Precision-engineered metal-organic frameworks: fine-tuning reverse topological structure prediction and design

Digital discoveries of metal-organic frameworks (MOFs) have been significantly advanced by the reverse topological approach (RTA). The node-and-linker assembly strategy allows predictable reticulations predefined by in silico coordination templates; however, reticular equivalents lead to substantial combinatorial explosion due to the infinite design space of building units (BUs). Here, we develop a fine-tuned RTA for the structure prediction of MOFs by integrating precise topological constraints and leveraging reticular chemistry, thus transcending traditional exhaustive trial-and-error assembly. From an extensive array of chemically realistic BUs, we subsequently design a database of 94 823 precision-engineered MOFs (PE-MOFs) and further optimize their structures. The PE-MOFs are assessed for post-combustion CO2 capture in the presence of H2O and top-performing candidates are identified by integrating three stability criteria (activation, water and thermal stabilities). This study highlights the potential of synergizing PE with the RTA to enhance efficiency and precision for computational design of MOFs and beyond.