Experimental Evaluation of Commercial Molecular Sieves 13X, 4A, and JLPM3 for Sustainable Direct Air CO2 Capture from Humid Air via Temperature-Swing Adsorption with Low-Temperature Regeneration: “Sieve the Atmosphere”

Direct air capture (DAC) of CO2 via temperature-swing adsorption (TSA) can support sustainable carbon dioxide removal, but only if sorbents regenerate with low energy demand and maintain performance under humid ambient air. Here, we evaluate three commercial molecular sieves (JLPM3, 13X and 4A) in packed-bed tests using humid ambient air. We compared 40 g samples as received with 200 g samples conditioned for 12 days at 100 °C to emulate prolonged exposure to regeneration temperature (the cumulative effect of many heating/desorption cycles); all cycle-stabilized uptake values are reported from the conditioned materials. JLPM3 delivered the highest stabilized CO2 uptake (0.24 ± 0.01 mmol·g-1), consistent with a combined physisorption/chemisorption mechanism. Its higher total porosity and smaller mesopores promoted rapid mass transfer and site accessibility, while slightly greater micropore area and volume than 13X supported its marginally higher capacity. Evidence of partial structural degradation under mechanical and thermal stress indicates that minimizing strain during cycling will be important for scale-up and for reducing sorbent replacement. Conditioning at 100 °C activated additional chemisorption sites across all sieves but reduced physisorption capacity. Importantly, a ~100 °C desorption step fully regenerated physisorbed CO2 while purging moisture from zeolite pores, indicating that low-temperature TSA (compatible with low-grade or waste heat) can replace harsher 300 °C regeneration and lower energy demand. CO2–H2O competition experiments confirmed substantial site occupancy by water vapor, which limits capture under humid conditions and motivates water-management strategies. Overall, maximizing DAC performance requires tailoring pore structure and operating conditions while preserving sorbent integrity; JLPM3 emerges as a promising candidate for more energy- and resource-efficient DAC.