First, the variables of interest for each process and their corresponding distributions were identified for the sensitivity analysis. The selection aimed to include variables related to each important adsorbent property or process parameter. For instance, parameters were included that describe heat and mass transfer, uptake of CO2 and H2O, adsorbent density and heat capacity, as well as pressure and temperature settings and cycle step times. These variables and their ranges are shown in Table , whilst the justification for our choices is found in the ESI Table . Meanwhile, from experience, we know that some model inputs are irrelevant to the research questions, so they were kept constant, and the values chosen are in the ESI Tables S4-S7. Email: jpy1@hw.ac.uk RCCS, Heriot-Watt University Uniform distributions were used for all parameters apart from the CO2 LDF constant, 𝑘 𝐶𝑂 2 . This was a conservative choice, which was implemented due to a lack of information to suggest otherwise, following the maximum entropy principle. For the CO2 LDF constant, the logarithm was varied uniformly instead. The parameters were varied around the properties of Lewatit® VP OC 1065 taken from our previous work. The ranges (minima and maxima) were assigned based on a literature review to encompass the typical design space of amine-functionalised adsorbents. We varied the isotherm parameters enough to have visibly different isotherms that are still likely to apply to aminefunctionalised adsorbents based on a visual inspection and our literature review. The range of isotherms can be observed in the ESI Figures . The heat transfer coefficient is still highly uncertain, but we varied our value around the range we used in previous work, which is based on earlier process modelling work. The process parameters were varied based on preliminary parametric work and operational limits that we imposed. Examples of these limits are: