Supersaturated wood-based biomass porous materials for oil/water separation
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摘要: 餐厨垃圾和工业废水中油和水的高效分离仍具挑战性。传统的油水分离技术主要包括重力沉降、离心、吸附、浮选和电化学等，存在着分离效率低、分离不彻底等问题。如何高效且低成本地实现油水分离已成为当前研究的热点。木材是一种可持续发展的生物材料，并且自身具有多级孔隙结构和丰富羟基官能团，其衍生物具备超浸润特性，因此其有望成为一种新型的油水分离材料。通过优化木材内部细胞孔径，对其进行超疏水或超亲水表面润湿性改性，进而促进木质基复合材料对油水混合乳液的物理化学过滤和吸附，最终实现废水中油污的有效去除。本文对油水混合物及含油废水的特性及危害进行了概述，并系统综述了具有超浸润特性(超亲水/水下超疏油、超疏水/超亲油)的木基多孔过滤膜和吸附材料用于分离含油废水的构建策略，概述了近年来具有超浸润特性的木基生物质多孔材料在油水分离领域的研究进展，并总结了这种材料存在的问题，展望了未来潜在的研究方向。Abstract: The efficient separation of oil and water from kitchen waste and industrial wastewater remains challenging. Traditional oil-water separation techniques mainly include gravity settling, centrifugation, adsorption, flotation and electrochemistry, which suffer from low separation efficiency and incomplete separation. How to realize oil-water separation with high efficiency and low cost has become a hot spot of current research. Wood is a sustainable biomaterial and has a multilevel pore structure and abundant hydroxyl functional groups, and its derivatives have super-wetting properties, so it is expected to be a new type of oil-water separation material. By optimizing the internal cell pore size of wood and modifying its superhydrophobic or superhydrophobic surface wettability, the physicochemical filtration and adsorption of wood-based composites on oil-water mixed emulsions can be promoted, and the effective removal of oil from wastewater can be realized. In this paper, the characteristics and hazards of oil-water mixtures and oily wastewater are summarized, and the construction strategies of wood-based porous filtration membranes and adsorbent materials with super-wetting properties (superhydrophobic/underwater superoleophobicity, superhydrophobic/superoleophilic) for the separation of oil-containing wastewater are reviewed systematically, and the progress of the research on wood-based biomass porous materials with super-wetting properties in the field of oil-water separation in recent years is summarized and the problems and potential future research directions of such materials are summarized and outlooked.
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图 2 (a)木材细胞壁的分层结构[25]；(b)英国橡木(栎)阔叶木的SEM图像；(c)苏格兰松(樟子松)针叶木的SEM图像[15]；(d)吸附法油水分离原理图[26]；(e)过滤法油水分离原理图[27]
M, P, S1, S2, S3—Middle layer, primary wall, secondary wall layer 1, 2, 3; W/O—Water-in-oil; PSP—Polystyrene pyridine; θ—Water contact angle
Figure 2. (a) Hierarchical structure of wood cell wall[25]; (b) SEM image of English oak (Quercus serrata) broadleaf wood; (c) SEM image of Scots pine (Cinnamomum camphora) coniferous wood[15]; (d) Schematic diagram of the adsorption method of oil-water separation[26]; (e) Schematic diagram of the filtration method of oil-water separation[27]
图 3 天然木材(a)和木膜(b)的实物和SEM图像(径向切向面和纵向切向面)；(c)使用木基过滤膜分离乳化油图片；(d) 乳化油分离前后效果图[2]；(e) Ag/木材过滤膜从水中去除有机染料亚甲基蓝(MB)；(f)过滤有机染料MB后的木基材料横切面图片；(g)银纳米颗粒(AgNPs)在木材管孔内对MB的催化降解示意图[30]；(h)原巴尔沙木和Ag@Wood反复过滤MB溶液前后的照片[6]
Figure 3. Physical and SEM images (radial tangential plane and longitudinal tangential plane) of natural wood (a) and wood membranes (b); (c) Pictures of emulsified oil separation using wood-based filtration membranes; (d) Before and after effect of emulsified oil separation[2]; (e) Removal of organic dyes methylene blue (MB) from water by Ag/wood filtration membranes; (f) Pictures of cross-sections of the wood-based materials after filtration of organic dyes MB; (g) Schematic diagram of the Ag nanoparticles (AgNPs) in the catalytic degradation of MB within the pores of wood tubes[30]; (h) Photographs of raw balsa wood and Ag@wood before and after repeated filtration of MB solution[6]
图 4 (a)真空浸渍和表面改性后的超疏水木片制备工艺和油水乳液分离示意图；(b)超疏水木材切片的表面FE-SEM图像[31]；(c)聚二乙烯基苯(PDVB)木膜对酸、碱、盐、水、可乐、咖啡、油等的润湿效果图；(d) PDVB木膜和天然木片的柔韧性对比图[33]；(e)聚二甲基硅氧烷(PDMS)@TiO2木材的制备过程和对油水混合物的分离效率统计图[34]
Figure 4. (a) Schematic diagram of the preparation process and oil-water emulsion separation of superhydrophobic wood slices after vacuum impregnation and surface modification; (b) Surface FE-SEM images of the superhydrophobic wood slices[31]; (c) Wetting effect diagram of PDVB(super-hydrophobic polydivinylbenzene)-wood membranes on acids, alkalis, salts, water, cola, coffee, and oils, etc.; (d) Comparison of flexibility between the PDVB-wood membranes and natural wood slices[33]; (e) Statistical graph of the preparation process and separation efficiency of polydimethylsiloxane (PDMS)@TiO2 wood for oil-water mixtures[34]
图 5 (a)椴木(BW)/聚螺吡喃(PSP)膜的油/水分离工艺[27]；(b) Janus木膜(JW)对油水混合物的选择性分离；(c) Janus木膜疏水(HO)表面和亲水(HI)表面实物图片；(d) Janus木膜HO表面分别对油和水的接触角；(e) Janus木膜HI表面的水下超疏油图片[36]
Figure 5. (a) Oil/water separation process with basswood (BW)/poly(spiropyran) (PSP) membranes[27]; (b) Selective separation of oil-water mixtures by Janus wood (JW) membranes; (c) Physical pictures of the hydrophobic (HO) surface and the hydrophilic (HI) surface of Janus wood membranes; (d) Contact angle of the HO surface of Janus wood membranes for oil and water, respectively; (e) Picture of the underwater super-hydrophobicity of the HI surface of Janus wood membranes[36]
SPAM—Sulfonated polyacrylamide
图 6 (a)木基海绵(WS)和硅烷化木基海绵(SWS)润湿性对比图；(b)不同木材样品及WS的红外图谱；(c)通过化学成分分析获得的不同木材样品及纤维素WS中纤维素、半纤维素和木质素的相对含量[40]；(d) Wood/共价有机框架(COF)的制造工艺示意图[26]；(e) 25℃ 和70℃下原油的黏度及PDMS@还原氧化石墨烯(GSH)木基材料对高黏度原油的吸附图片[42]
Figure 6. (a) Comparison of the wettability of wood-based sponges (WS) and silanised wood-based sponges (SWS); (b) Infrared spectra of different wood samples and WS; (c) Relative contents of cellulose, hemicellulose, and lignin in different wood samples and cellulose-based WS obtained by chemical composition analysis[40]; (d) Schematic diagram of the fabrication process of wood/covalent organic frameworks (COF)[26]; (e) Viscosity of crude oil and adsorption pictures of PDMS@reduced graphene oxide wood (GSH) wood-based materials on high viscosity crude oil at 25℃ and 70℃[42]
APTES—Silylation reaction of (3-aminopropyl)trimethoxysilane; DI—Deionized water
表 1 过滤型木基油水分离材料性能对比
Table 1. Comparison of the performance of filtered wood-based oil-water separation materials
Oil-water separation method Separation efficiency/% Flux/(L·m−2·h−1) Cycle Ref. Cetane/water mixture 99.90 3500 Not mentioned [29] Oil/water mixtures 99.42 462 10/efficiency maintained at 99% [2] Oil/water mixtures 99.00 2600 Not mentioned [30] Oil/water mixtures 98.89 4776 Not mentioned [6] Oil/water mixtures 98.00 11 6/efficiency maintained at 98% [31] Chloroform/water mixture 99.20 460 10/efficiency maintained at 98.7% [32] Hexane/water mixture 99.98 8829 20/efficiency maintained at 99.98% [33] Toluene/water mixture 93.40 4889 Not mentioned [34] Oil/water mixtures 97.50 Not mentioned Not mentioned [35] Toluene/water mixture 99.00 470 Not mentioned [36] 
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表 2 吸附型木基油水分离材料性能对比
Table 2. Comparison of performance of adsorbent wood-based oil-water separation materials
Oil-water separation method Water/oil absorption/(g·g−1) Cycle Ref. Crude oil/water mixtures 15.0 12 [39] Silicone oil/water mixture 41.0 Not mentioned [40] Dichloromethane/water mixture 5.2 11-14 [41] Cyclohexane/water mixture 930.0 20 [26] Crude oil/water mixtures 1.8 Not mentioned [42] Crude oil/water mixtures 11.2 10 [43]
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