So far it appears that the process performances and material rankings depend on both the definition of the LJ and the electrostatic potentials, however it seems that the choice of charge scheme has a stronger impact (Figure ). In practice, (E)Qeq may be chosen over DDEC in HTCS due to restricted computational resources, or they may be used to prescreen large databases and shortlist top performers for further refinement using higher accuracy charge assignment schemes. In an ideal scenario, DDEC charges are available or can be calculated for all candidate materials. In this case, the uncertainty embedded in one's choice of partial charge assignment would be eliminated as ab initio charges are the preferred level of molecular theory for HTCS of materials for carbon capture. If we confine the scope of our analysis to this ideal scenario, the only additional degree of freedom remaining is how to model the LJ interactions. In Figure (a), a direct comparison of the maximum CO2 purity predicted by either UFF or Dreiding in combination with DDEC charges reflects this ideal case study. Apart from FUFREE, the MOFs in this top performing subset show similar process-level responses. While it is tempting to attribute this behaviour to minor scattering in the adsorption data, we show later in section 3.4 that this may not strictly be the case as different adsorption patterns can lead to the same CO2 purity-recovery performances. On the contrary, differences between LJ FFs become much more pronounced at the energy-productivity Pareto level. For example, in Figure (b) we rank materials according to the maximum productivity they can achieve on their energyproductivity Pareto front (subject to the CCS constraints), and make a similar comparison between the top performers identified by UFF+DDEC and Dreiding+DDEC. It is evident from Figure that the predictions between LJ FFs are substantially more uncertain when the energy-productivity process KPIs are used. This observation is notable because the energyproductivity Pareto front more accurately reflects the separation potential of an adsorbent and, unlike the choice of charge scheme, the uncertainty that arises between different LJ parameter sets is unavoidable as the choice of UFF vs Dreiding is still somewhat arbitrary.