ZIF-67/PDMS复合膜分离废次烟草的中性香气组分

doi:10.11949/0438-1157.20241510

摘要/Abstract

摘要：

从废次烟草中分离中性香气组分是废次烟草资源化利用的重要途径之一。以聚偏氟乙烯（PVDF）为基膜，沸石咪唑酯骨架材料ZIF-67为改性填充物，制备了聚二甲基硅氧烷（PDMS）渗透汽化复合膜用于分离烟草的中性香气组分。采用SEM、FTIR、XRD和接触角测量仪等对复合膜材料进行表征，考察了复合膜对烟草中性香气组分的渗透汽化性能。结果表明，ZIF-67与PDMS基质为物理共混，膜的疏水性增强。随着ZIF-67添加量的增加，渗透通量和分离因子均先增大后减小。当填充量为5%（质量）时，复合膜的分离效果最佳，对2-苯乙醇、大马酮和二氢猕猴桃内酯的最大渗透汽化通量分别为3.61、2.07和0.81 g·m^-2·h^-1；最大分离因子分别为115.5，191.2和109.1。考察了复合膜对实际烟草提取液的分离效果，2-苯乙醇、大马酮和二氢猕猴桃内酯的平均渗透通量分别为16.2、11.6和9.8 mg·m^-2·h^-1。

关键词: 渗透汽化, 聚二甲基硅氧烷, ZIF-67, 中性香气组分, 废次烟草

Abstract:

The separation of neutral aromatic compounds from tobacco waste is one of the important ways to recycle waste tobacco resources. Polyvinylidene fluoride (PVDF) was used as the base membrane and zeolite imidazolate skeleton material ZIF-67 was used as the modified filler to prepare polydimethylsiloxane (PDMS) pervaporation composite membrane for separation of neutral aroma components of tobacco. SEM, contact angle measuring instrument, FTIR and XRD were used to characterize the physical and chemical properties of the composite membrane, and the performance of composite membrane for pervaporation of aromatic compounds was investigated. The results show that ZIF-67 is physically blended with the PDMS matrix, enhancing the hydrophobicity of the membrane. With the increase of ZIF-67 content, the permeation flux and separation factor increase firstly and then decrease. The pervaporation separation performance reaches its optimum when ZIF-67 filling content was 5%(mass). The maximum permeation fluxes of the ZIF-67/PDMS membrane are 3.61, 2.07 and 0.81 g·m^-2·h^-1, and the maximum separation factors are 115.5, 191.2 and 109.1 for 2-phenylethanol, damascenone and dihydroactinidiolide, respectively. The separation efficiency of the composite membrane for actual tobacco extract was investigated, and the average fluxes of the three aromatic compounds are 16.2, 11.6 and 9.8 mg·m^-2·h^-1, respectively.

Key words: pervaporation, PDMS, ZIF-67, neutral aromatic compounds, tobacco waste

中图分类号:

TQ 028.8

刘雨, 蔡振波, 纪利俊, 马晓华. ZIF-67/PDMS复合膜分离废次烟草的中性香气组分[J]. 化工学报, 2025, 76(5): 2337-2347.

Yu LIU, Zhenbo CAI, Lijun JI, Xiaohua MA. Separation of neutral aromatic compounds from tobacco waste by ZIF-67/PDMS composite membrane[J]. CIESC Journal, 2025, 76(5): 2337-2347.

图/表 13

表1 2-苯乙醇、大马酮和二氢猕猴桃内酯的理化性质

Table 1 Physicochemical properties of 2-PE、damascenone and dihydroactinidiolide

化合物	分子量	沸点/℃	lgP	拓扑极性面积/Å²
2-苯乙醇	122.16	219	1.4	20.2
大马酮	190.28	275.6	4.04	17.1
二氢猕猴桃内酯	180.24	296.1	2.2	26.3

图1 不同ZIF-67填充量的PDMS/PVDF复合膜与截断面的SEM图

Fig.1 SEM images of the surface and the cross-section of PDMS with different ZIF-67 loadings

图2 不同ZIF-67填充量的PDMS/PVDF复合膜的水接触角

Fig.2 Water contact angle of ZIF-67 filled PDMS/PVDF membranes with various ZIF-67 loadings

图3 ZIF-67与不同ZIF-67填充量的复合膜的XRD谱图

Fig.3 XRD patterns of ZIF-67 and PDMS with different ZIF-67 loadings

图4 ZIF-67与不同ZIF-67填充量的复合膜的FTIR谱图

Fig.4 FTIR spectra of ZIF-67 and PDMS with different ZIF-67 loadings

图5 ZIF-67/PDMS复合膜的溶胀度随2-PE浓度(a)和浸泡时间(b)的变化

Fig.5 Effect of 2-PE concentrations (a) and immerse time (b) on swelling degree of ZIF-67/PDMS membrane

图6 不同ZIF-67填充量对复合膜分离性能的影响

Fig.6 Effect of composite membranes with different ZIF-67 loading on pervaporation performance

图7 不同料液温度对单一香气组分/水[(a)、(c)、(d)]和三元香气组分/水(b)体系的渗透汽化性能的影响

Fig.7 Effect of temperature on pervaporation performance for aromatic compounds/water single systems [(a), (c), (d)] and ternary system(b)

图8 单一香气组分/水(a)和三元香气组分/水(b)体系中表观活化能拟合结果

Fig.8 Fitting lines of apparent energy in aromatic compounds/water single systems(a) and ternary system(b)

图9 不同浓度下香气组分/水二元体系的渗透通量(a)、分离因子及PSI(b)、渗透率(c)和选择性(d)

Fig.9 Fluxes (a), separation factor and PSI (b), permeability (c) and selectivity (d) of aromatic compounds/water binary system with different concentrations

图10 2-PE/大马酮/水(a)、2-PE/二氢猕猴桃内酯/水(b)和大马酮/二氢猕猴桃内酯/水(c)三元体系中不同浓度比的渗透通量

Fig.10 Fluxes at different concentration ratios in the ternary systems of 2-PE/damascenone/water(a), 2-PE/dihydroactinidiolide/water(b) and damascenone/dihydroactinidiolide/water(c)

图11 实际烟草提取液的连续实验中的渗透汽化通量变化

Fig.11 Fluxes in the continuous experiment of practical tobacco extract

图12 烟草提取液渗透汽化前后的GC-MS总离子流色谱图

Fig.12 GC/MS total ion current map of aromatic compounds in aqueous tobacco extract before and after pervaporation

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