Nanocluster superstructures assembled via surface ligand switching at high temperature
Nanocluster superstructures assembled via surface ligand switching at high temperature
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DOI：
10.1038/s44160-023-00304-8
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发表时间：
2023-05
期刊：
影响因子：
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通讯作者：
Grayson Johnson;M. Yang;Chang Liu;Hua Zhou;X. Zuo;D. Dickie;Sihan Wang;Wenpei Gao;Bukuru Anaclet-B
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文献类型：
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作者：
Grayson Johnson;M. Yang;Chang Liu;Hua Zhou;X. Zuo;D. Dickie;Sihan Wang;Wenpei Gao;Bukuru Anaclet-B
具有纳米级构建块的超级结构，当与组成单元的精确控制相结合时，为合理设计和制造所需的功能材料提供了机会。然而，用于大规模生产超结构的合成策略是稀缺的。我们报告了一个可扩展的和通用的方法来合成组装从原子精确的Ce24O28（OH）8和其他稀土金属氧化物纳米团簇的自组装机制的详细描述旁边的超结构。结合操作小角X射线散射，非原位分子和结构表征，和分子动力学模拟表明，高温配体开关机制，从油酸酯到苯甲酸酯，支配的纳米团簇组装的形成。表面配体的化学调节控制超结构的分解和重新组装，并且进一步地，使多组分超结构的合成成为可能。这种合成方法和准确的机理理解，是有希望的制备用于电子学，等离子体，磁学和催化的超结构。
Superstructures with nanoscale building blocks, when coupled with precise control of the constituent units, open opportunities in rationally designing and manufacturing desired functional materials. Yet, synthetic strategies for the large-scale production of superstructures are scarce. We report a scalable and generalized approach to synthesizing superstructures assembled from atomically precise Ce24O28(OH)8and other rare-earth metal-oxide nanoclusters alongside a detailed description of the self-assembly mechanism. Combining operando small-angle X-ray scattering, ex situ molecular and structural characterizations, and molecular dynamics simulations indicates that a high-temperature ligand-switching mechanism, from oleate to benzoate, governs the formation of the nanocluster assembly. The chemical tuning of surface ligands controls superstructure disassembly and reassembly, and furthermore, enables the synthesis of multicomponent superstructures. This synthetic approach, and the accurate mechanistic understanding, are promising for the preparation of superstructures for use in electronics, plasmonics, magnetics and catalysis.