Synergistic Interaction-regulated selective carbon dioxide adsorption of amino-functionalized porous organic polymers
Document Type
Article
Publication Date
7-1-2025
Abstract
Nitrogen-containing porous organic polymers (POPs) have attracted tremendous attention due to their adjustable structure, abundant specific surface area and basic sites. Thus, POPs have tremendous promising applications in the field of carbon dioxide (CO2) capture, utilization, and sequestration (CCUS). However, the structure-activity relationship between the amine groups trapped in POPs and the CO2 adsorption performance is still to be disclosed. In this study, POPs functionalized with different amine groups, including primary, secondary and tertiary, were rationally fabricated via the solvothermal copolymerization of amino-modified monomers and divinylbenzene. The as-produced amino-functionalized POPs exhibited a surface area ranging from 168 to 505 m2/g and pore size of 4.0 to 42.6 nm. Adsorption isotherms showcased that ethylenediamine-modified POP (POP-3) exhibited the highest isovolumetric adsorption heat (Qst = 54.8 kJ/mol) with CO2 among these POP absorbents. Notably, ideal adsorbed solution theory (IAST) calculation demonstrated that POP-3 also presented an excellent selectivity (202.4) for CO2 adsorption. The dynamic breakthrough experiments revealed that POP-3 possessed excellent separation performances for the simulated flue gas (CO2/N2, 15/85, v/v) and nature gas (CO2/CH4, 5/ 95, v/v), and the CO2 adsorption capacity could be maintained at least 10 cycles. In situ FTIR measurement and density-functional theory (DFT) calculation elucidated that the excellent adsorption and separation behaviors of POP-3 for CO2 was attributed to the synergistic effect of primary and secondary amine groups. Our finding thus provided theoretical insights into the fabrication of efficient adsorbents, which holds great potential for carbon capture and flue gas separation.
Keywords
CO2 capture, Porous organic polymers, Synergistic effect, Amino group
Divisions
PHYSICS
Funders
National Natural Science Foundation of China (NSFC) (21774101) ; (22472152),Natural Science Foundation of Zhejiang Province (LZY23B040001),Foundation of Zhejiang Sci-Tech University Shengzhou Innovation Research Institute (SYY2024C000002)
Publication Title
Separation and Purification Technology
Volume
361
Issue
1
Publisher
Elsevier
Publisher Location
RADARWEG 29, 1043 NX AMSTERDAM, NETHERLANDS