Generally, two-dimensional concatenation happens on 2D surfaces such as metal surfaces in CVD process or liquid-liquid interfaces in interfacial polymerization. However, such approaches suffer from minuscule synthetic and transfer efficiencies. Another strategy is to introduce microscopic reversibility, to achieve 2D crystals after extensive error correction. As a consequence, resulting materials are associated with low chemical stabilities, which further lead to problematic processabilities. Herein we demonstrate an irreversible 2D polymerization without any external 2D input can be achieved, resulting in covalently bonded 2D polymer platelets that are chemically stable and highly processable. Further fabrication of the product offers highly oriented, free-standing films which exhibit exceptional 2D elastic modulus and yield strength at 50.9±15.0 GPa and 0.976±0.113 GPa, respectively. Individual 2D molecules were found highly asymmetric by chemical AFM and their alignment is evidenced by polarized photoluminescence from different dipole transitions. This new synthetic route provides opportunities for 2D polymers in applications ranging from composite structures to barrier coatings.

Two-dimensional polymerization in a homogenous reaction system: theory and application

ACS Spring Meeting 2021

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