Abstract
In this work, Al2O3-SiO2 aerogels with low thermal conductivity and high strength were prepared using methyltriethoxysilane (MTES) as a silica precursor through the sol-gel method and high-temperature calcination. The effects of silica precursor on the thermal conductivity, chemical structure, and pore structure of aerogel as well as the effects of calcination temperature on the thermal conductivity, and mechanical properties of aerogel were investigated. The results indicated that MTES can reduce thermal conductivity by changing the microstructure of aerogel compared with tetraethyl orthosilicate (TEOS). The subsequent high-temperature calcination can further reduce thermal conductivity and improve mechanical properties. The prepared Al2O3-SiO2 aerogels have the characteristics of low thermal conductivity and high strength compared with previous reports. The Al2O3-SiO2 aerogels using MTES as silica precursor and calcined at 800 °C exhibited a density of 0.220 g/cm3, low thermal conductivity of 0.0232 W/(m·K), and a high compressive modulus of 74.29 MPa. In addition, the introduction of MTES can inhibit the sintering and phase transformation of alumina aerogel, and then improve the heat resistance of alumina aerogel. The specific surface areas of Al2O3-SiO2 aerogels before heat treatment, heat-treated at 1000 °C and heat-treated at 1200 °C are 639.68 m2/g, 337.28 m2/g, and 90.67 m2/g, respectively. This work provides a novel method for Al2O3-SiO2 aerogels to reduce thermal conductivity and improve mechanical properties.
Graphical Abstract
Highlights
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Compared with TEOS, Al2O3-SiO2 aerogels with MTES as silica precursor have lower thermal conductivity.
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High-temperature calcination can improve mechanical resistance and reduces the thermal conductivity of Al2O3-SiO2 aerogels.
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The addition of MTES can improve the heat resistance of Al2O3 aerogel.
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References
Lebedev AE, Menshutina NV, Khudeev II, Kamyshinsky RA (2020) Investigation of alumina aerogel structural characteristics at different «precursor-water-ethanol» ratio. J Non-Crystalline Solids 553:120475. https://doi.org/10.1016/j.jnoncrysol.2020.120475
Keysar S, Shter GE, Hazan YD, Cohen Y, Grader GS (1997) Heat Treatment of Alumina Aerogels. Chem Mater 9:2464–2467. https://doi.org/10.1021/cm970208s
Peng F, Jiang YG, Feng J, Liu FQ, Feng JZ, Li LJ (2022) Novel silica-modified boehmite aerogels and fiber-reinforced insulation composites with ultra-high thermal stability and low thermal conductivity. J Eur Ceram Soc 42:6684–6702. https://doi.org/10.1016/j.jeurceramsoc.2022.07.001
Almeida CMR, Ghica ME, Durães L (2020) An overview on Al2O3-SiO2-based aerogels. Adv Colloid Interface Sci 282:102189. https://doi.org/10.1016/j.cis.2020.102189
Zu GQ, Shen J, Zou LP, Wang WQ, Lian Y, Zhang ZH, Du A (2013) Nanoengineering Super Heat-Resistant, Strong Alumina Aerogels. Chem Mater 25:4757–4764. https://doi.org/10.1021/cm402900y
Zu GQ, Shen J, Wei XQ, Ni XY, Zhang ZH, Wang JC, Liu GW (2011) Preparation and characterization of monolithic alumina aerogels. J Non-Crystalline Solids 357:2903–2906. https://doi.org/10.1016/j.jnoncrysol.2011.03.031
Wu XD, Shao GF, Shen XD, Cui S, Wang L (2016) Novel Al2O3-SiO2 composite aerogels with high specific surface area at elevated temperatures with different alumina/silica molar ratios prepared by a non-alkoxide sol-gel method. RSC Adv 6:5611–5620. https://doi.org/10.1039/c5ra19764c
Peng F, Jiang YG, Feng JZ, Li LJ, Cai HF, Feng J (2020) A facile method to fabricate monolithic alumina-silica aerogels with high surface areas and good mechanical properties. J Eur Ceram Soc 40:2480–2488. https://doi.org/10.1016/j.jeurceramsoc.2020.01.058
Wang WQ, Zhang ZH, Zu GQ, Shen J, Zou LP, Lian Y, Liu B, Zhang F (2014) Trimethylethoxysilane-modified super heat-resistant alumina aerogels for high-temperature thermal insulation and adsorption applications. RSC Adv 4:54864–54871. https://doi.org/10.1039/C4RA08832H
Horiuchi T, Osaki T, Sugiyama T, Suzuki K, Mori T (2001) Maintenance of large surface area of alumina heated at elevated temperatures above 1300 °C by preparing silica-containing pseudoboehmite aerogel. J Non-Crystalline Solids 291:187–198. https://doi.org/10.1016/S0022-3093(01)00817-1
Shen J, Zhang XX (2021) Recent progress and applications of aerogels in China. J Sol-Gel Sci Technol 106:290–318. https://doi.org/10.1007/s10971-021-05639-2
Pierre AC, Pajonk GM (2002) Chemistry of Aerogels and Their Applications. Chem Rev 102:4243–4265. https://doi.org/10.1021/cr0101306
Nicholas L, Sotiriou-Leventis C, Zhang GH, Rawashdeh AMM (2002) Nanoengineering Strong Silica Aerogels. Nano Lett 2:957–960. https://doi.org/10.1021/nl025690e
Leventis N (2007) Three-Dimensional Core-Shell Superstructures: Mechanically Strong Aerogels. American Chemical Society. Acc Chem Res 40:874–884. https://doi.org/10.1021/ar600033s
Lu XP, Nilsson O, Fricke J, Pekala RW (1993) Thermal and electrical conductivity of monolithic carbon aerogels. J Appl Phys 73:581–584. https://doi.org/10.1063/1.353367
Fricke J, Lu X, Wang P, Büttner D, Heinemann U (1992) Optimization of monolithic silica aerogel insulants. Int J Heat Mass Transf 35:2305–2309. https://doi.org/10.1016/0017-9310(92)90073-2
Woignier T, Phalippou J (1988) Mechanical strength of silica aerogels. J Non-Crystalline Solids 100:404–408. https://doi.org/10.1016/0022-3093(88)90054-3
Zhong Y, Kong Y, Shen XD, Cui S, Yi XB, Zhang JJ (2013) Synthesis of a novel porous material comprising carbon/alumina composite aerogels monoliths with high compressive strength. Microporous Mesoporous Mater 172:182–189. https://doi.org/10.1016/j.micromeso.2013.01.021
Wu XD, Zhong Y, Kong Y, Shao GF, Cui S, Wang L, Jiao J, Shen XD (2015) Preparation and characterization of C/Al2O3 composite aerogel with high compressive strength and low thermal conductivity. J Porous Mater 22:1235–1243. https://doi.org/10.1007/s10934-015-0001-2
Zhong Y, Shao GF, Wu XD, Kong Y, Wang X, Cui S, Shen XD (2019) Robust monolithic polymer(resorcinol-formaldehyde) reinforced alumina aerogel composites with mutually interpenetrating networks. RSC Adv 9:22942–22949. https://doi.org/10.1039/c9ra03227d
Meador MAB, Fabrizio EF, Ilhan F, Dass A, Zhang GH, Vassilaras P, Johnston JC, Leventis N (2005) Cross-linking Amine-Modified Silica Aerogels with Epoxies:Mechanically Strong Lightweight Porous Materials. Chem Mater 17:1085–1098. https://doi.org/10.1021/cm048063u
Zu GQ, Shen J, Wang WQ, Zou LP, Lian Y, Zhang ZH, Liu B, Zhang F (2014) Robust, Highly Thermally Stable, Core-Shell Nanostructured Metal Oxide Aerogels as High-Temperature Thermal Superinsulators, Adsorbents, and Catalysts. Chem Mater 26:5761–5772. https://doi.org/10.1021/cm502886t
Ma J, Ye F, Yang CP, Ding JJ, Lin SJ, Zhang B, Liu Q (2017) Heat-resistant, strong alumina-modified silica aerogel fabricated by impregnating silicon oxycarbide aerogel with boehmite sol. Mater Des 131:226–231. https://doi.org/10.1016/j.matdes.2017.06.036
Hou XB, Zhang RB, Wang BL (2018) Novel self-reinforcing ZrO2-SiO2 aerogels with high mechanical strength and ultralow thermal conductivity. Ceram Int 44:15440–15445. https://doi.org/10.1016/j.ceramint.2018.05.199
Yu HJ, Tong ZW, Qiao YC, Yang ZC, Yue S, Li XL, Su D, Ji HM (2020) High thermal stability of SiO2-ZrO2 aerogels using solvent-thermal aging. J Solid State Chem 291:121624. https://doi.org/10.1016/j.jssc.2020.121624
Liu DB, Zhang C, Xue YH (2023) Synthesis and characterization of sol-gel derived lanthanum zirconate ceramic aerogels toward ultralow thermal conductivity. Mater Sci Eng B 287:116127. https://doi.org/10.1016/j.mseb.2022.116127
Baumann TF, Gash AE, Chinn SC, Sawvel AM, Maxwell RS, Satcher JH (2005) Synthesis of High-Surface-Area Alumina Aerogels without the Use of Alkoxide Precursors. Chem Mater 17:395–401. https://doi.org/10.1021/cm048800m
Peng F, Jiang YG, Feng J, Cai HF, Feng JZ, Li LJ (2021) Thermally insulating, fiber-reinforced alumina–silica aerogel composites with ultra-low shrinkage up to 1500 °C. Chem Eng J 411:128402. https://doi.org/10.1016/j.cej.2021.128402
Wu XD, Shao GF, Cui S, Wang L, Shen XD (2015) Synthesis of a novel Al2O3-SiO2 composite aerogel with high specific surface area at elevated temperatures using inexpensive inorganic salt of aluminum. Ceram Int 42:874–882. https://doi.org/10.1016/j.ceramint.2015.09.012
Himmel B, Gerber T, Biirger H, Holzhfiter G, Olbertz A (1995) Structural characterization of SiO2-A12O3 aerogels. J Non-Crystalline Solids 186:149–158. https://doi.org/10.1016/0022-3093(95)00045-3
Aravind PR, Mukundan P, Pillai PK, Warrier KGK (2006) Mesoporous silica-alumina aerogels with high thermal pore stability through hybrid sol-gel route followed by subcritical drying. Microporous Mesoporous Mater 96:14–20. https://doi.org/10.1016/j.micromeso.2006.06.014
Yi XB, Zhang LL, Wang FY, Shen XD, Cui S, Zhang J, Wang XC (2014) Mechanically reinforced composite aerogel blocks by self-growing nanofibers. RSC Adv 4:48601–48605. https://doi.org/10.1039/c4ra07383e
Thommes M, Kaneko K, Neimark AV, Olivier JP, Rodriguez-Reinoso F, Rouquerol J, Sing KSW (2014) Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report). Pure Appl Chem 87:1051–1069. https://doi.org/10.1515/pac-2014-1117
Hegde ND, Rao AV (2007) Physical properties of methyltrimethoxysilane based elastic silica aerogels prepared by the two-stage sol-gel process. J Mater Sci 42:6965–6971. https://doi.org/10.1007/s10853-006-1409-5
Wang XD, Tian YL, Yu CL, Liu L, Zhang Z, Wu Y, Shen J (2022) Organic/inorganic double-precursor cross-linked alumina aerogel with high specific surface area and high-temperature resistance. Ceram Int 48:17261–17269. https://doi.org/10.1016/j.ceramint.2022.02.287
Wu LA, Qiao XS, Cui S, Hong ZL, Fan XP (2015) Synthesis of monolithic aerogel-like alumina via the accumulation of mesoporous hollow microspheres. Microporous Mesoporous Mater 202:234–240. https://doi.org/10.1016/j.micromeso.2014.10.015
Poco JF, Satcher Jr JH, Hrubesh LW (2001) Synthesis of high porosity, monolithic alumina aerogels. J Non-Crystalline Solids 285:57–63. https://doi.org/10.1016/S0022-3093(01)00432-X
Hayase G, Kugimiya K, Ogawa M, Kodera Y, Kanamori K, Nakanishi K (2014) The thermal conductivity of polymethylsilsesquioxane aerogels and xerogels with varied pore sizes for practical application as thermal superinsulators. J Mater Chem A 2:6525–6531. https://doi.org/10.1039/c3ta15094a
Lee OJ, Lee KH, Yim TJ, Kim SY, Yoo KP (2002) Determination of mesopore size of aerogels from thermal conductivity measurements. J Non-Crystalline Solids 298:287–292. https://doi.org/10.1016/S0022-3093(01)01041-9
Acknowledgements
The authors would like to thank the National Natural Science Foundation of China (12172229) for their financial.
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This work was supported by the National Natural Science Foundation of China (12172229).
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All authors contributed to the study conception and design. Material preparation, data collection and analysis were performed by Guoqi Li, Li Hu, Kai Zhang, Sifan Hou and Jinpeng Fan. The first draft of the manuscript was written by Guoqi Li and all authors commented on previous versions of the manuscript. All authors read and approved the final manuscript.
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Li, G., Hu, L., Zhang, K. et al. Synthesis of Al2O3-SiO2 aerogels with low thermal conductivity and high strength by methyltriethoxysilane as a silica precursor. J Sol-Gel Sci Technol 108, 35–46 (2023). https://doi.org/10.1007/s10971-023-06164-0
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DOI: https://doi.org/10.1007/s10971-023-06164-0