グラフェン上における水素分子の物理吸着エネルギーのab initio分子軌道法による再検討
This computational study re-examined the physisorption energy of molecular hydrogen on graphene using ab initio molecular orbital theory under a rigid monomer supermolecular framework. The graphene surface was approximated by a coronene-like cluster (C24H12), and basis set superposition error was addressed via the counterpoise correction. Systematic evaluation of basis set and electron correlation combinations—including aug-cc-pVQZ and coupled cluster with single, double, and perturbative triple excitations—identified asymmetric and local modeling strategies as computationally efficient. An asymmetric scheme employing aug-cc-pVTZ for the adsorbate and nearest substrate atoms, with cc-pVTZ for remaining atoms at the MP2 level, was selected as the reference treatment. The resulting physisorption energy was approximately 0.06 eV, roughly 25% below previously published values, while prior reference data were found to carry errors on the order of 60%. Despite the lower energy estimate, carbon-based physisorptive hydrogen storage remains energetically feasible according to these calculations.
Dispersion-dominated physisorption of H2 on graphene was recalculated at the MP2/aug-cc-pVTZ level, yielding approximately 0.06 eV. Prior overestimates were attributed to inadequate numerical treatment and basis set superposition errors.
The delivery route is not clearly identifiable from this paper. For hydrogen intake, inhalation is the most efficient route; inhalation, however, carries explosion risk (empirical LFL of 10%; high-concentration devices are not recommended).
See also:
https://h2-papers.org/en/papers/15836347