Abstract
This study presents a comprehensive comparison between the packed bed and monolith contactor configurations for direct air capture (DAC) via process modeling of a temperature-vacuum swing adsorption (TVSA) process. We investigate various design parameters to optimize performance across different contactor geometries, including pellet size, monolith wall thickness, active sorbent content in monoliths, and packed bed structure configurations, considering both a traditional long column (PB(40)) and multiple shorter columns configured in parallel (PB(5)). Our parametric analysis assesses specific exergy consumption, sorbent, and volume requirements across different operating conditions of a five-step TVSA cycle. For minimizing sorbent requirements, PB(5) and monoliths with over 80% sorbent loading were the best-performing contactor designs with overlapping performance in the low-exergy region. Beyond this region, PB(5) faced limitations in reducing sorbent requirements further and was constrained by a maximum velocity at which it is sensible to operate without substantially increasing the exergy demand. In contrast, monoliths decreased sorbent requirements with minimal exergy increase due to reduced mass transfer resistances and lower pressure drop associated with their thin walls. The analysis of volume requirement-specific exergy Pareto fronts revealed that PB(5) was less competitive with this metric due to the requirements for additional void space in the contactor configuration. The study also revealed that optimal sorbent loading for reducing volume requirements in monoliths differed from those minimizing sorbent usage, with the most effective loading being below 100%. Thus, the optimal contactor design varies depending on the goals of minimizing sorbent and volume requirements, and the choice and design of the contactor will depend on the relative costs of these factors. Lastly, our findings challenge the assumption that higher velocities are always preferable for direct air capture, suggesting instead that the operating velocity depends on the contactor configuration.