Electronic Supplementary Information Adsorption Behaviour of CH 4 on Microporous Carbons : Effect of Surface Heterogeneity

Validation of computational methodology Density functional theory (DFT) In the current work, the equilibrium interlayer distance of perfect graphite is optimized to be 3.40 Å, consistent with the experimental value of 3.35 Å 1 and the DFT result of 3.34 Å 2 within an error of 0.2%. Bader charge analysis As shown in Table S1, for the Bader charge analysis in the current work, the atomic partial charges of H and O atoms in hydroxyl group are 0.359 ~ 0.552 e and-0.737 ~-0.914 e, respectively. These results agree well with the DFT results of Wilcox et al 3 (0.575 e and-0.996 e corresponding to H and O atoms, respectively). The adsorption isotherms of CH 4 in perfect graphite pore (pore width = 20.4 Å) at 313 K is chosen to compared with the results of D. D. Do et al. 4 Although two different force field types are used, there is a minor difference in adsorption isotherms for one-site model. The good agreement between our result and the experimental and previous theoretical observations demonstrates the reliability of our model and levels of theory (including DFT, Bader charge analysis and GCMC).