by Andrea Darù; Jianheng Ling; Xiaoliang Wang; Julian S. Magdalenski; Haomiao Xie; Omar K. Farha; Massimiliano Delferro; John S. Anderson and Laura Gagliardi
We report an end-to-end computational-experimental workflow for the discovery of metal–organic frameworks (MOFs), demonstrated by the computational design and synthesis of two novel Zn-based frameworks, UCHI-1 and UCHI-2, exhibiting enhanced methane uptake and selectivity at low pressure under ambient conditions (298 K, 1 bar). The workflow enables the rational selection and experimental realization of metal–organic frameworks combining data mining, machine-learning driven adsorption prediction, and structure generation, with experimental synthesis and validation within a closed-loop discovery pipeline. Analysis of existing and newly generated MOFs reveals the structure–property relationships governing low-pressure methane adsorption, identifying an optimal pore size and shape, framework densities, linker functionalities, and framework topologies that maximize dispersive C–H/π and van der Waals interactions. Beyond the specific materials identified herein, the results establish this workflow as a scalable and extensible platform for accelerated MOF discovery, with clear routes toward further optimization and automation while demonstrating practical applicability beyond purely theoretical exploration of hypothetical materials.