Therefore, it is quite common to see an almost arbitrary combination of the LJ parameters and charge assignment schemes used in HTCS of MOFs. This raises some concerns on the quality of the FFs used for predicting equilibrium adsorption data in molecular simulations. Several studies have endeavoured to understand how the choice of charge scheme or LJ FF changes the rankings of MOFs for CO2 capture. However, these studies do not extend beyond a simple material-level analysis (i.e., up to step 2 in Figure ). In order to align with the advancements achieved in HTCS, the uncertainty embedded within the process-level KPIs must be understood (i.e., up to step 3 in Figure ), given that the adsorption data plays a pivotal role in PSA-based CO2 capture processes. Without this level of analysis, a shadow of doubt on the outcomes of theoretical studies will remain, which only serves to hinder the transition of the recommended materials to the experimental campaign and ultimately to practical, industrial systems.