High sorption capacities and enhanced interaction strengths are the two most fundamental prerequisites for the deployment of carbon-based materials as hydrogen-storage media. In spite of continued research efforts over the two past decades, no substrate appears to meet the stringent requirements set by the US Department of Energy for automotive applications. This proposal seeks to fill an important gap in our present understanding of hydrogen uptake by carbon-based nanostructures via a systematic exploration of a series of graphite-oxide substrates with variable interlayer spacing. To this end, we will make use of the unique capabilities of the IRIS spectrometer to explore the microscopic details of how extreme molecular confinement may be further exploited to enhance hydrogen storage capacities.