Review on recent advances in nanocellulose aerogels for oil-water separation
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摘要: 石油泄漏事件频繁发生，对环境和人类健康造成了极大的危害，因此亟需对含油废水进行有效的处理。目前的吸油材料存在局限性，如吸附量小、成本高和对环境有害等，而纳米纤维素气凝胶由于具有高孔隙度、高比表面积和低密度等特点，经疏水改性后能够吸附大量的油，在油水分离中有着显著优势。本文综述了纳米纤维素气凝胶的制备和疏水改性方法；介绍了纳米纤维素气凝胶结构特点及对其吸附性能的影响，综述了近年来纳米纤维素气凝胶在油和有机溶剂的吸附以及油水混合物分离中的应用；最后提出了纳米纤维素气凝胶的发展现状以及对未来的展望。Abstract: The frequent occurrence of oil spills has caused great threat to environment and human health, so it is urgent to treat oily wastewater effectively. Current oil absorbing materials have limitations, such as low absorption capacity, high cost and environmental harm. Nanocellulose aerogel can absorb a large amount of oil because of its high porosity, high specific surface area and low density. After hydrophobic modification, nanocellulose aerogel has a significant advantage in oil-water separation. The preparation and hydrophobic modification of nanocellulose aerogel are reviewed in this paper. The structural characteristics of nanocellulose aerogel and their influence on absorption performance were introduced. The application of nanocellulose aerogel in adsorption of oil and organic solvent and separation of oil-water mixture in recent years were reviewed. Finally, the development status and future prospects of nanocellulose aerogel are presented.
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Key words:
- aerogels /
- nanocellulose /
- absorption /
- hydrophobicity /
- oil absorption /
- oil-water separation
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图 3 (a) CVD改性BNC气凝胶示意图[39]; (b)改性前后BNC气凝胶的疏水性及相应水接触角[39]; (c)不同MTMS添加量下CNF气凝胶的水接触角[40]
Figure 3. (a)Illustration for the CVD process of BNC aerogel[39]; (b) Hydrophobicity and corresponding water contact Angle of BNC aerogel before and after modification[39]; (c) Water contact Angle of CNF aerogels at different MTMS supplemental levels[40]
图 4 (a)不同交联方式和不同前驱体浓度下纳米纤维素气凝胶的比表面积[46]; (b)不同NC/Al2O3质量比气凝胶的吸附能力[49]
Figure 4. (a)Specific surface area of nanocellulose aerogel under different crosslinking methods and different precursor concentrations[46]; (b) Adsorption capacity of aerogel for thiophene at different weight ratios of NC to Al2O3[49]
图 5 (a)通过冷冻干燥制备气凝胶的SEM图像[50]; (b)通过超临界CO2干燥制备气凝胶的SEM图像[50]; (c)不同MTES含量下气凝胶的孔隙结构及对应吸附能力[52]
Figure 5. (a) SEM images of the aerogels obtained by freeze drying[50]; (b) SEM images of typical aerogels obtained by supercritical CO2 drying[50]; (c) Pore structure and adsorption capacity of aerogel with different MTES content[52]
图 6 (a)不同干燥方法下气凝胶的应力应变曲线[50]; (b)不同PDA含量下CNF气凝胶的应力应变曲线[51]; (c) CNF/PVA定向冷冻干燥过程[54]; (d) 100次压缩-卸载循环下气凝胶的应力应变[54]; (e)40次吸附解吸循环下气凝胶的吸附能力[54]
Figure 6. (a) SEM images of the aerogels obtained by freeze drying[50]; (b) SEM images of typical aerogels obtained by supercritical CO2 drying[51]; (c) The directional freeze drying process of CNF/PVA aerogel[54]; (d) Stress-strain of aerogel under 100 compression-unload cycles[54]; (e) Adsorption capacity of aerogel after 40 adsorption and desorption cycles[54]
图 7 (a) 气凝胶油水分离机理[56];(b) CNC/CS复合气凝胶对油和有机溶剂的吸附能力[58]; (c) CNC/CS复合气凝胶吸附能力与溶剂密度关系[58]
Figure 7. (a) Oil-water separation mechanism of aerogel[56]; (b) The ability of CNC/CS composite aerogel to adsorb oils and organic solvents[58];(c) Relationship between adsorption capacity of CNC/CS composite aerogel and solvent density[58]
图 8 (a) CNF/PML气凝胶对机油、柴油和原油的吸附容量-时间曲线以及伪一阶模型和伪二阶模型[60]; (b) CNF/PML气凝胶对柴油的循环吸附测试[60]
Figure 8. (a) The adsorption capacity-time curve of CNF/PML aerogel on oil, diesel and crude oil: pseudo-first-order model and pseudo-second-order model[60]; (b) Cyclic adsorption test of CNF/PML aerogel on diesel oil[60]
图 9 (a) CNC/GO复合气凝胶快速吸附乙酸乙酯和四氯甲烷[64]; (b) CNC/GO复合气凝胶对各种油和有机溶剂的吸附能力[64]; (c) CNC/GO复合气凝胶的重复使用性能[64]
Figure 9. (a) CNC/GO composite aerogel quickly adsorbed ethyl acetate and tetrachloromethane[64]; (b) The ability of CNC/GO composite aerogel to adsorb oils and organic solvents[64]; (c) Reusable performance of CNC/GO composite aerogel[64]
图 10 (a) 气凝胶厚度与通量的关系[67]; (b) 泵驱动下的连续油水分离过程[68]; (c) CNF/PDMS气凝胶对正己烷、甲苯和甲基环己烷的分离通量[68]; (d)气凝胶分离乳液过程及分离前后液滴尺寸[70]; (e) 气凝胶分离乳液机理 [70]; (f)气凝胶初始分离通量、总分离量和分离效率[70];(g) 气凝胶对四种油包水乳液的分离效率[71]
Figure 10. (a) Relationship between aerogel thickness and flux[67]; (b) A continuous oil-water separation process driven by a pump; (c) Separation fluxes of CNF/PDMS aerogel for n-hexane, toluene and methylcyclohexane[68]; (d) Aerogel separation emulsion process and droplet size before and after separation[70]; (e) Mechanism of aerogels separating emulsion[70]; (f) Initial separation flux, total separation amount and separation efficiency of aerogel[70]; (g) Separation efficiency of aerogel for four water-in-oil emulsions[71]
表 1 不同原料和干燥方法下纳米纤维素气凝胶的基本性能
Table 1. Basic properties of nanocellulose aerogels under different raw materials and drying methods
Material Content/wt% Density/(mg·cm−3) Porosity/% Specific surface area/(m2·g−1) Drying Ref. BNC 1 90 93.6 660 Supercritical Drying [31] CNF 0.5 9.42 99.26 362.7 Freezing drying [33] CNF 1.5 58.82 / 22.4 Atmospheric Pressure Drying [36] BNC 0.4 46 97.7 / Freezing drying [41] CNC 0.5 5.6 99.6 / Freezing drying [42] CNC 2 21.7 98.6 250 Freezing drying [42] CNF 0.5 4 99.8 42 Freezing drying [43] CNF 0.6 8 99.5 30 Freezing drying [44] CNF 2 23 99 90 Freezing drying [45] Notes: BNC - Bacterial nanocellulose; CNF - cellulose nanofiber; CNC- cellulose nanocrystal. 
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表 2 不同纳米纤维素复合气凝胶的性能及油水分离性能比较
Table 2. Comparison of the properties and oil-water separation performances of different nanocellulose composite aerogel
Materials Density/
(mg·cm−3)Oil types Maximum
Absorption
capacity(g·g−1)WCA/(°) Porosity/% Specific surface
area/(m2·g−1)Reusability/
timesMaximum oil
flux /(L·m−2·h−1)Ref. CNF/CS 8.4 Trichloromethane 253 148 96 / 50 / [58] CNF/PML 5.1 Tetrachloromethane 160 129 / 9.8 15 [60] CNC\RGO 4.98 Tetrachloromethane 276 / 99.6 272.2 10 / [64] CNF/PEI/EGDE 53.8 Tetrachloromethane 28.03 130 95.73 / 10 5400 [67] CNF/PDMS 22.7 Toluene 48 163.5 98.4 / 20 145 [68] CNF/SiO2 6.43 / 168.4 129 99.6 108.6 20 1910 [70] CNF/TA/ICO 24 Dichloromethane 113.8 134.8 98.32 / / 4783.8 [71] BNC/PMSQ 5.74 Trichloromethane 203 168 99.59 / 10 473.8 [80] CNF/SA 24.2 Silicone Oil 88.91 144.5 97.85 149.64 20 / [81] CNF/CS/ZIF-8 15.87 Trichloromethane 74.55 132.6 99.01 5.51 20 13167.5 [82] Notes: CS—chitosan; PML—Premna microphylla leaves; RGO—Reduced graphene oxide; PEI—Polyethyleneimine; EGDE—Ethylene glycol diglycidyl ether; PDMS—polydimethylsiloxane; PMSQ—polymethylsilsesquioxane; SA—sodium alginate; WCA—Water contact angle;ZIF-8—Zeolitic Imidazolate Framework-8.
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