Environmental safety has become increasingly important with respect to hydrogen use in society. Monitoring techniques for explosive gaseous hydrogen are essential to ensure safety in sustainable hydrogen utilization. Here, we reveal molecular hydrogen detection mechanisms with monolithic three-dimensional nanoporous reduced graphene oxide under gaseous hydrogen flow and at room temperature. Nanoporous reduced graphene oxide significantly increased molecular hydrogen physisorption without the need to employ catalytic metals or heating. This can be explained by the significantly increased surface area in comparison to two-dimensional graphene sheets and conventional reduced graphene oxide flakes. Using this large surface area, molecular hydrogen adsorption behaviors were accurately observed. In particular, we found that the electrical resistance firstly decreased and then gradually increased with higher gaseous hydrogen concentrations. The resistance decrease was due to charge transfer from the molecular hydrogen to the reduced graphene oxide at adsorbed molecular hydrogen concentrations lower than 2.8 ppm; conversely, the resistance increase was a result of Coulomb scattering effects at adsorbed molecular hydrogen concentrations exceeding 5.0 ppm, as supported by density functional theory. These findings not only provide the detailed adsorption mechanisms of molecular hydrogen, but also advance the development of catalyst-free non-heated physisorption-type molecular detection devices.
Keywords: graphene oxide, hydrogen adsorption; porous graphene.