Improved hydrogen storage performance of defected carbon nanotubes with Pd spillover catalysts dispersed using supercritical CO2 fluid

Hydrogen storage properties of carbon nanotubes (CNTs) modified by oxidative etching and decoration of Pd spillover catalysts are investigated. A mixed H2SO4/H2O2 solution containing ferrous ions (Fe2+) is useful to open the caps, to shorten the length, and to generate defects on CNTs. The Pd catalysts are deposited on the CNTs with the aid of supercritical carbon dioxide (scCO2); as a result, a highly dispersed Pd nanoparticles and an intimate connection between Pd and carbon surface can be obtained. Combination of the two approaches can optimize a hydrogen spillover reaction on CNTs, resulting in a superior hydrogen storage capacity of 1.54 wt% (at 25 °C and 6.89 MPa), which corresponds to an enhancement factor of ∼4.5 as compared to that of pristine CNTs.

► A mixed H2SO4/H2O2 solution containing Fe2+ is useful to create defects on CNTs.
► Supercritical CO2 fluid can highly disperse Pd nanoparticles on the defected CNTs.
► Combining the two approaches can optimize the hydrogen spillover reaction on CNTs.
► The resulting hydrogen capacity is 4.5 times higher than that of pristine CNTs.