Mesoporous Zn4O(−COO)6-based metal–organic frameworks (MOFs), including UMCM-1, MOF-205, MUF-7a, and the newly synthesized MOFs, termed ST-1, ST-2, ST-3, and ST-4 (ST = ShanghaiTech University), have been systematically investigated for ultrahigh capacity methane storage. Exceptionally, ST-2 was found to have the highest deliverable capacity of 289 cm3STP/cm3 (567 mg/g) at 298 K and 5–200 bar, which surpasses all previously reported records held by porous materials. We illustrate that the fine-tuned mesoporosity is critical in further improving the deliverable capacities at ultrahigh pressure.

A guest-induced reversible crystal-structure transformation is identified in a new 3D covalent organic framework (COF) by comprehensive analyses using powder X-ray diffraction, organic vapor sorption isotherm, and 129Xe NMR spectroscopy. The revolving imine bond in interpenetrating 3D networks is uncovered as the key to the dynamic behavior, the potential applications of which are illustrated by gas separation and heterogeneous catalysis, thus paving the way to the design of stimuli-responsive and multifunctional COF materials.