Structure-performance relationship of additive-incorporated tetraethylenepentamine-functionalized SiO_(2) in direct air capture of CO_(2)  

作　　者：Zuoyan Yang Yuqi Zhou Hongjie Cui Zhenmin Cheng Zhiming Zhou 

机构地区：[1]State Key Laboratory of Green Chemical Engineering and Industrial Catalysis,School of Chemical Engineering,East China University of Science and Technology,Shanghai 200237,China [2]Industrial Catalysis Center,Department of Chemical Engineering,Tsinghua University,Beijing 100084,China

出　　处：《Frontiers of Chemical Science and Engineering》2025年第2期21-33,共13页化学科学与工程前沿(英文版)

基　　金：Financial support from the National Natural Science Foundation of China(Grant No.22278143)is gratefully acknowledged.

摘　　要：Direct air capture (DAC) using amine-functionalized solid adsorbents holds promise for achieving negative carbon emissions. In this study, a series of additive-incorporated tetraethylenepentamine-functionalized SiO_(2) adsorbents with varying tetraethylenepentamine and additive contents were prepared via a simple impregnation method, characterized by various techniques, and applied in the DAC process. The structure-performance relationship of these adsorbents in DAC was investigated, revealing that the quantity of active amine sites (or the tetraethylenepentamine content in the exposed layer), as determined by CO_(2)-TPD measurement, was an important factor affecting the adsorbent performance. This factor, which varied with the tetraethylenepentamine content, additive type, and additive content, showed a positive correlation with the CO_(2) adsorption capacity of the adsorbents. The optimal adsorbent, 40TEPA-10PEG/SiO_(2) containing 40 wt % tetraethylenepentamine and 10 wt % polyethylene glycol (Mn = 200), exhibited a stable CO_(2) capacity of 2.1 mmol·g^(-1) and amine efficiency of 0.22 over 20 adsorption–desorption cycles (adsorption at 400 ppm CO_(2)/N2 and 30℃ for 60 min, and desorption at pure N2 and 90℃ for 20 min). Moreover, even after deliberate accelerated oxidation treatment (pretreated in air at 100℃ for 10 h), the CO_(2) capacity of 40TEPA-10PEG/SiO_(2) remained at 2.0 mmol·g^(-1). The superior thermal and oxidative stability of 40TEPA-10PEG/SiO_(2) makes it a promising adsorbent for DAC applications.

关 键 词：tetraethylenepentamine-functionalized adsorbent direct air capture active amine sites CO_(2)adsorption capacity thermal and oxidative stability 

分 类 号：O64[理学—物理化学]