Theoretical studies in the stability of vacancies in zeolite templated carbon for hydrogen storage.

Abstract In this work, we report DFT calculations of the energy formation and stability of multi-vacancies in a unit of Zeolite Template Carbon (C 39 H 9). We label as V n the respective vacancy where n carbon atoms have been removed from the pristine C 39 H 9 structure. The results show that V 2 , V 4 , V 6 and V 9 are the most stable vacancies on the ZTC structure. This result agrees with many other studies. Besides, the most stable vacancy of ZTC structure is when nine carbon atoms are removed (V 9) from the ZTC structure. The formation of pentagon rings in the reconstruction of the ZTC vacancy give drastic effect on the energetics stability. Therefore, the formation of pentagon rings eliminates the dangling bonds thus lowering the energy formation. It is also carried out the decoration of ZTC vacancy with Lithium and Calcium atoms, this is the way to use de ZTC vacancy decorated as a medium for hydrogen storage. The results show that the ZTC vacancy decorated with 3 Lithium atoms can adsorb a maximum of nine hydrogen molecules (3 hydrogen molecules per Lithium atom). This gives a gravimetric storage capacity of 4.44 wt percent (wt. %), which is not enough for meeting DOE gravimetric target. On the other hand, to reach DOE gravimetric target, the study of ZTC vacancy decorated with 3 Calcium atoms is carried out, which can adsorb maximum of fifteen hydrogen molecules (5 hydrogen molecules per Calcium atom), this gives gravimetric storage capacity of 5.81 wt %, which meet DOE gravimetric targets, besides the binding energy of hydrogen molecules on ZTC vacancy decorated with 3 Calcium is calculated. These energies are in the range 0.2453–0.2053 eV/H 2 , which are desirable energies for hydrogen adsorption. This is demonstrated by building isotherm adsorption path. The results show that forming vacancies on ZTC structure decorated with three Calcium atoms (3Ca C 30 H 9) is good candidate as medium for hydrogen storage. Highlights • Creation of vacancy in ZTC structure (C 39 H 9) using DFT calculations. • Decoration of ZTC vacancy with metallic atoms (Ca and Li) using DFT theory. • Adsorption energies of H 2 molecules on 3Ca C 30 H 9 are in range 0.2453–0.2053 eV/H. • Maximum storage capacity of H 2 molecules on 3Ca C 30 H 9 system is 5.81 wt %. • Equilibrium pressure is 20–25 MPa for the 3Ca C 30 H 9 nH 2 system. [ABSTRACT FROM AUTHOR]