The utilization of inexpensive and efficient amine-functionalized adsorbents has become a research hotspot in post-combustion capture technology. Meanwhile, the structure of the support and the selection of organic amines are the primary considerations affecting the CO2 adsorption performance. Herein, the novel solid amine adsorbent materials with amine-support interfacial effect were successfully synthesized in this study by loading four organic amines (TETA, TEPA, PEHA, and PEI) onto expanded vermiculite (EVMT) support with the layered structure. The results indicated that EVMT-50TETA exhibited superior CO2 adsorption capacity (132.5 mg/g) along with effective regeneration capability. This was attributed to the unique layered structure of EVMT that facilitates the dispersion of TETA on its surface or between layers as well as the formation of hydrogen bonds between surface functional groups (–OH) and amines to enhance the amine-support interfacial interaction. Furthermore, the minimal volume expansion of TETA during CO2 adsorption enables improved diffusion of CO2 in channels and enhanced accessibility to active sites. DFT calculations show higher binding energies and faster CO2 adsorption-diffusion rates between TETA and EVMT support. In situ DRIFTS experiments revealed that the process of CO2 adsorption followed the zwitterion mechanism, in which the zwitterion can be reversibly deprotonated to form ammonium carbamate and carbamic acid. This study provides comprehensive insights into the supports and amines interfacial effects through systematic investigation, offering both simplified synthesis strategies and profound theoretical support for studying solid amine adsorbents.
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