Highly Efficient CO₂/C₂H₂ Separation by Porous Graphene via Quadrupole Gating Mechanism

Acetylene (C₂H₂) is an important and widely used raw material in various industries (such as petrochemical). Generally, a product yield is proportional to the purity of C₂H₂; however, C₂H₂ from a typical industrial gas-production process is commonly contaminated by CO₂. So far, the achievement of high-purity C₂H₂ separated from a CO₂/C₂H₂ mixture is still challenging due to their very close molecular dimensions and boiling temperatures. Taking advantage of their quadrupoles with opposite signs, here, we show that the graphene membrane embedded with crown ether nanopores can achieve an unprecedented separation efficiency of CO₂/C₂H₂. Combining the molecular dynamics simulation and the density functional theory (DFT) approaches, we discovered that the electrostatic gas-pore interaction favorably allows the fast transport of CO₂ through crown ether nanopores while completely prohibiting C₂H₂ transport, which yields a remarkable permeation selectivity. In particular, the utilized crown ether pore is capable of allowing the individual transport of CO₂ while completely rejecting the passage of C₂H₂, independent of the applied pressures, fed gases ratios, and exerted temperatures, featuring the superiority and robustness of the crown pore in CO₂/C₂H₂ separation. Further, DFT and PMF calculations demonstrate that the transport of CO₂ through the crown pore is energetically more favorable than the transport of C₂H₂. Our findings reveal the potential application of graphene crown pore for CO₂ separation with outstanding performance.