米簇的合成和应用的研究热情。