Publication date: 11th July 2022
Unraveling the structure and dynamics of formation of covalent and non-covalent organic based 2D crystalline materials is key to control the quality of these materials, i.e. the defect density, and their size. These characteristics are important to understand and control their properties. In this contribution, our efforts on the use of scanning probe microscopy, and in particular scanning tunneling microscopy (STM), to visualize the structure and the dynamics of formation of substrate-supported metal organic frameworks (sMOF) and substrate-supported covalent organic frameworks (sCOF), at the liquid-solid interface, are highlighted.
It is shown that the quality of monolayer metal organic frameworks (MOF) depends critically on the solvent mixture. Moreover, using chiral solvents, homochiral lattices can be formed, in case of the metal containing supramolecular networks, while no chiral induction is observed in absence of the metal ion.
Covalent organic frameworks are formed based on boroxine chemistry. We report on a model boroxine 2D dynamic covalent polymer, and unveil both qualitative and quantitative details of the nucleation–elongation processes in real time and under ambient conditions. Sequential data analysis enable observation of the amorphous-to-crystalline transition, the time-dependent evolution of nuclei, the existence of ‘non-classical’ crystallization pathways and, importantly, the experimental determination of essential crystallization parameters with excellent accuracy, including critical nucleus size, nucleation rate and growth rate. In addition, we show that in specific cases, the electric field between the STM tip and the substrate can induce, on demand, the polymerization or depolymerization process.
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