Research status and analysis of cement and geopolymer hydrophobic composites
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摘要: 混凝土的长期耐久性问题是其面临的主要问题之一，造成耐久性破坏的主要原因是水在混凝土的多孔结构中的迁移，使有害离子更容易进入基材内部。采用超疏水材料对水泥及地聚物进行改性复合处理，赋予其超疏水特性，避免水分在其孔隙中的传输，从而防止有害离子的迁移及侵蚀，增强混凝土的耐久性。本文总结了目前研究当中对于水泥及地聚物胶凝材料超疏水改性方法，包括整体改性和表面改性两种；归纳了整体改性方式中超疏水改性剂加入到水泥及地聚物混凝土中的改性机制，以及与无机物基体中的连接键合方式；概括了目前研究当中表面改性常用的改性方法，包括喷涂法、浸渍法、模板法等，并分析了表面改性机制。与表面改性所得到的超疏水复合涂层相比，整体改性的水泥及地聚物基复合材料在实际应用场景当中具有更大的优势。此外，分析了疏水改性后对复合材料润湿性、防水性、抗压性能以及防腐性能的影响规律，发现其抗压强度降低了约20%~60%。最后，阐述了水泥及地聚物复合材料的疏水改性研究中存在的一些问题并对未来的研究方向进行了展望，建议从体积型超疏水、提高抗压强度、成本控制及疏水外加剂在材料内部实现均匀化分散等方面进行研究。Abstract: The long-term durability of concrete is one of the main problems it faces, and the main cause of durability damage is the migration of water in the porous structure of concrete, which makes it easier for harmful ions to enter the interior of the substrate. Modifying the cement and geopolymer with superhydrophobic materials is a valid method to avoid the transmission of water, thereby preventing the migration of harmful ions and increased its durability of concrete. This review summarized the superhydrophobic modification methods of cement and geopolymer cementitious materials and categorized into superhydrophobic surface and bulk modification; the modification mechanism of superhydrophobic modifier added to cement and geopolymer and their bonding mode with inorganic matrix in the internal modification method. Besides, the modification methods commonly used for surface modification in the present research are summarized, divided into external coating, maceration, template method, etc., and the surface modification mechanism is analyzed. Compared with the superhydrophobic composite coatings, the monolithically modified cement and geopolymer matrix composites have greater advantages in practical application scenarios. In addition, the effects of hydrophobic modification on the wettability, waterproofing, compressive properties and anti-corrosion properties of composites are concluded, and their compressive strength was reduced by about 20%~60%. Finally, some problems in the research of hydrophobic modification of cement and geopolymer composites are described and the future research direction is prospected, and it is suggested to carry out research on volumetric super-hydrophobicity, improvement of compressive strength, cost control, and homogeneous dispersion of hydrophobic admixture inside the material.
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图 1 水泥或地聚物材料的改性机制
Figure 1. Mechanisms for modification of cement or geopolymer materials
图 2 水泥基材料中不同改性剂的改性机制图
Figure 2. Modification mechanism diagram of different modifiers in cementitious materials
图 3 地聚物材料中不同改性剂的改性机制图
Figure 3. Modification mechanism diagram of different modifiers in geopolymer material
图 4 水泥/地聚物改性后孔隙率变化图
Figure 4. Changes in porosity after cement /geopolymer modifications
图 5 超疏水水泥基材料28 d抗压强度降低程度
Figure 5. Degree of reduction in 28 d compressive strength of superhydrophobic cementitious materials
图 6 未疏水改性和疏水改性水泥基混凝土的SEM对比图
Figure 6. SEM comparison of unhydrophobically modified and hydrophobically modified cementitious concrete
图 7 超疏水地聚物材料28 d抗压强度的升降程度
Figure 7. Degree of elevation and reduction of 28 d compressive strength of superhydrophobic geopolymer materials
表 1 不同改性方法对水泥及地聚物材料表面改性的优劣对比
Table 1. Comparison of advantages and disadvantages of different modification methods for surface modification of cement and geopolymer materials
Cementitious types Coating preparation Method Test method WCA/(°) Surface coating of cementitious materials DC-30 (contains mainly octane-silane and siloxane)[27] External coating Abrasion of 200 grit sandpaper for 20 m under a load of 2.5 kpa 158 Aqueous solution of sodium laurate[33] Maceration — 150 Sandpaper and polydimethylsiloxane [35] Template — 142 Triethoxyoctysilane and diatomaceous earth low
surface materials [36]External coating Sandpaper for 18.00 m under 24.50 kpa load 158 Organosilicon functionalized Al2O3 + solid resins materials [37] External coating 400 cm abrasion of sandpaper under 200 g load 165 Surface coating of geopolymer materials Polymethylhydrosiloxane [40] External coating — 161 Polydimethylsiloxane solution containing
polytetrafuoroethylene /
stearic acid and fly ash [39]Maceration Polydimethylsiloxane -only coatings have higher adhesion than polydimethylsiloxane coatings containing fly ash 159 Notes: WCA—water contact angle 
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表 2 整体改性对超疏水水泥及地聚物材料的水化/聚合作用的影响
Table 2. Effect of Integral Modification on the Hydration/Polymerization of Superhydrophobic Cementitious and Geopolymer Materials
Cementitious types Coating preparation Test method Effects on hydration/polymerization WCA/(°) ordinary silicate cement[62] non-toxic lauric acid and covering metal mesh XRD Integral superhydrophobic concrete has fewer hydration products than ordinary silicate concrete. 153 magnesium oxychloride based cement [48] hydroxyl-terminated polydimethylsil-oxane XRD、SEM Nanoscale needle-like phases are covered by hydrophobic silicone rubber. >150 ordinary silicate cement[50] functionalization of SiO2 with fluorine-free silanes XRD、FTIR Silanes in superhydrophobic powders react with cement hydration products to slow down the cement hydration rate. 153.8 ordinary silicate cement[61] Stearic acid modified fly ash TGA Fly ash can increase the water-cement ratio and facilitate cement hydration, providing more nucleation sites for cement hydration. 93.2 ordinary silicate cement[64] nano-silica and isobutyl-triethoxysilane isothermal calorimeter Silane can mitigate the loss of flowability caused by nano-silica to some extent, while nano-silica can completely compensate for the delay of silane in the early hydration process. 153.5 fly ash based polymer materials [53] polymethylhydrosiloxane Hot Plate Method Thermal conductivity decreases with increasing amount of polymethylhydrosiloxane, and the higher the porosity, the lower the bulk density. 161 fly ash based polymer materials [58] polymethylhydrosiloxane TEM Grafting of poly(methylhydrosiloxane) is not exactly proportional to the amount of geopolymer produced. 152 fly ash-slag base polymer materials [56] isooctyltriethoxysilane BSE、EDX Silanes slow down the hydration kinetics, while the increase in the modulus of the alkali activator inhibits the formation of hydration products. 118.1 slag mortar [57] polydimethylsiloxane MIP、SEM、EDS Polydimethylsiloxane increases internal defects in the body. 128
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表 3 不同改性剂的超疏水水泥基材料的接触角和滑动角
Table 3. WCA and SA of superhydrophobic cementitious materials with different modifiers
Cementitious types Hydrophobic Modifiers Modification type WCA/(°) SA/(°) ordinary silicate cement [62] 0.8 wt% non-toxic lauric acid Integral 153 10 magnesium oxychloride based cement [48] 6 wt% hydroxyl-terminated polydimethylsiloxane Integral ＞150 ＜10 high belite sulphoaluminate cement [65] lauric acid Integral 153.2 — ordinary silicate cement [66] 1H, 1H, 1H, 2H-perfluorodecyl-triethoxysilane Surface 163.3 — ordinary silicate cement [67] contains mainly octane-silane and siloxane Surface 160±1 6.5±0.5 ordinary silicate cement[68] hydrophobic silica nanoparticles Surface 160 1.7 Notes: SA—sliding angle
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表 4 不同改性剂的超疏水地聚物材料的接触角和滑动角
Table 4. WCA and SA of superhydrophobic geopolymer materials with different modifiers
Geopolymer types Hydrophobic Modifiers Modification type WCA/(°) SA/(°) calcined clay and slag [69] 5 wt% polydimethylsiloxane Integral 120 — fly ash [70] 5 wt% stearic acid Integral 96.67 — metakaolin[71] 5 wt% polydimethylsiloxane Integral 127.5 — metakaolin [40] polymethylhydrosiloxane Surface 161 2 dust/silicate cement [72] polydimethylsiloxane Surface 154.1 6.1
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表 5 超疏水水泥及地聚物复合材料的吸水率降低程度和原因
Table 5. Extent and causes of water absorption reduction in superhydrophobic cement and geopolymer composites
categories Materials and Dosages Modification type water absorption/% reason ordinary silicate cement 1 wt% stearic acid[74] Integral −86% Surface water is rejected by the surface. 1.4 wt%
cetyltrimethoxysilane[76]Integral −86% The internal inorganic mineralized layer further prevents water intrusion through a relatively dense micro/nano-scale two-layer structure. 5 wt% SiO2 silica solution[30] Surface −90% Hydration products and some unhydrated nanoparticles can clog capillaries, thus blocking water transfer paths. geopolymer materials 60 wt% iron ore tailings +1.5 wt% stearic acid[79] Integral −43% The particle size of superhydrophobic iron ore tailing is much smaller than that of sand, and the fine superhydrophobic iron ore tailing can easily fill up the pores of the mortar, making the mortar more dense and leading to a decrease in water absorption. 10 wt% hydrophobic metakaolin + polydimethylsiloxane [55] Integral −26%~−27.6% Weakening of the capillary's ability to absorb and hold water. polydimethylsiloxane + polypropylene fiber [81] Integral −70% Polypropylene fiber easily adsorbs polydimethylsiloxane but does not easily trap water vapor, blocking the water vapor diffusion channel.
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表 6 超疏水水泥及地聚物材料的腐蚀电位和腐蚀电流密度
Table 6. Corrosion potential and corrosion current density of superhydrophobic cement and geopolymer materials
Concrete material name Hydrophobic Modifiers Ecror /V Icorr/(A·cm−2) hardened cement mortar [47] polydimethylsiloxane − 0.07204 4.10×10−8 superhydrophobic surface for concrete [29] stearic acid − 0.28225 — superhydrophobic concrete [82] containing silane and siloxane — 7.702×10−6 superhydrophobic concrete [52] lauric acid −0.477 1.26×10−5 superhydrophobic concrete [96] stearic acid −0.173 5.921×10−7 superhydrophobic iron ore tailings [79] stearic acid −0.321 1.451×10−6 Notes：Ecror is a mixed electrode potential determined by the cathode and anode reactions on the corroded surface; Icorr is the amount of electricity per unit area per unit time of cathodic protection on a metal electrode.
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