Reaching a historic high of 36.3 gigatonnes in 2021, global CO₂ emissions from fossil fuel combustion continue to increase at an alarming rate. CO₂ removal technologies are part of the solution to tackle this crucial environmental challenge. Thus, the development of porous materials for storage and capture of gas molecules (in particular, carbon capture and storage) has attracted great interest both in academic and industrial communities due to its potential in mitigating atmospheric CO₂ concentrations.

Atomic-scale studies in porous materials are essential to stimulate progress in the design of better CO₂-adsorbents by elucidating gas-sorption surface mechanisms.

Spectroscopic techniques have the potential to shed light on the structural details of distinct materials' surfaces, including the type of chemical species formed upon CO₂ adsorption. Herein, we review the last 5 years of scientific developments wherein solid-state NMR and computational studies have been explored to investigate at the atomic level the structure and molecular dynamics of CO₂ species formed at porous surfaces.