Porous Carbon Materials Based on Graphdiyne Basis Units by the Incorporation of the Functional Groups and Li Atoms for Superior CO2 Capture and Sequestration

5 years ago

Porous Carbon Materials Based on Graphdiyne Basis Units by the Incorporation of the Functional Groups and Li Atoms for Superior CO2 Capture and Sequestration

Wenyue Guo, Lianming Zhao, Yong Dang, Houyu Zhu

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 = −NH₂, −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 CO₂ capture and sequestration (CCS). The pore topology and morphology and CO₂ 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 CO₂ capture with an extremely CO₂ 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 CO₂ over CH₄, Li@GDY-OH is verified to be one of the most promising materials for CO₂ capture and separation.

Publisher URL: http://dx.doi.org/10.1021/acsami.7b10836

DOI: 10.1021/acsami.7b10836