Near-cryogenic direct air capture using adsorbents

Abstract

Direct air capture (DAC) of CO₂ is a key component in the portfolio of negative emissions technologies for mitigating global warming. However, even with the most potent amine sorbents, large-scale DAC deployment remains limited by high energy and capital costs. Recently, adsorbents relying on weak interactions with CO₂ have emerged as a potential alternative, thanks to their rapid adsorption kinetics and superior long-term stability, particularly under sub-ambient conditions (∼253 K). Despite these advantages, their use is hindered by the need for a water-removal process, location-specific constraints, and insufficient working capacity even in cold climates. In this study, we hypothesized that further reducing the adsorption temperature to a near-cryogenic range (160–220 K) could enable cost-effective DAC by utilizing the full potential of physisorbents. We primarily consider integrating DAC with a relatively untapped source of cold energy—liquified natural gas (LNG) regasification—to perform near-cryogenic DAC. From large-scale molecular simulations, Zeolite 13X and CALF-20 were identified as promising candidates. These materials were subsequently examined through experiments, including breakthrough analyses at 195 K. Their high CO₂ sorption capacity (4.5–5.5 mmol g⁻¹), combined with a low desorption enthalpy and robust long-term stability, led to a threefold reduction in the levelized cost of capture (down to 68.2 USD per tonne CO₂). Estimates of the global LNG regasification resource suggest that LNG–DAC coupling could potentially enable the capture of 103–142 megatonnes of CO₂ annually as of 2050.