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Abstract
The 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 CO
2
/CH
4
and CO
2
/N
2
. This paper reports on a dense CAU‐10‐H MOF membrane that is exceptionally CO
2
‐selective (ideal selectivity of 42 for CO
2
/N
2
and 95 for CO
2
/CH
4
). The proposed membrane also achieves the highest CO
2
permeability (approximately 500 Barrer) among existing pure MOF membranes with CO
2
/CH
4
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 CO
2
‐selective MOF membranes.