论文标题
在形成金属有机框架薄膜期间,时间分辨的原位液相原子力显微镜和红外纳米光谱
Time-Resolved In Situ Liquid-Phase Atomic Force Microscopy and Infrared Nanospectroscopy during the Formation of Metal-Organic Framework Thin Films
论文作者
论文摘要
金属有机框架(MOF)薄膜表现出无与伦比的承诺,如智能膜和照片催化涂层。但是,它们由复杂的分子组装过程产生的成核和生长尚不清楚,但对于控制薄膜特性至关重要。在这里,我们直接观察到Cu-BTC溶液中不同温度下实时的原位AFM观察到HKUST-1薄膜的成核和生长行为。结合前坐骨红外(纳米)光谱,在25°C下的合成显示了迅速生长的Hkust-1岛的初始成核,这些岛屿被连续成核但慢慢生长的HKUST-1地毯包围。在13°C和50°C下进行监测显示温度对薄膜形成的强烈影响,从而导致(部分)成核和生长抑制。成核和生长机制及其动力学提供了见解,以帮助MOF薄膜的未来理性设计。
Metal-organic framework (MOF) thin-films show unmatched promise as smart membranes and photo-catalytic coatings. However, their nucleation and growth resulting from intricate molecular assembly processes are not well understood, yet crucial to control the thin-film properties. Here, we directly observe the nucleation and growth behaviour of HKUST-1 thin-films by real-time in-situ AFM at different temperatures in the Cu-BTC solution. In combination with ex-situ infrared (nano-)spectroscopy, synthesis at 25°C reveals initial nucleation of rapidly growing HKUST-1 islands surrounded by a continuously nucleating, but slowly growing HKUST-1 carpet. Monitoring at 13°C and 50°C shows the strong impact of temperature on thin-film formation, resulting in (partial) nucleation and growth inhibition. The nucleation and growth mechanisms as well as their kinetics provide insights to aid in future rational design of MOF thin-films.