Framework-templated gas lattices in metal-organic frameworks

A gas lattice is a crystalline-like arrangement of adsorbates stabilized inside a porous host by confinement and periodic binding, providing a structurally defined adsorption state that links uptake and transport. Here, we present an end-to-end pipeline to discover and design framework-templated gas lattices in metal-organic frameworks (MOFs) using Xenon as a proof-of-concept guest. High-throughput screening with a lattice-aware descriptor identified Co-CAU-36 as a host that stabilizes a pore-spanning Xenon lattice, while isotherm analysis resolved shell formation, pore filling, and cooperative lattice establishment under application-relevant conditions. In Xenon/Krypton mixtures, Co-CAU-36 exhibited strong pore-scale core-shell segregation, and NEB calculations indicated a low-barrier core diffusion pathway for Krypton, implying separation relevance. Finally, ML-guided genetic optimization over a pillared-MOF space yielded candidates with Xenon lattice signatures. Here, we show that framework-templated gas lattices constitute a distinct adsorbed phase, characterized by long-range periodic order, collective transport pathways, and non-additive mixture behavior.