化工进展 ›› 2023, Vol. 42 ›› Issue (12): 6452-6460.DOI: 10.16085/j.issn.1000-6613.2023-0176

• 材料科学与技术 • 上一篇    

多级孔硅铝酸盐纳米球的合成及其吸附分离多环芳烃

武鲁明1,2(), 于海斌2(), 臧甲忠2, 王亚权1, 李滨2, 孙振海2   

  1. 1.天津大学化工学院,天津 300350
    2.中海油天津化工研究设计院有限公司,天津 300131
  • 收稿日期:2023-02-10 修回日期:2023-03-22 出版日期:2023-12-25 发布日期:2024-01-08
  • 通讯作者: 于海斌
  • 作者简介:武鲁明(1990—),女,博士研究生,主要研究方向为催化材料的制备及其催化机理。E-mail: wuluming8363@163.com
  • 基金资助:
    中海油能源发展股份有限公司项目(HFZXKT-TJY2020-06)

Synthesis of hierarchically porous aluminosilicate nanospheres and their adsorption and separation of polycyclic aromatic hydrocarbons

WU Luming1,2(), YU Haibin2(), ZANG Jiazhong2, WANG Yaquan1, LI Bin2, SUN Zhenhai2   

  1. 1.School of Chemical Engineering and Technology, Tianjin University, Tianjin 300350, China
    2.CNOOC Tianjin Chemical Research and Design Institute Co. , Ltd. , Tianjin 300131, China
  • Received:2023-02-10 Revised:2023-03-22 Online:2023-12-25 Published:2024-01-08
  • Contact: YU Haibin

摘要:

以阳离子表面活性剂十六烷基三甲基溴化铵(CTAB)和阴离子聚电解质聚丙烯酸(PAA)形成的介观复合物为动态模板,以异丙醇铝为铝源,原位合成了不同硅铝比的多级孔硅铝酸盐纳米球(NKM-5-Al-x)。采用X射线衍射仪(XRD)、氮气吸附脱附、程序升温(NH3-TPD)、核磁(27Al NMR)、扫描电镜(SEM)、透射电镜(TEM)等表征方法对多级孔硅铝酸盐纳米球进行了表征分析,并对比孔径结构相对均一的SBA-15和MCM-41氧化硅材料,考察材料的多级孔结构和酸性质对多环芳烃吸附分离性能的影响。结果表明,孔分布和酸性质对多环芳烃分离性能影响显著,多级孔结构有利于多环芳烃的扩散,酸性增强有利于提高多环芳烃分离效率,具有较强酸量和多级孔结构的NKM-5-Al-5呈现出最优的多环芳烃分离效果,分离度R多环芳烃/非芳烃>1.2,且脱吸附速率较快,脱/吸附速率比接近1。

关键词: 多级孔纳米球, 孔分布, 酸性质, 多环芳烃, 吸附分离

Abstract:

Hierarchically porous aluminosilicate nanospheres (NKM-5-Al-x) with different Si/Al ratios were synthesized by employing organic mesomorphous complexes of cationic surfactant cetyltrimethylammonium bromide (CTAB) and anionic polyelectrolyte polyacrylic acid (PAA) as the dynamic template and aluminum isopropoxide as the aluminum source. The hierarchically porous aluminosilicate nanospheres were characterized by X-ray diffraction (XRD), nitrogen adsorption desorption, temperature programmed (NH3-TPD), nuclear magnetic resonance (27Al NMR), scanning electron microscopy (SEM) and transmission electron microscopy (TEM). The SBA-15 and MCM-41 silica materials with relatively uniform pore structure were compared. The effects of the hierarchically porous structure and acid properties of the materials on the adsorption and separation performance of polycyclic aromatic hydrocarbons (PAHs) were investigated. The results showed that the pore distribution and acid properties had a significant impact on the separation performance of PAHs. The hierarchically porous structure was profit for the diffusion of PAHs. The increase of acid content was beneficial to improve the separation efficiency of PAHs. NKM-5-Al-5 with strong acid content and hierarchically porous structure indicated the best PAHs separation effect. The separation degree of RPAHs/non-aromatics was above 1.2 and the desorption/adsorption rate was fast with the desorption/adsorption rate ratio close to 1.

Key words: hierarchically porous nanospheres, pore distribution, acidic properties, polycyclic aromatic hydrocarbons, adsorption separation

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