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Atomic-Layer Deposition into 2- versus 3-Dimensionally Ordered Nanoporous Media: Pore Size or Connectivity?
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-06-27 00:00:00 , DOI: 10.1021/acs.chemmater.8b01615 Changdeuck Bae 1 , Hyunchul Kim 1 , Eunsoo Kim 1 , Hyung Gyu Park 2 , Hyunjung Shin 1
Chemistry of Materials ( IF 7.2 ) Pub Date : 2018-06-27 00:00:00 , DOI: 10.1021/acs.chemmater.8b01615 Changdeuck Bae 1 , Hyunchul Kim 1 , Eunsoo Kim 1 , Hyung Gyu Park 2 , Hyunjung Shin 1
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Atomic-layer deposition (ALD) is now being recognized as a powerful, general tool for modifying the surfaces of nanomaterials in applications for many energy conversion devices. However, ALD involves slow processes particularly when it is subjected to nanoporous media with high-aspect ratios. Predicting the exact experimental conditions of the desired reactions for coating inside deep pores by ALD is not available because of the lack of complete understanding of diffusion in nanoporous media. Here, we report a comparative study of the ALD coating onto two distinctive templates having nanopores, i.e., 2- and 3-dimensionally ordered media (DOM), of similar porosity and pore dimension. Self-supporting, crack-free templates were carefully prepared in centimeters for both 2- and 3-DOM and thus avoid any possible sources of uncontrollable diffusion of precursor gas molecules through unwanted microvoids and cracks. Comparison of the ALD coating profiles across the thickness of both templates reveals a fundamentally distinct coating mechanism. While a uniform growth zone develops along the pores of the 2-DOM (i.e., 1-D diffusion path), a gradual decrease in the deposition is observed in those of the 3-DOM (i.e., 3-D diffusion path) as ALD pulse time increases. This observation suggests an essential role of the pore connectivity, rather than individual pore sizes, in the gas diffusion dynamics inside nanoporous media. The present model can universally predict the ALD behaviors in nanoporous media even with different types of pore connectivity.
中文翻译：
将原子层沉积到2维或3维有序纳米多孔介质中：孔径或连通性？
如今，原子层沉积（ALD）被认为是一种功能强大的通用工具，用于在许多能量转换设备的应用中修饰纳米材料的表面。然而，ALD涉及缓慢的过程，特别是当其以高纵横比的纳米多孔介质处理时。由于缺乏对纳米孔介质中扩散的完全了解，因此无法通过ALD预测深孔内包衣所需反应的确切实验条件。在这里，我们报告了在两个具有纳米孔的独特模板上的ALD涂层的比较研究，这些纳米孔即具有相似孔隙率和孔径的二维和3维有序介质（DOM）。自给自足，精心准备了以厘米为单位的2-DOM和3-DOM的无裂纹模板，从而避免了前驱气体分子通过有害的微孔和裂纹扩散的任何可能来源。横跨两个模板厚度的ALD涂层轮廓的比较揭示了根本不同的涂层机理。虽然沿着2-DOM（即1-D扩散路径）的孔形成了均匀的生长区，但是在3-DOM（即3-D扩散路径）的沉积中，沉积沉积逐渐减少，这是因为ALD脉冲时间增加。该观察结果表明，在纳米孔介质内部的气体扩散动力学中，孔连通性而不是单个孔的大小起着至关重要的作用。本模型可以普遍预测纳米多孔介质中的ALD行为，即使具有不同类型的孔连通性也是如此。
更新日期：2018-06-27
中文翻译：
将原子层沉积到2维或3维有序纳米多孔介质中：孔径或连通性？
如今，原子层沉积（ALD）被认为是一种功能强大的通用工具，用于在许多能量转换设备的应用中修饰纳米材料的表面。然而，ALD涉及缓慢的过程，特别是当其以高纵横比的纳米多孔介质处理时。由于缺乏对纳米孔介质中扩散的完全了解，因此无法通过ALD预测深孔内包衣所需反应的确切实验条件。在这里，我们报告了在两个具有纳米孔的独特模板上的ALD涂层的比较研究，这些纳米孔即具有相似孔隙率和孔径的二维和3维有序介质（DOM）。自给自足，精心准备了以厘米为单位的2-DOM和3-DOM的无裂纹模板，从而避免了前驱气体分子通过有害的微孔和裂纹扩散的任何可能来源。横跨两个模板厚度的ALD涂层轮廓的比较揭示了根本不同的涂层机理。虽然沿着2-DOM（即1-D扩散路径）的孔形成了均匀的生长区，但是在3-DOM（即3-D扩散路径）的沉积中，沉积沉积逐渐减少，这是因为ALD脉冲时间增加。该观察结果表明，在纳米孔介质内部的气体扩散动力学中，孔连通性而不是单个孔的大小起着至关重要的作用。本模型可以普遍预测纳米多孔介质中的ALD行为，即使具有不同类型的孔连通性也是如此。
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