Mixed Diethanolamine and Polyethyleneimine with Enhanced CO₂ Capture Capacity from Air

Supported polyethyleneimine (PEI) adsorbent is one of the most promising commercial direct air capture (DAC) adsorbents with a long research history since 2002. Although great efforts have been input, there are still limited improvements for this material in its CO₂ capacity and adsorption kinetics under ultradilute conditions. Supported PEI also suffers significantly reduced adsorption capacities when working at sub-ambient temperatures. This study reports that mixing diethanolamine (DEA) into supported PEI can increase 46% and 176% of pseudoequilibrium CO₂ capacities at DAC conditions compared to the supported PEI and DEA, respectively. The mixed DEA/PEI functionalized adsorbents maintain the adsorption capacity at sub-ambient temperatures of −5 to 25 °C. In comparison, a 55% reduction of CO₂ capacity is observed for supported PEI when the operating temperature decreases from 25 to −5 °C. In addition, the supported mixed DEA/PEI with a ratio of 1:1 also shows fast desorption kinetics at temperatures as low as 70 °C, resulting in maintaining high thermal and chemical stability over 50 DAC cycles with a high average CO₂ working capacity of 1.29 mmol g⁻¹. These findings suggest that the concept of “mixed amine”, widely studied in the solvent system, is also practical to supported amine for DAC applications.