Direct air capture (DAC) technologies have been vigorously pursued to achieve the goal of net-zero CO2 emissions due to the dramatic increase in atmosphere CO2 concentrations and global temperatures. In practical DAC conditions, variations in temperature and humidity can lead to different CO2 adsorption outcomes. Current studies lack comprehensive information on the optimal temperature and humidity conditions for DAC. In this study, a comparison between PMSU-F (impregnating polyethyleneimine (PEI600) on MSU-F support) and PPMSU-F (co-impregnating polyethylene glycol (PEG200) with PEI600 on MSU-F support) under different temperature and relative humidity conditions were conducted. Under dry conditions, the addition of PEG200 effectively enhanced the adsorption capacity, adsorption rate, and amine efficiency and decreased the energy consumption for desorption depending on the comparison of the two absorbents. Under the popular atmospheric temperature ranges (−5 °C–45 °C), an increase in temperature favors CO2 adsorption. Under humid conditions, the presence of PEG200 had a negative effect due to its strong hydrophilicity. By comparing dry and humid conditions, the introduction of moisture generally enhanced overall CO2 adsorption performance, and the adsorption capacity interestingly further increased under low-temperature conditions. The highest CO2 adsorbing capacity of PMSU-F (3.82 mmol/g) and PPMSU-F (3.76 mmol/g) appeared at −5 °C and 75% relative humidity, indicating that low temperature and relatively high relative humidity were more favorable for DAC, which is possibly attributed to the thermodynamic control under low temperatures with moisture. The results indicate that the adsorbents chosen in this study are promising for DAC under low temperatures and relatively high humidity conditions. The performances of modified DAC adsorbents, e.g., adsorption capacity, stability, antioxidant property for industrial-grade DAC system should be evaluated in the next work.
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