The unique geometry and novel properties of graphene have tremendously motivated scientists to explore other monolayer materials, especially those with separately distributed and exposed metal ions for magnetism, hydrogen storage, CO2 capture and catalysis. The recent successful synthesis of 2D organometallic sheets has opened a new pathway to design and fabricate such desirable 2D materials going beyond graphene and other inorganic sheets.

This article briefly reviews the recent advances in computational studies of 2D organometallic sheets based on density functional theory, quantum chemistry modeling and Monte Carlo simulation focusing on stability, magnetic coupling, magnetism tuning, hydrogen storage, CO2 capture and catalysis. Future research directions in this field are also discussed.

This paper was originally published in Computational Materials 112, Part B, (2016) 492–502.