Impact of H2O on CO2 adsorption and co-adsorption: Mechanism and high-performance adsorbents for efficient H2O-CO2 capture

Physical adsorbents used for CO2 capture from air directly and wet CO2 flue gas have limited effectiveness due to competitive adsorption of H2O and CO2. Therefore, it is crucial to understand the impact of H2O on CO2 adsorption and investigate the co-adsorption mechanism in order to enhance the screening, design, and optimization of carbon capture systems. Herein, heat treatments are performed on commercial NaX zeolites to modify the composition of the O-T-O (T = Al, Si) framework. Our systematic investigation based on thermogravimetric analysis/differential scanning calorimetry (TG-DSC), infrared spectroscopy (IR), solid-state nuclear magnetic resonance (SSNMR), and density-functional theory (DFT) calculation, the connection between the structure of NaX zeolite and H2O and CO2 adsorption/desorption is established. The heat-induced changes in the O-T-O (T = Al, Si) framework produce movements of the loaded Na+ ions. Hydrogen bonds formed by agglomerated adsorbed H2O constitute the primary source of desorption heat, which adversely affects CO2 mass transfer and adsorption. Our findings illustrate that modifying the distribution of Na+ ions in the O-T-O (T = Al, Si) framework can reduce the CO2 adsorption energy and prevent the formation of water agglomerates. Our findings provide insights into the design of efficient and high-capacity adsorbents for CO2 capture that can be operated in the presence of H2O.