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High-surface-area carbons are of interest as potential candidates to store H₂ for fuel−cell power applications. Earlier work has been ambiguous and inconclusive on the effect of boron doping on H₂ binding energy. Here, we describe a systematic dispersion−corrected density functional theory study to evaluate the effect of boron doping. We observe some enhancement in H₂ binding, due to the presence of a defect, such as terminal hydrogen or distortion from planarity, introduced by the inclusion of boron into a graphene ring, which creates hydrogen adsorption sites with slightly increased binding energy. The increase is from −5 kJ/mol H₂ for the pure carbon matrix to −7 kJ/mol H₂ for the boron−doped system with the boron content of ~7%. The H₂ binding sites have little direct interaction with boron. However, the largest enhancement in physi-sorption energy is seen for systems, where H₂ is confined between layers at a distance of about 7 Å, where the H₂ binding nearly doubles to −11 kJ/mol H₂. These findings suggest that interplanar nanoconfinement might be more effective in enhancing H₂ binding. Smaller coronene model is shown to be beneficial for understanding the dependence of interaction energy on the structural configurations and preferential H₂ binding sites.