Dispatchable low-carbon power underpins the transition to a sustain16 able energy system, providing balancing load for the integration of intermittent renewable power. In such load-following operation, the post-combustion carbon capture process must be capable of highly transient operation. Here we have developed a computational frame work that integrates process design, operability and techno-economic
assessment of a pressure-vacuum swing adsorption process for CO2 capture. We demonstrate that the cost-optimal design has limited process flexibility, challenging reactiveness to disturbances in the flue gas conditions. Flexibility can be introduced by relaxing the CO2 recovery constraint on the operation, albeit at the expense of the
capture efficiency of the process. We discover that adsorption-based processes can be designed to enhance flexibility, while improving per formance with respect to the operational constraints on CO2 recovery and purity. The results herein demonstrate a trade-off between process economics and process operability, which must be ratio nalised to integrate CO2 capture units in low-carbon energy systems.