In comparison to post-combustion CO2 capture and oxy-fuel combustion based processes, pre-combustion CO2 capture carries a number of advantages that may be of benefit for its rapid industrial implementation. Perhaps most significantly, the gases are produced at high pressure, and the partial pressure of CO2 in the mixture is high compared with post-combustion flue gas. As a result, regeneration of the loaded adsorbent can occur through a drop to the atmospheric pressure, which is energetically favorable and is more practical compared with a temperature or vacuum swing-based process. Furthermore, the CO2/H2 separation is inherently easier to perform than CO2/N2 or O2/N2 separations, owing to the greater differences in the polarizability and quadrupole moment of the molecules. Thus, for purely physisorption-based separations, a greater selectivity for CO2 over H2 can be anticipated, which may allow next-generation pre-combustion CO2 capture materials to be more rapidly developed than new adsorbents for post-combustion CO2 capture or oxy-fuel combustion.