Recent progress in special infiltrating nanocellulose-based aerogel for oil-water separation
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摘要: 随着石油化工、纺织工业、钢铁等行业的飞速发展，产生了大量的含油废水而严重破坏了人类的生存环境，并造成了水资源短缺问题的加剧。在碳达峰、碳中和全球共识下，如何有效分离油水混合物成为当前的研究热点。特殊浸润性纳米纤维素基气凝胶具有对油水两相浸润性不同的特点，同时有高效的油水分离效果，在油水分离领域有广阔的应用前景。本文系统总结了几种浸润模型和基本作用机制，重点围绕纳米纤维素基气凝胶在油水分离领域的应用和制备工艺进行分析和介绍，探讨了当前特殊浸润性纳米纤维素基气凝胶在研发中面临的问题，并对其未来的发展趋势做出展望。Abstract: The development of petrochemical, textile industry, steel and other industries has produced oily wastewater that has seriously damaged the eco-logical environment of humans and has aggravated the shortage of water resources. How to effectively separate oil-water mixture has become a current research hotspot under the global consensus of carbon peaking and carbon neutral. The special infiltrating nanocellulose-based aerogel has the characteristics of different infiltration to oil and water phases and has high efficiency of oil-water separation, so it has a broad application prospect in the field of oil-water separation. This article systematically summarized several infiltration models and basic action mechanisms, focusing on detailed analysis of nanocellulose-based aerogels in oil-water separation field and preparation process. Finally, the existing problems of special infiltrating nanocellulose-based aerogels are discussed with looking forward to their future development.
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图 4 三嗪衍生物活化反应构建生物质气凝胶的策略: (a) 羧甲基纤维素(CMCs)和纤维素纺锤(CNF)在4-(4, 6-二甲氧基三嗪-2-基)-4-甲基吗啉盐酸盐(DMTMM)存在下的反应方案和凝胶化机制；(b)干燥气凝胶的示意图(包括交联、冷冻、乙醇解冻和丙酮溶剂交换)；(c)干燥制备的气凝胶； (d)干燥气凝胶的形貌；(e)气凝胶可承受其质量的2 500倍，并在装卸后显示出良好的回收性[35]
TEMPO—2, 2, 6, 6-tetramethylpiperidine-1-oxyl); m—Mass; ρ—Density; D—Diameter
Figure 4. Strategy to construct biomass aerogels through a triazine derivative activated reaction at ambient conditions: (a) Proposed reaction scheme and gelation mechanism of carboxymethyl cellulose (CMCs) and cellulose nanofibrils (CNF) in the presence of 4-(4, 6-dimethoxy-1, 3, 5-triazin-2-yl)-4-methylmorpholinium chloride (DMTMM); (b) Schematic illustration of preparing aerogel for ambient drying, including cross-linking, freezing, ethanol thawing, and acetone solvent exchange; (c) Aerogels prepared by ambient-drying and freeze-drying aerogel prepared in the same size tubes to show approximate size; (d) Photographs of seven ambient-dried aerogels with a cylinder shape and one aerogel on top of two flower petals; (e) An ambient-dried aerogel withstands 2 500 times its mass and shows good recoverability following loading and unloading[35]
图 7 (a) 油用油红、水用亚甲基蓝在L-海藻酸钠-纤维素纳米纤丝(L-SA/CN)气凝胶表面(插图为L-SA/CN气凝胶的油和水接触角图像)；(b) 用于测量L-SA/CN气凝胶油和有机溶剂的质量吸收能力；(c) 溶剂吸收变化[43]
CA—Contact angle
Figure 7. (a) Oil colored with oil red and water colored with methylene blue and then spotted on the surface of L-sodium alginate-cellulose nanofibers (L-SA/CN) aerogel (The insets were the oil and water contact angle images of the L-SA/CN aerogel); (b) Measuring the mass absorption capacity of L-SA/CN aerogel for oil and organic solvents; (c) Solvent absorption change[43]
表 1 纳米纤维素的化学制备方法
Table 1. Chemical preparation method of nanocellulose
Preparation method Benefit Drawback Hydrogen peroxide oxidation High product yield, simple environmental
procedures and lower costEasy incomplete oxidation, poor stability Carboxymethylation Lower preparation cost, milder preparation
conditions and less pollutionPreparation process is more complex, it requires a significant amount of water for dialysis Acid hydrolysis High and stable product yield, simple preparation
process and easy operationProduction of waste acids and residual impurities in the
reaction system, difficult to achieve recyclingPickering emulsion High product yield, exhibits good thermal stability Limited experimental environment, longer production cycles Ionic liquid Production process is environmentally green Most ionic liquids have high toxicity, they are
expensive and have high recycling costsAVAP Production cost is low, crystallinity is high, and chemical substances can be recycled SO2 is required during the pretreatment process,
limitations to the production conditionsNote: AVAP—Ethanol and SO2. 
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表 2 特殊浸润性纳米纤维素基气凝胶的水接触角(WCA)和油接触角(OCA)
Table 2. Water contact angle (WCA) and oil contact angle (OCA) of special wetting nanocellulose based aerogel
Raw materials WCA/(°) OCA/(°) Ref. Cellulose nanocrystal/Methyltrichlorosilane 148.5 0 [42] α-cellulose/Polylactic acid/1H, 1H, 2H, 2H-perfluorodecyltriethoxysilane 146.7 0 [44] α-cellulose/Polylactic acid/Methylhydrosiloxane 141.0 0 [45] α-cellulose/Dimethicone 160.0 0 [46] α-cellulose/Dodecanol 149.0 0 [47] α-cellulose/Methyltrimethoxysilane 132.6 0 [48] Cellulose nanocrystal/Polyvinyl alcohol/Methyltrichlorosilane 144.5 0 [49] α-cellulose/Trimethoxymethylsilane 160.0 0 [50] Nanofibrillated cellulose/Polydopamine/Dioctadecylamine 152.5 0 [32] Regenerated cellulose silica/Methyltrichlorosilane 160 0 [51] α-cellulose/Sodium sulfite sulfonation 0 150.0 [52] α-cellulose/Isocyanic acid/ Fluorocarbon surfactant 0 118.0 [53] Nanofibrillated cellulose/Sodium alginate 0 162.0 [54]
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