The interaction of hydrogen with heteroatoms (B, N)-doped porous graphene: A computational study

Abstract

Based on first-principles computations, the adsorption ability of hydrogen on heteroatom (B, N)-doped porous graphene has been illustrated. It is found that the adsorption energy (−\u20090.117\u2009~\u2009−\u20090.173 eV) of hydrogen on heteroatom (B, N)-doped porous graphene meets the optimal adsorption energy (−\u20090.1\u2009~\u2009−\u20090.2 eV) on high-performance adsorbent, indicating that the porosity and heteroatom dopant would be the important role for the H2 adsorption. In addition, the interaction is found to be enhanced by applying positive and negative charges into the system. More important, we demonstrate that the adsorption energy can be dramatically increased to −\u20090.738 eV on the B-doped porous graphene with one positive charge. The H2 adsorption/desorption process on the positively charged B-doped porous graphene is spontaneous, reversible, and readily controlled by injecting/removing the additional positive charge. The gravimetric density is predicted to be 10.8 wt % on the positively charged B-doped porous graphene. Based on density functional theory computations, we investigate the adsorption ability of hydrogen on heteroatom (B, N)-doped porous graphene. Calculation results show that the H2 adsorption/desorption process on the positively charged B-doped porous graphene is spontaneous and reversible with fast kinetics and readily controlled by the adding/removing the additional positive charge.