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Carbon-based materials, due to their low cost and weight, have long been considered as suitable physisorption substrates for the reversible storage of hydrogen. Nanoporous carbons can be engineered to achieve exceptional storage capacities: gravimetric excess adsorption of 0.073 ± 0.003 kgH₂/kg carbon, gravimetric storage capacity of 0.106 ± 0.005 kgH₂/kg carbon, and volumetric storage capacity of 0.040 ± 0.002 kgH₂/liter carbon, at 80 K and 50 bar. The nanopores generage high storage capacity by having a very high surface are, by generating a high H₂-wall interaction potential, and by allowing multi-layer adsorption of H₂ (at cryogenic temperatures). In this paper we show how the experimental adsorption isotherms can be understood from basic theoretical considerations and computational simulations of the adsorption in a bimodal distribution of narrow and wide pore spaces. We also analyze the …