Charge‐Induced Defective MOF‐801 with Enhanced Sorption Heat for Efficient Hydrogen Storage

Abstract Metal–organic frameworks (MOFs) are considered ideal candidates for H 2 physisorption materials due to their high surface area and tunable pore structures/environments. However, their interaction with hydrogen is too weak to fully exploit their surface area advantages, necessitating the exploration of effective adsorption enhancement strategies. Here, a defective MOF‐801 is reported as an H 2 physisorption material and investigate the enhancement of hydrogen adsorption by charge‐inducing. Based on the excellent stability of MOF‐801, the material retains good porosity after acid vapor etching, compared to the initial MOF‐801 (810 m 2 g −1 ), the surface area reaching up to 970 m 2 g −1 . The mild etching method leads to excess charges around the zirconium (Zr) of MOF‐801, forming specific defective sites with excellent adsorption heat, inducing hydrogen polarization, and enhancing hydrogen capacity. The total H 2 uptake increases from 5.02 wt.% (MOF‐801) to 8.58 wt.% (Cl@MOF‐801) at 77 K and 80 bar. Additionally, the material exhibits excellent cycling performance, stably cycling 10 times at 8 MPa and maintaining a total capacity of 8.56 wt%. The results reveal that tuning H 2 adsorption heat by charge induction is a promising strategy to exploit the potential of porous materials for efficient H 2 storage.