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浙江大学学报(工学版)
Journal of ZheJiang University (Engineering Science)  2022, Vol. 56 Issue (8): 1588-1596    DOI: 10.3785/j.issn.1008-973X.2022.08.013
    
Graphene modification in amine-functionalized SBA-15 and its CO2 adsorption capacity
Meng GUO(),Yu-ru ZHANG,Xing WEI,Wen-jing WANG*()
School of Life Sciences, Hebei University, Baoding 071002, China
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Abstract  

The amine-functionalized sorbent, graphene/SBA-15/hyperbranched polymer (G/SBA-15/HBP), was prepared by wet impregnation method for CO2 capture, to improve the adsorption capacity and stability of amine-functionalized SBA-15 and promote its practical application for post-combustion CO2 capture. The microstructure and chemical composition of adsorbents were characterized by SEM, TEM, N2 adsorption, XRD and FTIR. The effects of HBP mass fraction, adsorption temperature and desorption temperature on CO2 adsorption performance were analyzed, and the reaction conditions were optimized. The thermal stability and cycle performance of the adsorbents before and after graphene modification were investigated. With the HBP mass fraction of 50%, the CO2 adsorption capacity of G/SBA-15/HBP was 1.50 mmol/g, increasing by 51.51% as compared to that of conventional SBA-15/HBP. Graphene-doping decreased particle agglomeration and facilitated gas diffusion. Increasing 12% surface area and 31% pore volume of supports benefited the uniform dispersion of loaded HBP and helped to expose more adsorption sites. Graphene-doping improved the thermal stability of amine-functionalized adsorbents and enhanced its working lifespan and cycle stability.

Key words： graphene      silica      solid amine      adsorption      CO2 capture     
Received: 11 January 2022      Published: 30 August 2022
CLC:  X 51  
Fund:  国家自然科学基金资助项目(52106141)；河北省自然科学基金资助项目 (E2020201022)
Corresponding Authors: Wen-jing WANG     E-mail: guom_mail@126.com;wangwenjing@hbu.edu.cn
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Meng GUO
Yu-ru ZHANG
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Wen-jing WANG
Cite this article:

Meng GUO,Yu-ru ZHANG,Xing WEI,Wen-jing WANG. Graphene modification in amine-functionalized SBA-15 and its CO2 adsorption capacity. Journal of ZheJiang University (Engineering Science), 2022, 56(8): 1588-1596.

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https://www.zjujournals.com/eng/10.3785/j.issn.1008-973X.2022.08.013     OR     https://www.zjujournals.com/eng/Y2022/V56/I8/1588


固胺负载SBA-15的石墨烯改性及其CO2吸附性能

为了提高固胺负载SBA-15的CO2吸附性能及稳定性，推进其在燃烧后CO2捕集中的实际应用，采用湿法浸渍制备新型石墨烯掺杂超支链聚合物（HBP）负载SBA-15（G/SBA-15/HBP）固胺负载吸附剂用于CO2捕集. 通过SEM、TEM、N2吸附、XRD、FTIR对吸附剂的微观结构和化学组成进行表征，研究分析HBP负载量、吸附温度和脱附温度对CO2吸附性能的影响并优化反应条件，探讨石墨烯改性前、后吸附剂的热稳定性和循环性能. 结果表明，当HBP负载量达到50%时，G/SBA-15/HBP的CO2吸附量为1.50 mmol/g，相较传统SBA-15/HBP提升了51.51%. 石墨烯掺杂能减少颗粒团聚，有利于气体扩散；增加载体12%比表面积及31%孔隙容积，有利于负载HBP的均匀分散，暴露更多的吸附位点. 石墨烯掺杂提升了固胺负载吸附剂的热稳定性，提高了吸附剂的使用寿命及循环稳定性.


关键词： 石墨烯,  二氧化硅,  固态胺,  吸附,  CO2捕集 
Fig.1 SEM、TEM images and structure models
Fig.2 N2 adsorption/desorption isotherms
样品 SBET/(m2·g?1) Vtotal/(cm3·g?1) PBJH/ nm
G/SBA-15 666.82 0.89 7.76
SBA-15 595.69 0.68 8.04
G/SBA-15/HBP 37.98 0.074 8.37
SBA-15/HBP 15.44 0.030 16.05
Tab.1 Pore structure parameters before and after HBP loading
Fig.3 Small angle XRD patterns of SBA-15 and G/SBA-15
Fig.4 Infrared spectra of SBA-15 and G/SBA-15 before and after 50% HBP impregnation and CO2 adsorption
Fig.5 Effect of HBP mass fraction and reaction time on CO2 adsorption capacities of G/SBA-15/HBP and SBA-15/HBP
吸附剂类型 θ/℃ p/kPa c/(mmol·g?1) 参考文献
G/SBA-15/HBP (50) 75 100 1.50 本研究
PEI改性碳 75 100 1.09 [41]
石墨纳米带 30 100 0.26 [42]
NaY沸石 50 100 2.17 [43]
Cu-MOF 25 100 0.65 [44]
PEI/SBA-15 25 10 0.65 [45]
氨基硅烷接枝气凝胶 25 100 1.68 [46]
分子印迹吸附剂（MIPs） 60 100 0.48 [47]
PEI 改性膨润土 75 100 1.10 [48]
咪唑基聚离子液体 25 100 0.30 [49]
Tab.2 Comparison of CO2 adsorption performance of G/SBA-15/HBP with other different sorbents
Fig.6 Effect of adsorption and desorption temperatureon on CO2 adsorption capacity of G/SBA-HBP (50)
Fig.7 Thermal stability of G/SBA-15/HBP (50), SBA-15/HBP (50) and HBP with increase of temperature and during cycles (N2 atmosphere)
Fig.8 Cyclic performance of G/SBA-15/HBP (50) and SBA-15/HBP (50)
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