Pillared Graphene: A New 3-D Innovative Network Nanostructure Augments Hydrogen Storage

Abstract

Nowadays, people have turned into finding an alternative power source for everyday applications. One of the most promising energy fuels is hydrogen. It can be used as an energy carrier at small portable devices (e.g. laptops and/or cell phones) up to larger, like cars. Hydrogen is considered as the perfect fuel. It can be burnt in combustion engines and the only by‐product is water. For hydrogen‐powered vehicles a big liming factor is the gas tank and is the reason for not using widely hydrogen in automobile applications. According to United States’ Department of Energy (D.O.E.) the target for reversible hydrogen storage in mobile applications is 6% wt. and 45 gr. H2/L and these should be met by 2010.After their synthesis Carbon Nanotubes (CNTs) were considered as ideal candidates for hydrogen storage especially after some initially incorrect but invitingly results. As it was proven later, pristine carbon nanotubes cannot achieve D.O.E.’s targets in ambient conditions of pressure and temperature. Therefore, a way to increase their hydrogen storage capacity should be found. An attempt was done by doping CNTs with alkali metal atoms. Although the results were promising, even that increment was not enough. Consequently, new architectures were suggested as materials that could potentially enhance hydrogen storage. In this work a novel three dimensional (3‐D) nanoporous carbon structure called Pillared Graphene (Figure 1) is proposed for augmented hydrogen storage in ambient conditions.Pillared Graphene consists of parallel graphene sheets and CNTs that act like pillars and support the graphene sheets. The entire structure (Figure 1) can be resembled like a building in its early stages of construction, where the floors are represented by graphene sheets and the pillars are the CNTs. As shown in Figure 1, CNTs do not penetrate the structure from top to bottom. Instead, they alternately go up and down, so that on the same plane do not exist two neighboring CNTs with the same orientation. In addition, the structure has no expanding limits and this is shown by the unfinished CNTs on the top and bottom of the structure (Figure 1). Obviously, the length and the intertube distance of the CNTs can be changed at will in order to have a material with tunable pores. This tailored porosity is a key aspect of our material and thus its usage can be extended to other applications besides hydrogen storage.The stability of the structure was determined by DFT calculations using the Turbomole ab‐initio package. As it was shown by these calculations, our material is stable and in principle it can be formed. Its hydrogen storage capacity was then evaluated by Grand Canonical Monte Carlo (GCMC) calculations and the results showed a spectacular increase when Pillared Graphene was doped with lithium atoms. The increment on the loading when lithium atoms were present was so high that our material was able to store 6.1% wt. and 41 gr./L of hydrogen under ambient conditions.