High-capacity hydrogen storage in zirconium decorated zeolite templated carbon: Predictions from DFT simulations

The hydrogen (H2) storage capacity of Zirconium (Zr) decorated zeolite templated carbon (ZTC) has been investigated using sophisticated density functional theory (DFT) simulations. The analysis shows that the Zr atom gets bonded with ZTC strongly with binding energy (BE) of −3.92 eV due to electron transfer from Zr 4d orbital to C 2p orbital of ZTC. Each Zr atom on ZTC can attach 7H2 molecules with average binding energy of −0.433 eV/H2 providing gravimetric wt% of 9.24, substantially above the limit of 6.5 wt% set by the DoE of the United States of America. The H2 molecules are involved via Kubas interaction with Zr atom, which involves the charge transfer between Zr 4d orbital and H 1s orbital with interaction energy higher than physisorption but lower than chemisorption. The structural integrity of the system is confirmed via molecular dynamics (MD) simulations at room temperature and at highest desorption temperature of 500 K. We have investigated the chances of metal clustering by computing diffusion energy (ED) barrier for the movement of Zr atom, and we obtained via calculation, we can infer that the presence of ED barrier of ∼2.36 eV may prevent the possibility. As the system ZTC has been synthesized, Zr doped ZTC is stable, existence of sufficient diffusion barrier prevents the clustering and adsorption energy and wt% of H2 are within the range prescribed by DoE, we feel that Zr decorated ZTC can be fabricated as promising hydrogen storage material for fuel cell applications.