Omar M. Yaghi and William A. Goddard III reported COFs as exceptional hydrogen storage materials. They predicted the highest excess H uptakes at 77 K are 10.0 wt % at 80 bar for COF-105, and 10.0 wt % at 100 bar for COF-108, which have higher surface area and free volume, by grand canonical Monte Carlo (GCMC) simulations as a function of temperature and pressure. This is the highest value reported for associative H storage of any material. Thus 3D COFs are most promising new candidates in the quest for practical H storage materials. In 2012, the lab of William A. Goddard III reported the uptake for COF102, COF103, and COF202 at 298 K and they also proposed new strategies to obtain higher interaction with H. Such strategy consists of metalating the COF with alkali metals such as Li. These complexes composed of Li, Na and K with benzene ligands (such as 1,3,5-benzenetribenzoate, the ligand used in MOF-177) have been synthesized by Krieck et al. and Goddard showed that the THF is important to their stability. If the metalation with alkali meals is performed in the COFs, Goddard et al. calculated that some COFs can reach 2010 DOE gravimetric target in delivery units at 298 K of 4.5 wt %: COF102-Li (5.16 wt %), COF103-Li (4.75 wt %), COF102-Na (4.75 wt %) and COF103-Na (4.72 wt %). COFs also perform better in delivery units than MOFs because the best volumetric performance is for COF102-Na (24.9), COF102-Li (23.8), COF103-Na (22.8), and COF103-Li (21.7), all using delivery g H/L units for 1–100 bar. These are the highest gravimetric molecular hydrogen uptakes for a porous material under these thermodynamic conditions.