Discovery of anion‐pillared metal–organic frameworks for efficient SO2 / CO2 separation via computational screening

Abstract 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 top‐ranked MOFs, is identified and experimentally synthesized for the verification. The high SO2 uptake (14.7 mmol g−1), IAST selectivity (120 for a mixture of 0.2/99.8 molar ratio), and excellent balance between the regenerability (63.5%) and adsorbent performance score (36.3) make it superior to the performance of most reported adsorbents. This work not only provides an excellent candidate for SO2/CO2 separation, but also will facilitate the development of theoretical prediction‐experimental verification methodology in the discovery of novel materials.