Solutions Are the Problem: Ordered Two-Dimensional Covalent Organic Framework Films by Chemical Vapor Deposition

材料科学 化学气相沉积 X射线光电子能谱 化学工程 薄膜 拉曼光谱 结晶度 聚合物 微晶 纳米技术 复合材料 光学 物理 工程类 冶金
作者
Jeremy P. Daum,Alec Ajnsztajn,Sathvik Ajay Iyengar,Jacob H. Lowenstein,Soumyabrata Roy,Guanhui Gao,Esther H. R. Tsai,Pulickel M. Ajayan,Rafael Verduzco
出处
期刊:ACS Nano [American Chemical Society]
卷期号:17 (21): 21411-21419 被引量:21
标识
DOI:10.1021/acsnano.3c06142
摘要

Covalent organic frameworks (COFs) are a promising class of crystalline polymer networks that are useful due to their high porosity, versatile functionality, and tunable architecture. Conventional solution-based methods of producing COFs are marred by slow reactions that produce powders that are difficult to process into adaptable form factors for functional applications, and there is a need for facile and fast synthesis techniques for making crystalline and ordered covalent organic framework (COF) thin films. In this work, we report a chemical vapor deposition (CVD) approach utilizing co-evaporation of two monomers onto a heated substrate to produce highly crystalline, defect-free COF films and coatings with hydrazone, imine, and ketoenamine COF linkages. This all-in-one synthesis technique produces highly crystalline, 40 nm-1 μm-thick COF films on Si/SiO2 substrates in less than 30 min. Crystallinity and alignment were proven by using a combination of grazing-incidence wide-angle X-ray scattering (GIWAXS) and transmission electron microscopy (TEM), and successful conversion of the monomers to produce the target COF was supported by Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), and UV-vis measurements. Additionally, we used atomic force microscopy (AFM) to investigate the growth mechanisms of these films, showing the coalescence of triangular crystallites into a smooth film. To show the wide applicability and scope of the CVD process, we also prepared crystalline ordered COF films with imine and ketoenamine linkages. These films show potential as high-quality size exclusion membranes, catalytic platforms, and organic transistors.
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