Cong-Cong Liang,# Zhao-Lin Shi,# Chun-Ting He,# Jing Tan, Hu-Die Zhou, Hao-Long Zhou, Yongjin Lee, and Yue-Biao Zhang,*
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.