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Adsorptive removal of SO2 from its low‐concentrated gas mixtures is significant to the health and environment. However, the on‐demand discovery of such adsorbents remains a great challenge. Herein, a high‐throughput computational screening for SO2/CO2 separation is performed in an anion‐pillared metal–organic framework (MOF) database. As a proof‐of‐concept, SIFSIX‐7‐Cu, one of the computationally...