Observing polymerization in 2D dynamic covalent polymers

Gaolei Zhan, Zhen-Feng Cai (), Karol Strutyński, Lihua Yu, Niklas Herrmann, Marta Martínez-Abadía, Manuel Melle-Franco, Aurelio Mateo-Alonso and Steven De Feyter ()
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Gaolei Zhan: KU Leuven
Zhen-Feng Cai: KU Leuven
Karol Strutyński: University of Aveiro
Lihua Yu: KU Leuven
Niklas Herrmann: KU Leuven
Marta Martínez-Abadía: University of the Basque Country UPV/EHU
Manuel Melle-Franco: University of Aveiro
Aurelio Mateo-Alonso: University of the Basque Country UPV/EHU
Steven De Feyter: KU Leuven

Nature, 2022, vol. 603, issue 7903, 835-840

Abstract: Abstract The quality of crystalline two-dimensional (2D) polymers1–6 is intimately related to the elusive polymerization and crystallization processes. Understanding the mechanism of such processes at the (sub)molecular level is crucial to improve predictive synthesis and to tailor material properties for applications in catalysis7–10 and (opto)electronics11,12, among others13–18. We characterize a model boroxine 2D dynamic covalent polymer, by using in situ scanning tunnelling microscopy, to unveil both qualitative and quantitative details of the nucleation–elongation processes in real time and under ambient conditions. Sequential data analysis enables 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. The experimental data have been further rationalized by atomistic computer models, which, taken together, provide a detailed picture of the dynamic on-surface polymerization process. Furthermore, we show how 2D crystal growth can be affected by abnormal grain growth. This finding provides support for the use of abnormal grain growth (a typical phenomenon in metallic and ceramic systems) to convert a polycrystalline structure into a single crystal in organic and 2D material systems.

Date: 2022
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DOI: 10.1038/s41586-022-04409-6

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