As discussed previously, C NMR experiments can be implemented easily and provide a wealth of information about the number and type of carbon environments present in sorbent materials. More detailed information about the binding mechanisms can be gained by exploring the local connectivity of the carbon atoms through correlation experiments. However, this approach is typically limited by the low natural abundance of C and as such, the use of isotopically enriched 13 CO2 gas and/or more complex sensitivity-enhanced experiments. In solids, the cross polarisation (CP) experiment can be used to transfer magnetisation via dipolar couplings from a high abundance, high g nucleus, such as 1 H, to a low abundance, low g nucleus, such as C, thus increasing the sensitivity and decreasing spectral acquisition time. The build-up of magnetisation on the low g nuclei is governed by the distance between the coupled spins, as well as molecular dynamics. By using short transfer pulses, only spins in close proximity will be selectively enhanced in the NMR spectrum and therefore the CP experiment can be used as a spectral editing technique. Longer-range couplings can be explored by increasing the transfer time, however, this build-up can be impeded by the T1r relaxation of the high g nuclei and as such, the absolute intensities of signals in these experiments should be treated with care. Furthermore, cross polarisation can be used to transfer magnetisation in two-dimensional HETCOR experiments, which allows for the observation of correlations between coupled spins. For these experiments, an ex situ CO2 loading approach is favoured to gain high-resolution spectra of the final adsorption products under MAS conditions. Here we present a case study showing how one-dimensional C MAS and two-dimensional 1 H- C HETCOR experiments can be used to investigate binding mechanisms in MOF materials.