喻树楠,马奎,周昶安,宋磊,岳海荣
YU Shunan,MA Kui,ZHOU Chang'an,SONG Lei,YUE Hairong

• 1:四川大学化学工程学院
• 2:四川大学新能源与低碳技术研究院

摘要(Abstract)：

吸附法捕集CO_2是实现工业尾气中CO_2分离和脱除的重要技术。固体胺吸附剂由于优异的CO_2吸附容量和选择性及较低的再生能耗被广泛研究。传统粉末吸附剂由于压降大等问题，需成型加工才能应用于实际工业过程。但整型吸附剂仍面临吸附性能不足、机械性能差等问题。以大孔环氧树脂聚合物为模板、正硅酸乙酯为硅源，采用牺牲模板法制备整型大孔SiO_2,并在其基础上负载四乙烯五胺(TEPA)开发整型大孔SiO_2基固体胺吸附剂。整型大孔SiO_2材料以交联的中空SiO_2微球为骨架，具有典型的大孔结构，且TEPA均匀分布在骨架表面。TEPA负载量为70%的70T-MS样品在75℃、0.1 MPa(12%CO_2/88%N_2)条件下，CO_2吸附量高达191 mg/g,经50次吸脱附循环可稳定在160 mg/g以上。动态吸附试验表明，其CO_2吸附动力学遵循Avrami模型，说明其受传质扩散限制影响较小。整型大孔SiO_2基固体胺吸附剂机械强度可达0.72 MPa(轴向)和30.30 N/cm(径向),满足工业吸附剂要求。吸附剂还具有良好的热稳定性和较低的热容(2.79 J/(g·℃)),有望实现低能耗再生。
Capturing CO_2 by adsorption method is an important technology to realize the separation and removal of CO_2 from industrial exhaust gas. Solid amine adsorbents have been widely explored due to its excellent adsorption capacity and selectivity of CO_2, and low energy consumption for desorption. In fact, traditional powder adsorbents can only be used after molding in actual industrial processes due to its large pressure drop and other problems. However, monolithic adsorbents still face challenges such as insufficient adsorption capacity and poor mechanical properties. Herein, using macroporous epoxy resin polymer as template and tetraethyl orthosilicate as silicon source, the monolithic macroporous SiO_2 was prepared by sacrificial template method. On this basis, the monolithic macroporous SiO_2-based solid amine adsorbent was obtained by impregnating different amount of tetraethylene pentaamine(TEPA). The monolithic macroporous SiO_2 material takes the cross-linked hollow SiO_2 microspheres as the skeleton, which has a typical macroporous structure, and TEPA is evenly distributed on the surface of the skeleton. Under 75 ℃ and 0.1 MPa(12% CO_2/88% N_2), the CO_2 adsorption capacity of 70 T-MS sample with 70% TEPA loading is up to 191 mg/g, which can be stably maintained above 160 mg/g even after 50 adsorption-desorption cycles. Dynamic adsorption results show that the CO_2 adsorption kinetics follow the Avrami model, indicating that the adsorption process is less affected by mass transfer diffusion limitations. Furthermore, the mechanical strength of the adsorbents can reach 0.72 MPa(axial) and 30.30 N/cm(radial), meeting the requirements of industrial adsorbents. Moreover, the adsorbents also exhibit excellent thermal stability and low heat capacity(2.79 J/(g·℃)), which is expected to achieve low-energy desorption and regeneration.

关键词(KeyWords)： CO_2捕集;固体胺;整型吸附剂;大孔SiO_2;机械强度
CO_2 capture;solid amine;monolithic adsorbents;macroporous SiO_2;mechanical strength

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金资助项目(22008160,22078208);; 内蒙古自治区科技重大专项资助项目(2020ZD0025);; 中国石油化工集团公司技术开发资助项目(420011)

作者(Author): 喻树楠,马奎,周昶安,宋磊,岳海荣
YU Shunan,MA Kui,ZHOU Chang'an,SONG Lei,YUE Hairong

DOI: 10.13226/j.issn.1006-6772.CN22050501

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