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The graphdiyne family has attracted a high degree of concern because of its intriguing and promising properties. However, graphdiyne materials reported to date represent only a tiny fraction of the possible combinations. In this work, we demonstrate a computational approach to generate a series of conceivable graphdiyne-based frameworks (GDY-Rs and Li@GDY-Rs) by introducing a variety of functional groups (R = -NH, -OH, -COOH, and -F) and doping metal (Li) in the molecular building blocks of graphdiyne without restriction of experimental conditions and rapidly screen the best candidates for the application of CO capture and sequestration (CCS). The pore topology and morphology and CO adsorption and separation properties of these frameworks are systematically investigated by combining density functional theory (DFT) and grand canonical Monte Carlo (GCMC) simulations. On the basis of our computer simulations, combining Li-doping and hydroxyl groups strategies offer an unexpected synergistic effect for efficient CO capture with an extremely CO uptake of 4.83 mmol/g at 298 K and 1 bar. Combined with its superior selectivity (13 at 298 K and 1 bar) for CO over CH, Li@GDY-OH is verified to be one of the most promising materials for CO capture and separation.

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