“…Therefore, the development of efficient sorbents for CO 2 capture is not only vital for environmental protection but also important for the development of a CO 2 circular economy, which involves the further utilization of captured CO 2 as a sustainable chemical commodity . In this direction, porous organic polymers (POPs) have been considered as promising alternatives for CO 2 capture and separation because of their structural tunability, high porosity, and chemical stability. − Moreover, POPs have also found applications in atmospheric water capture, semiconducting materials, heterogeneous catalysis, precious metal recovery, water purification, iodine (I 2 ) capture, and many others. , The structural tunability of POPs allows one to control the nature of chemical functionalities by choosing suitable precursors. − The porosity and pore size of POPs, on the other hand, are determined by the length, dimensions, and rigidity of the building block as well as the degree of interpenetration of the polymer backbone . Hence, the ability to control the porosity, especially in three-dimensional (3D) POPs, is essential for the design of new polymers with the desired porosity for target applications.…”