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【目的】针对垃圾焚烧电厂烟气中SO2导致固态胺吸附剂不可逆失活的问题,本研究旨在开发一种具有优异抗硫性能的固态胺吸附材料,以提升其在含硫烟气中的CO2捕集循环稳定性。【方法】本研究提出采用环氧丙烷(propylene oxide,PO)改性四乙烯五胺(tetraethylenepentamine,TEPA)的抗硫策略,通过分子结构调控改变有机胺分子的伯胺、仲胺和叔胺官能团的比例,从而提高固态胺的抗硫循环稳定性。【结果】研究表明,SO2对未改性TEPA@SiO2吸附剂的中毒作用显著,6次循环后吸附容量衰减超过90%。PO改性后,1.0PO-TEPA@SiO2和2.0PO-TEPA@SiO2吸附剂的循环稳定性得到显著提升,但初始CO2吸附容量也有所降低。为兼顾吸附容量与循环稳定性,设计合成了混胺改性MPO-TEPA@SiO2吸附剂,在体积浓度为5.0×10-3高浓度SO2条件下表现出优异的综合吸附性能;在模拟实际工况的体积浓度10.0×10-6 SO2条件下,100次循环的平均单次衰减仅为0.21%,展现出了优异的长期运行稳定性。【结论】PO改性及混胺策略为提升固态胺吸附剂的抗硫性能提供了有效途径,对垃圾焚烧电厂烟气CO2捕集的工程化应用及电力行业的低碳转型具有重要意义。
Abstract:[Objective]To address the issue of irreversible deactivation of solid amine adsorbents caused by SO2 in the flue gas of waste incineration power plants, this study aims to develop a solid amine adsorption material with excellent sulfur resistance to enhance its CO2 capture cycle stability in sulfur-containing flue gas.[Methods] This study proposes a sulfur resistance strategy by modifying tetraethylenepentamine(TEPA) with propylene oxide(PO). The distribution of primary, secondary, and tertiary amine functional groups in the organic amine molecules was regulated through molecular structure modulation to improve the cyclic stability of the solid amine under sulfur-containing conditions.[Results] The results indicate that SO2 caused significant poisoning of the unmodified TEPA@SiO2 adsorbent, with the adsorption capacity decaying by over 90% after 6 cycles. After PO modification, the cyclic stability of the 1.0 PO-TEPA@SiO2 and 2.0 PO-TEPA@SiO2 adsorbents was significantly improved, although the initial CO2 adsorption capacity also decreased. To balance adsorption capacity and cyclic stability, a mixed-amine modified MPO-TEPA@SiO2 adsorbent was designed and synthesized. It exhibited excellent comprehensive adsorption performance under a high SO2 concentration of 5.0×10-3(v/v), and under simulated practical conditions with a SO2 concentration of 10.0×10-6(v/v), the average decay per cycle over 100 cycles was only 0.21%, demonstrating outstanding long-term operational stability.[Conclusion] The PO modification and mixed-amine strategy provide an effective pathway for enhancing the sulfur resistance of solid amine adsorbents, which is of great significance for the engineering application of CO2 capture from flue gas in waste incineration power plants and the low-carbon transition of the power industry.
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基本信息:
DOI:10.19944/j.eptep.1674-8069.2025.06.008
中图分类号:X773
引用信息:
[1]邹金生,谭玲君,林俊豪,等.垃圾焚烧电厂CO_2捕集抗硫固态胺吸附材料的研究[J].电力科技与环保,2025,41(06):941-949.DOI:10.19944/j.eptep.1674-8069.2025.06.008.
基金信息:
国家自然科学基金项目(52574469)