Empiric evaluations of fundamental characteristics of interactions of gaseous hydrogen with different kinds of graphite and novel carbonaceous nanomaterials and revealing the micromechanisms have been carried out. The approaches used were those of the thermodynamics of reversible and irreversible processes for analysis of the adsorption, absorption, diffusion, TPD and other experimental data and comparing the analytical results with first-principle calculations. Such analysis of a number of the known experimental and theoretical data has shown a real possibility of the multilayer specific adsorption (intercalation) of hydrogen between graphene layers in novel carbonaceous nanomaterials, relevance for solving the bottle-neck problem of the hydrogen on-board storage in fuel-cell-powered vehicles, and other technical applications.

In this analytical review, some thermodynamic, physical and nanotechnological aspects of the graphene/graphane problem are considered (in a correlation), relevance to developing a much simpler and efficient method (in comparison with the megabar compression dynamic and static ones) of producing a high-density solid molecular hydrogen carrier. It is achieved by the hydrogen intercalation (at the cost of the hydrogen association energy) in closed multigraphane (carbohydride-like) nanostructures of the megabar strength properties. The limiting density value (0.7±0.2 g/cm3(H2)) of such intercalated high-purity reversible hydrogen carrier corresponds to a megabar compression. The “volumetric” hydrogen capacity is of 0.3±0.1 g/cm3(system), and the “gravimetric” one being ≥ 15 wt %( H2). Such a hydrogen storage nanotechnology can exceed and/or correspond to the known U.S. DOE requirements-targets on the hydrogen on-board storage for 2015 (www.eere.energy.gov /hydrogenandfuelcells), with respect to the hydrogen capacities (0.081 g/cm3(system), 9.0 wt %( H2)), safety, reversibility and purity.

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An annotated analytical essay of possible nanofabrication and nanotechnology applications is presented with respect to: (1) some techniques and original results [1-4] concerning the regularities and micromechanisms (physics) of the hydrogen fluoride gas activator influence on the diffusion-controlled oxidation processes of titanium, zirconium and zirconium-based alloys with niobium, and also – on nitriding, boriding and carbiding a series of refractory metals (Ti, Zr, Nb, Mo, W, Ta); (2) some techniques, original results and physics of the diffusion-controlled formation processes of the compound-like nanosegregation [5-13] and the results [13-23] on the liquid-like phase at grain boundary regions in metals and alloys. In the scope of this review, a constructive analysis, the Arrhenius-type treatment, and the original data interpretation [16-21] has been carried out for the first time; (3) some techniques, original analytical results, and physics [24, 25] of the diffusion-controlled processes of the hydrogen multilayer intercalation (physisorption of a condensation or clustering type) with carbonaceous nanostructures. The main objective of the given analytical essay is to attract the researchers’ attention to the expediency of such a non-conventional data analysis and interpretation.

Urgent open questions and their solution ways are considered of the thermodynamic stimuli and mechanisms of the enhanced Fickian diffusion mass-transport providing the unusual structuralphase transformations in metallic materials undergoing the intensive cold deformation, those can not be described in the framework of the conventional phase diagrams.