In Situ Encapsulation of Atomically Precise Nanoclusters in Reticular Frameworks via Mechanochemical Synthesis

IF 27.4 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2024-10-30 DOI:10.1002/adma.202412768

Yi-Ming Li, Dongxia Shi, Jian Yuan, Rui-Min Zuo, Hui Yang, Jinhui Hu, Shu-Xian Hu, Hongting Sheng, Manzhou Zhu

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Abstract

The combination of atomically precise nanoclusters (APNCs) and reticular frameworks is promising for generating component-specific nanocomposites with emergent properties. However, traditional liquid-phase synthesis often hampers this potential by damaging APNCs and limiting combination diversity. Here, mechanochemical synthesis to explore the encapsulation of diverse oil- and water-soluble APNCs within various reticular frameworks is employed, establishing a database of 21 unique APNC−framework combinations, including metal−organic frameworks (MOFs), covalent−organic frameworks (COFs), hydrogen−bonded organic frameworks (HOFs), and multivariate MOFs. These framework coatings not only spatially immobilize APNCs but also secure their structures, preventing aggregation and degradation while enhancing stability and activity. Encapsulating Au₂₅ in HOFs resulted in a remarkable 315-fold increase in catalytic activity compared to Au₂₅ homogeneous catalyst, highlighting the framework's crucial role in catalytic enhancement. The mechanochemical synthesis strategy facilitates tailored support screening, catering to specific needs, and shows promise for developing multifunctional systems, including enzyme−APNC@frameworks material for cascade reactions.

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通过机械化学合成将原子精度的纳米团簇原位封装在网状框架中

原子精密纳米团簇（APNC）与网状框架的结合有望产生具有新特性的特定成分纳米复合材料。然而，传统的液相合成往往会破坏 APNCs 并限制组合的多样性，从而阻碍这一潜力的发挥。在这里，我们采用机械化学合成的方法，探索在各种网状框架内封装不同的油溶性和水溶性 APNC 的方法，建立了一个包含 21 种独特 APNC 框架组合的数据库，其中包括金属有机框架 (MOF)、共价有机框架 (COF)、氢键有机框架 (HOF) 和多元 MOF。这些框架涂层不仅能在空间上固定 APNC，还能固定其结构，防止聚集和降解，同时提高稳定性和活性。与 Au25 均相催化剂相比，将 Au25 封装在 HOFs 中使其催化活性显著提高了 315 倍，突出了框架在催化增强中的关键作用。这种机械化学合成策略有助于筛选定制的支持物，满足特定需求，并有望开发出多功能系统，包括用于级联反应的酶-APNC@框架材料。

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.