Tailoring a MOF ‐based adsorbent with partitioned aliphatic pore spaces for efficient CH4 purification from natural gas

Abstract Separation of CH4 from natural gas is an essential but extremely challenging process in the petrochemical industry. Here, we tailored a MOF‐based adsorbent with partitioned aliphatic pore spaces through the simultaneous incorporation of the aliphatic sites and the symmetrically matched partition agent. The resulting adsorbent demonstrates exceptional adsorption capacity for C3H8 and C2H6 compared to CH4, along with remarkably competitive adsorption selectivities for C3H8/CH4 and C2H6/CH4. Breakthrough experiments further support the excellent dynamic separation efficiency of the adsorbent for the purification of CH4 from natural gas. Moreover, detailed density functional theory calculations and molecular simulations elucidate the synergistic interactions between the aliphatic sites and the partitioned pore spaces within the adsorbent, which promote the stronger binding affinities for C3H8 and C2H6 over CH4.