Chiou D.-S.Yu H.J.Hung T.-H.Lyu Q.Chang C.-K.Lee J.S.Lin L.-C.DUN-YEN KANGLI-CHIANG LIN2022-05-242022-05-242021https://www.scopus.com/inward/record.uri?eid=2-s2.0-85092153844&doi=10.1002%2fadfm.202006924&partnerID=40&md5=41a0bf07cb68eac06d22010b75ddd82ehttps://scholars.lib.ntu.edu.tw/handle/123456789/611457The topology and chemical functionality of metal–organic frameworks (MOFs) make them promising candidates for membrane gas separation; however, few meet the criteria for industrial applications, that is, selectivity of >30?for CO2/CH4 and CO2/N2. This paper reports on a dense CAU-10-H MOF membrane that is exceptionally CO2-selective (ideal selectivity of 42 for CO2/N2 and 95 for CO2/CH4). The proposed membrane also achieves the highest CO2 permeability (approximately 500 Barrer) among existing pure MOF membranes with CO2/CH4 selectivity exceeding 30. State-of-the-art atomistic simulations provide valuable insights into the outstanding separation performance of CAU-10-H at the molecular level. Adsorbent–adsorbate Coulombic interactions are identified as a crucial factor in the design of CO2-selective MOF membranes. ? 2020 Wiley-VCH GmbHCarbon dioxideAtomistic simulationsChemical functionalityCoulombic effectsCoulombic interactionsIdeal selectivitiesMolecular levelsSeparation performanceState of the artGas permeable membranes[SDGs]SDG13journal article10.1002/adfm.2020069242-s2.0-85092153844