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Building high-coverage monolayers of covalently bound magnetic nanoparticles

机译：构建共价键合的磁性纳米粒子的高覆盖率单层

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摘要

This work presents an approach for producing a high-coverage single monolayer of magnetic nanoparticles using "click chemistry" between complementarily functionalized nanoparticles and a flat substrate. This method highlights essential aspects of the functionalization scheme for substrate surface and nanoparticles to produce exceptionally high surface coverage without sacrificing selectivity or control over the layer produced. The deposition of one single layer of magnetic particles without agglomeration, over a large area, with a nearly 100% coverage is confirmed by electron microscopy. Spectroscopic techniques, supplemented by computational predictions, are used to interrogate the chemistry of the attachment and to confirm covalent binding, rather than attachment through self-assembly or weak van der Waals bonding. Density functional theory calculations for the surface intermediate of this copper-catalyzed process provide mechanistic insight into the effects of the functionalization scheme on surface coverage. Based on this analysis, it appears that steric limitations of the intermediate structure affect nanoparticle coverage on a flat solid substrate; however, this can be overcome by designing a functionalization scheme in such a way that the copper-based intermediate is formed on the spherical nanoparticles instead. This observation can be carried over to other approaches for creating highly controlled single or multilayered nanostructures of a wide range of materials to result in high coverage and possibly, conformal filling. (C) 2015 Elsevier B.V. All rights reserved.
机译：这项工作提出了一种利用互补功能化的纳米颗粒和平坦基材之间的“点击化学”来生产磁性纳米颗粒的高覆盖率单层方法。该方法突出了用于基材表面和纳米颗粒的功能化方案的基本方面，以产生异常高的表面覆盖率，而不会牺牲选择性或对所生产层的控制。通过电子显微镜确认了在没有附聚的情况下在大面积上以几乎100％的覆盖率沉积了一层单层的磁性粒子。光谱技术，再加上计算预测，可用于检验连接的化学性质并确认共价结合，而不是通过自组装或弱范德华键进行连接。此铜催化过程的表面中间体的密度泛函理论计算可提供有关功能化方案对表面覆盖率影响的机械原理。基于该分析，似乎中间结构的空间限制会影响纳米颗粒在平坦的固体基材上的覆盖率。然而，这可以通过设计一种功能化方案来克服，该方案使铜基中间体代替地在球形纳米颗粒上形成。可以将此观察结果延续到其他方法中，以创建可控制范围很广的材料的单个或多层纳米结构，以实现高覆盖率和可能的保形填充。 （C）2015 Elsevier B.V.保留所有权利。

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