“…As emerging porous solid materials, metal–organic frameworks (MOFs) have obvious advantages over zeolite, activated carbon, silica gel, and other traditional adsorbents, owing to their high porosity, adjustable pore sizes/shapes, and easily functionalized internal pore surface. − It is expected to achieve efficient separation between mixtures with slight differences such as C 2 H 2 /CO 2 . Researchers have reported various MOFs for C 2 H 2 /CO 2 separation recently, − where major efforts have been made to adjust the 3D framework to generate appropriate pore space, for instance, introducing open metal sites, ,, introducing polar functional groups, − constructing hydrogen bonding nanotraps, pore space partition strategies, , constructing interpenetration structures, ligand derivatization, ,,, partial linker substitution strategy, induced-fit transformation strategy, etc. Significant progress has been made by these contributions, but the design of C 2 H 2 selective adsorbents that combines high adsorption capacity with high selectivity remains a challenge. ,,,, Layered 2D MOFs are a class of MOFs with 2D infinite extension networks, which have no rigid chemical bonds between layers compared with traditional porous materials and 3D MOFs.…”