Progress in research and application of special wettable composite materials based on in situ polymerization
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摘要: 本文总结了基于原位聚合构造特殊润湿性复合材料的最新进展，首先介绍了基于特殊润湿性的机制及自然界中的特殊润湿性现象，指出人工构造特殊润湿性复合材料的常见方法，举例说明了各类方法的优势与缺陷，并指出原位聚合法构造特殊润湿性复合材料的原理及其优势。其次，以原位聚合法为核心，讨论了3种类型的特殊润湿性复合材料构造现状，包括特殊润湿性涂层复合材料、特殊润湿性纤维复合材料、特殊润湿性多孔复合材料。同时还讨论了原位聚合构造特殊润湿性复合材料在油水分离、水雾收集、液滴操控等领域的应用现状，对其作用机制、材料类型、应用性能进行了综述。最后总结了原位聚合构造特殊润湿性复合材料目前面对的挑战和未来前景。Abstract: In this paper, the latest development of special wettable composite materials based on in situ polymerization is summarized. Firstly, the mechanism of special wettability and special wettable phenomenon in nature are introduced, the common methods of constructing special wettable composite materials are pointed out, and the advantages and disadvantages of these methods are illustrated with examples. Secondly, three types of special wettable composite materials are discussed based on in situ polymerization, it includes special wettable coating composite materials, special wettable fiber composite materials and special wettable porous composite materials. At the same time, the application of special wettable composite materials constructed by in situ polymerization in the fields of oil-water separation, water mist collection and droplet control is also discussed, the mechanism of action, material type and application performance were reviewed. Finally, the challenges and prospects of special wettable composite materials constructed by in-situ polymerization are summarized.
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Key words:
- in situ polymerization /
- special wettability /
- surface /
- polymer /
- composite materials
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图 1 自然界中的特殊润湿现象：(a)荷叶表面[1]；(b)玫瑰花瓣[2]；(c)蝴蝶翅膀[3]；(d)仙人掌刺[4]；(e)沙漠甲虫背甲[5]；(f)猪笼草内表面[6-7]
RO—Rolling orientationally
Figure 1. Special wettability in nature: (a) Lotus leaf surface[1]; (b) Rose petals[2]; (c) Butterfly wings[3]; (d) Cactus thorn[4]; (e) Desert beetle carapace[5]; (f) Pitcher grass inner surface[6-7]
图 2 (a)基于SiC、多巴胺(DOPA)、十八胺(ODA)的超疏水莫来石织物制备过程示意图[34]；(b)基于异佛尔酮二异氰酸酯(IPDI)、SiO2及聚(脲-甲醛)纳米颗粒(PUF NPs)的超疏水微胶囊制备示意图[35]
Figure 2. (a) Schematic illustration of superhydrophobic mullite fabric based on SiC, dopamine (DOPA) and octadecylamine (ODA)[34]; (b) Preparation of superhydrophobic microcapsules based on isophorone diisocyanate (IPDI) , SiO2 and poly(urea formaldehyde) nanoparticles (PUF NPs)[35]
图 3 (a)基于甲基三氯硅烷(MTS)、过乙烯基三氯硅烷(VTS)的3种超疏水聚酯(PET)纤维结构制备路径示意图[40]；(b)基于纤维素乙酸酯(CA)、含氟聚苯并噁嗪(F-PBZ)、多聚甲醛单体/SiO2纳米颗粒(BAF-tfa/SiO2 NPs)的静电纺超疏水/超亲油纳米纤维膜合成示意图[41]
Figure 3. (a) Diagram of the preparation path for three types of superhydrophobic polyester (PET) fiber structures based on methyl trichlorosilane (MTS) and polyvinyl trichlorosilane (VTS)[40]; (b) Diagram of electrospinning superhydrophobic/superhydrophilic nanofiber membranes based on cellulose acetate (CA), fluorinated polybenzoxazine (F-PBZ), paraformaldehyde/SiO2 nanoparticles (BAF-tfa/SiO2 NPs)[41]
图 4 (a) 基于纤维素纳米纤维与壳聚糖气凝胶基质(m-CNS)、(3-巯基丙基)三甲氧基硅烷(MPTMS)、聚二甲基硅氧烷(PDMS)的超疏水复合气凝胶(P-CNS)制造过程图解[47]；(b) 基于DOPA、N-(3, 4-二羟基苯乙基)丙烯酰胺(DBDOPA)的超疏水聚氨酯(PU)海绵合成示意图[48]；(c) 基于聚乙烯醇(PVA)、海藻酸钠(SA)、苯胺单体及硫酸铵溶液(APS)浸泡的超亲水复合气凝胶制备过程示意图[49]
Figure 4. (a) Diagram of superhydrophobic composite aerogel (P-CNS) based on cellulose nanofibers and chitosan aerogel matrix (m-CNS), (3-mercaptopropyl) trimethoxysilane (MPTMS) and polydimethylsiloxane (PDMS)[47]; (b) Diagram of superhydrophobic polyurethane (PU) sponge synthesis based on DOPA and N-(3, 4-dihydroxyphenylethyl) acrylamide (DBDOPA)[48]; (c) Schematic illustration of the preparation process for superhydrophilic composite aerogel based on polyvinyl alcohol (PVA), sodium alginate (SA) , aniline momomer and ammonium sulfate solution (APS) immersion
图 5 (a)超疏水共轭微孔聚合物涂层海绵(CMP@sponges)制备及其连续油水分离示意图[64]；(b)超疏水不锈钢网(SSW)的原位热聚合 (ISTP)制备过程及其油水分离应用[65]
Figure 5. (a) Schematic illustration for superhydrophobic conjugated microporous polymer-coated sponges (CMP@sponges) and its schematic diagram of continuous oil-water separation[64]; (b) In situ thermal polymerization (ISTP) preparation of superhydrophobic stainless steel mesh (SSW) and its application in oil-water separation[65]
图 6 (a) 基于二乙烯苯(DVB)的超疏水聚二乙烯苯织物(PDVB@fabric)制备过程示意图；原始织物(b)和PDVB@fabric (c)的SEM图像(右上角插图为相应的水接触角(WCA)光学图像)；(d) 具有不对称润湿性的Janus织物制备路线图[69]；(e) 磁性可变形超疏水织物的制备路径图[70]
Figure 6. (a) Schematic illustration for preparation process of superhydrophobic polydivinylbenzene fabric (PDVB@fabric) based on diethylene benzene (DVB); SEM images of original fabric (b) and PDVB@fabric (c) (Inset on the top right are the corresponding WCA optical photos); (d) Schematic illustration of Janus fabric with asymmetric wettability[69]; (e) Schematic illustration of magnetic deformable superhydrophobic fabric[70]
图 7 (a) 基于F-PBZ、4, 4-(六氟异丙基)二苯酚(BAF)、SiO2 NPs、ODA的超疏水薄膜制备路径及单体合成路线示意图[76]；(b) 电纺聚氨酯(PU-E)、多层纳米薄片(MXene)、DOPA修饰的聚多巴胺(PDA) Janus膜(PU-E/MXene@PDA-PU)制备过程示意图；(c) 当水滴滴在Janus膜的疏水层和反向上时Janus膜实时定向水传输现象[77]
Figure 7. (a) Schematic illustration of the preparation path and monomer synthesis route of superhydrophobic films based on F-PBZ, 4, 4-(hexafluoroisopropyl)diphenol (BAF), SiO2 NPs and ODA[76]; (b) Schematic diagram of electrospun polyurethane (PU-E), multi-layer nanosheets (MXene), DOPA modified polydopamine (PDA) Janus film (PU-E/MXene@PDA-PU); (c) Real-time directional water transport phenomena of the Janus membrane when waterdroplets were dripped on its hydrophobic layer and the reverse direction[77]
图 8 基于3-氨基丙基三乙氧基硅烷(AEMO)、甲基丙烯酸甲酯共聚丙烯酸3-(三甲氧基甲硅烷基)丙酯(MMA-co-KH570)修饰的智能pH响应织物的合成过程及其在可控油水分离中的应用示意图[79]
Figure 8. Schematic illustration of intelligent pH responsive fabric modified with 3-aminopropyltriethoxysilane (AEMO) and methyl methacrylate co polyacrylic acid 3-(trimethoxysilyl) propyl ester (MMA-co-KH570) and it applications in controllable oil/water separation[79]
图 9 基于抗坏血酸(VC)及氧气等离子体处理的三氟甲基/氧化铜智能自修复超疏水棉织物制备示意图(a)及其表面氧气等离子体蚀刻高温自愈示意图(b)[80]
Figure 9. Schematic illustration of intelligent self-healing superhydrophobic cotton fabric based on ascorbic acid (VC) and oxygen plasma treatment (a) and its surface oxygen plasma etching with high temperature self-healing (b)[80]
表 1 特殊润湿性复合材料的制备方法比较
Table 1. Comparison of preparation methods for special wettable composite materials
Method Material Principle Advantage Disadvantage Ref. Femtosecond laser Superhydrophobic memory surface Femtosecond laser directly treats the surface of the material to form micro-columns Simple, stability High equipment cost [8] Etching Aluminum plate superhydrophobic surface Chemical etching aluminum plate structure roughness, and then use low surface energy reagent modification Fast, stable Perfluorinated compounds are used [9] Template Underwater super hydrophobic oil film A hydrophilic casting solution is used to form a film on a polytetrafluoroethylene substrate Simple operation,
not harsh application conditionsUnstable, the product
is prone to structural damage, which has certain requirements for the synthesis system[10] Sol-gel Superhydrophobic coating The low surface energy precursor and the roughness component are mixed in the liquid phase to form the gel Good chemical uniformity and uniform microscale distribution Poor durability and
high cost[11] Induced deposition Superhydrophobic/
superhydrophilic patternUnder the action of laser, thin films are formed on the glass substrate, and regular repeated geometric patterns are formed
by depositionHigh speed and
wear resistanceIt needs to be carried out at high temperatures, and
some substrates cannot withstand it, which poses risks[12]
Layer by layer self-assemblyLubricating superhydrophobic patterned surfaces Through the strong interaction of the components in the solution, low surface energy compounds are driven to spontaneously associate and form superhydrophobic surfaces on the substrate Simple operation
and high product controllabilityMultiple steps, time-consuming [13] In-situ polymerization Superhydrophobic cotton fabric Based on the thermal initiation and non volatility of ionic liquid precursors, a
sturdy polymer layer can be in-situ generated in an air atmosphere and
coated onto the fabricSimple and convenient operation, low cost,
and strong product durability
It is difficult to regulate the polymerization accurately[14] 
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表 2 油水分离用特殊润湿性复合材料性能对比
Table 2. Performance comparison of special wettability composite materials for oil-water separation
Material Contact angle Separation object Separation efficiency Separation flux/(L·m−2·s−1) Ref. CMP@sponges WCA/OCA: 153.92°/0° Diesel oil/water, Gasoline/water, Toluene/water emulsion 98.98%-99.81% 10.2-16.3 [64] Superhydrophobic SSM WCA/OCA: 158°/0° n-hexane/water 99.8% 15.65 [65] P(MMA-co-GMA) membrane WCA/OCA: 0°/150° (Underwater) n-hexane in water emulsion 98.3% 90 [66] SP-PVDF membrane WCA/OCA: 168.4°/
162.3° (Underoil)n-hexane in water emulsion,
n-hexane, water in n-hexane emulsion99.4% 484.8/599.3 [67] Notes: WCA—Water contact angle; OCA—Oil contact angle; P(MMA-co-GMA)—Poly(methyl methacrylate-co-glycidyl methacrylate); SP-PVDF—Silica decoration-poly(vinylidene fluoride).
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