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Significance Bulk CO2 or dry ice has seven polymorphs, namely, CO2 I–VII. Here, we show molecular dynamics simulation evidence of 20+ two-dimensional (2D) CO2 polymorphs and polyamorphs. This remarkable 2D polyamorphism of CO2 and the diverse array of structures is not seen in other molecular systems with weak intermolecular van der Waals (vdW) interactions. Our findings may promote a new research direction for vdW molecular systems, i.e., 2D polymorphism. The rich 2D polymorphic and polyamorphic solid CO2 structures not only enrich our knowledge of the phase behavior of CO2 in slit nanopores, but also have implications to the sequestration of CO2 in microporous materials under high pressure.

Two-dimensional dry ices with rich polymorphic and polyamorphic phase behavior