Lithium‐Functionalized Metal–Organic Frameworks that Show >10 wt % H 2 Uptake at Ambient Temperature

We have used grand canonical Monte Carlo simulations with a first‐principles‐based force field to show that metal–organic frameworks (MOFs) with Li functional groups (i.e. CLi bonds) allow for exceptional H 2 uptake at ambient temperature. For example, at 298 K and 100 bar, IRMOF‐1‐4Li shows a total H 2 uptake of 5.54 wt % and MOF‐200‐27Li exhibits a total H 2 uptake of 10.30 wt %, which are much higher than the corresponding values with pristine MOFs. Li‐functionalized MOF‐200 (MOF‐200‐27Li) shows 11.84 wt % H 2 binding at 243 K and 100 bar. These hydrogen‐storage capacities exceed the 2015 DOE target of 5.5 wt % H 2 . Moreover, the incorporation of Li functional groups into MOFs provides more benefits, such as higher delivery amount, for H 2 uptake than previously reported Li‐doped MOFs.