Abstract
Herein, a facile method on fabricating aerogels with hierarchical porous structures was created by freeze-drying the cellulose nanofibril (CNF)/methyltrimethoxysilan (MTMS)/fumed silica (FS) suspension. FS was introduced for its porous structure, which could improve the thermal insulation performance of freeze-dried aerogels. The as-prepared aerogels were hydrophobic with improved mechanical properties (elastic recovery rate was up to 99.7%) and reduced thermal conductivity (0.027 Wm−1 K−1 at 25 °C). Most importantly, the addition of FS was proved to improve the thermal insulation stability of cellulose aerogels efficiently in different values of relative humidity (RH) and temperatures. The thermal conductivity of pure CNF aerogel conditioned at 25 °C and 95% RH was 196% higher than that of the fully-dried one, while the increase was 56% for the composite aerogel. Besides, at 30% RH, the thermal conductivity increased by 24% for the pure CNF aerogel when tested from 20 to 60 °C while only a 2% increase for the composite aerogel. Moreover, when tert-butanol was used as the solvent to optimize the distribution of the pores of freeze-dried aerogels, their thermal insulation performance was further improved. Our work provides easily available CNF/MTMS/FS ternary aerogels, which are stable in thermal conductivity in the changing environment.
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Aditya L et al (2017) A review on insulation materials for energy conservation in buildings. Renew Sust Energ Rev 73:1352–1365. https://doi.org/10.1016/j.rser.2017.02.034
Bendahou D, Bendahou A, Seantier B, Grohens Y, Kaddami H (2015) Nano-fibrillated cellulose-zeolites based new hybrid composites aerogels with super thermal insulating properties. Ind Crop Prod 65:374–382. https://doi.org/10.1016/j.indcrop.2014.11.012
Bledzki AK, Mamun AA, Volk J (2010) Physical, chemical and surface properties of wheat husk, rye husk and soft wood and their polypropylene composites. Compos A 41:480–488. https://doi.org/10.1016/j.compositesa.2009.12.004
Cervin NT, Aulin C, Larsson PT, Wågberg L (2012) Ultra porous nanocellulose aerogels as separation medium for mixtures of oil/water liquids. Cellulose 19:401–410. https://doi.org/10.1007/s10570-011-9629-5)
Chen W, Yu H, Li Q, Liu Y, Li J (2011) Ultralight and highly flexible aerogels with long cellulose I nanofibers. Soft Matter 7:10360. https://doi.org/10.1039/c1sm06179h
Cheng H et al (2017) Chemical crosslinking reinforced flexible cellulose nanofiber-supported cryogel. Cellulose 25:573–582. https://doi.org/10.1007/s10570-017-1548-7
El Rassy H, Pierre AC (2005) NMR and IR spectroscopy of silica aerogels with different hydrophobic characteristics. J NonCryst Solids 351:1603–1610. https://doi.org/10.1016/j.jnoncrysol.2005.03.048
Feng J, Le D, Nguyen ST, Tan Chin Nien V, Jewell D, Duong HM (2016) Silica colloids and surfaces a: physicochemical and engineering aspectscellulose hybrid aerogels for thermal and acoustic insulation applications. Colloids Surf A Physicochem Eng Asp 506:298–305. https://doi.org/10.1016/j.colsurfa.2016.06.052
Feng J, Liu M, Ma S, Yang J, Mo W, Su X (2020) Micro-nano scale heat transfer mechanisms for fumed silica based thermal insulating composite. Int Commun Heat Mass Transf 110:104392. https://doi.org/10.1016/j.icheatmasstransfer.2019.104392
Guo L, Chen Z, Lyu S, Fu F, Wang S (2018) Highly flexible cross-linked cellulose nanofibril sponge-like aerogels with improved mechanical property and enhanced flame retardancy. Carbohydr Polym 179:333–340. https://doi.org/10.1016/j.carbpol.2017.09.084
Han Y, Zhang X, Wu X, Lu C (2015) Flame retardant, heat insulating cellulose aerogels from waste cotton fabrics by in situ formation of magnesium hydroxide nanoparticles in cellulose gel nanostructures. ACS Sustainable Chem Eng 3:1853–1859. https://doi.org/10.1021/acssuschemeng.5b00438
Hayase G, Kanamori K, Abe K, Yano H, Maeno A, Kaji H, Nakanishi K (2014) Polymethylsilsesquioxane-cellulose nanofiber biocomposite aerogels with high thermal insulation, bendability, and superhydrophobicity. ACS Appl Mater Interfaces 6:9466–9471. https://doi.org/10.1021/am501822y
Hrubesh LW, Pekala RW (2011) Thermal properties of organic and inorganic aerogels. J Mater Res 9:731–738. https://doi.org/10.1557/jmr.1994.0731
Jiang F, Hsieh Y-L (2014) Amphiphilic superabsorbent cellulose nanofibril aerogels. J Mater Chem A 2:6337–6342. https://doi.org/10.1039/c4ta00743c
Jiang F, Hsieh Y-L (2016) Self-assembling of TEMPO oxidized cellulose nanofibrils as affected by protonation of surface carboxyls and drying methods. ACS Sustainable Chem Eng 4:1041–1049. https://doi.org/10.1021/acssuschemeng.5b01123
Jiang F, Kondo T, Hsieh Y-L (2016) Rice straw cellulose nanofibrils via aqueous counter collision and differential centrifugation and their self-assembled structures. ACS Sustainable Chem Eng 4:1697–1706. https://doi.org/10.1021/acssuschemeng.5b01653
Kaya M (2017) Super absorbent, light, and highly flame retardant cellulose-based aerogel crosslinked with citric acid. J Appl Polym Sci 134:45315. https://doi.org/10.1002/app.45315
Kim KH, Oh Y, Islam MF (2013) Mechanical and thermal management characteristics of ultrahigh surface area single-walled carbon nanotube aerogels. Adv Funct Mater 23:377–383. https://doi.org/10.1002/adfm.201201055
Kuhn J, Gleissner T, Arduinischuster M, Korder S, Fricke J (1995) Integration of mineral powders into SiO2 aerogels. J Non Cryst Solids 186:291–295
Laskowski J, Milow B, Ratke L (2015) The effect of embedding highly insulating granular aerogel in cellulosic aerogel. J Supercrit Fluids 106:93–99. https://doi.org/10.1016/j.supflu.2015.05.011
Lee O, Lee K, Yim T, Kim S, Yoo K (2002) Determination of mesopore size of aerogels from thermal conductivity measurements. J Non Cryst Solids 298:287–292
Li Y, Wang B, Sui X, Xu H, Zhang L, Zhong Y, Mao Z (2017) Facile synthesis of microfibrillated cellulose/organosilicon/polydopamine composite sponges with flame retardant properties. Cellulose 24:3815–3823. https://doi.org/10.1007/s10570-017-1373-z
Liu A, Medina L, Berglund LA (2017) High-strength nanocomposite aerogels of ternary composition: poly(vinyl alcohol), clay, and cellulose nanofibrils. ACS Appl Mater Interfaces 9:6453–6461. https://doi.org/10.1021/acsami.6b15561
Luo X, Shen J, Ma Y, Liu L, Meng R, Yao J (2020) Robust, sustainable cellulose composite aerogels with outstanding flame retardancy and thermal insulation. Carbohydr Polym 230:115623. https://doi.org/10.1016/j.carbpol.2019.115623
Miao X, Lin J, Tian F, Li X, Bian F, Wang J (2016) Cellulose nanofibrils extracted from the byproduct of cotton plant. Carbohydr Polym 136:841–850. https://doi.org/10.1016/j.carbpol.2015.09.056
Nguyen ST, Feng J, Ng SK, Wong JPW, Tan VBC, Duong HM (2014) Advanced thermal insulation and absorption properties of recycled cellulose aerogels. Colloids Surf A Physicochem Eng Asp 445:128–134. https://doi.org/10.1016/j.colsurfa.2014.01.015
Park SJ et al (2015) Soluble polycyclosilane–polysiloxane hybrid material and silicon thin film with optical properties at 193 nm and etch selectivity. J Mater Chem C 3:239–242. https://doi.org/10.1039/c4tc01917b
Rao AV, Bhagat SD, Hirashima H, Pajonk GM (2006) Synthesis of flexible silica aerogels using methyltrimethoxysilane (MTMS) precursor. J Colloid Interface Sci 300:279–285. https://doi.org/10.1016/j.jcis.2006.03.044
Rodriguez-Robledo MC et al (2018) Cellulose-silica nanocomposites of high reinforcing content with fungi decay resistance by one-pot synthesis. Materials. https://doi.org/10.3390/ma11040575
Roque-Malherbe RMA (2007) Adsorption and diffusion in nanoporous materials. CRC Press, Boca Raton
Sehaqui H, Zhou Q, Berglund LA (2011a) High-porosity aerogels of high specific surface area prepared from nanofibrillated cellulose (NFC). Compos Sci Technol 71:1593–1599. https://doi.org/10.1016/j.compscitech.2011.07.003
Sehaqui H, Zhou Q, Berglund LA (2011b) Nanostructured biocomposites of high toughness—a wood cellulose nanofiber network in ductile hydroxyethylcellulose matrix. Soft Matter 7:7342–7350. https://doi.org/10.1039/c1sm05325f
Shang K, Yang JC, Cao ZJ, Liao W, Wang YZ, Schiraldi DA (2017) Novel polymer aerogel toward high dimensional stability, mechanical property, and fire safety. ACS Appl Mater Interfaces 9:22985–22993. https://doi.org/10.1021/acsami.7b06096
Shi J, Lu L, Guo W, Zhang J, Cao Y (2013) Heat insulation performance, mechanics and hydrophobic modification of cellulose–SiO2 composite aerogels. Carbohydr Polym 98:282–289. https://doi.org/10.1016/j.carbpol.2013.05.082
Thai QB et al (2020) Cellulose-based aerogels from sugarcane bagasse for oil spill-cleaning and heat insulation applications. Carbohydr Polym 228:115365. https://doi.org/10.1016/j.carbpol.2019.115365
Thakur VK, Thakur MK (2014) Processing and characterization of natural cellulose fibers/thermoset polymer composites. Carbohydr Polym 109:102–117. https://doi.org/10.1016/j.carbpol.2014.03.039
Thakur M, Sharma A, Ahlawat V, Bhattacharya M, Goswami S (2020) Process optimization for the production of cellulose nanocrystals from rice straw derived α-cellulose. Mater Sci Energ Technol 3:328–334. https://doi.org/10.1016/j.mset.2019.12.005
Tian J, Shafi S, Tan H, Zhao Y (2020) Mechanical and thermal-insulating performance of silica aerogel enhanced jointly with glass fiber and fumed silica by a facile compressing technique. Chem Phys Lett 739:136950. https://doi.org/10.1016/j.cplett.2019.136950
Wang Q, Ni H, Pietzsch A, Hennies F, Bao Y, Chao Y (2011) Synthesis of water-dispersible photoluminescent silicon nanoparticles and their use in biological fluorescent imaging. J Nanopart Res 13:405–413. https://doi.org/10.1007/s11051-010-0047-7)
Wang H, Zhang X, Jiang Z, Li W, Yu Y (2015) A comparison study on the preparation of nanocellulose fibrils from fibers and parenchymal cells in bamboo (Phyllostachys pubescens). Ind Crop Prod 71:80–88. https://doi.org/10.1016/j.indcrop.2015.03.086
Wei G, Liu Y, Zhang X, Yu F, Du X (2011) Thermal conductivities study on silica aerogel and its composite insulation materials. Int J Heat Mass Transf 54:2355–2366. https://doi.org/10.1016/j.ijheatmasstransfer.2011.02.026
Wong JCH, Kaymak H, Tingaut P, Brunner S, Koebel MM (2015) Mechanical and thermal properties of nanofibrillated cellulose reinforced silica aerogel composites. Microporous Mesoporous Mater 217:150–158. https://doi.org/10.1016/j.micromeso.2015.06.025
Yang X, Han F, Xu C, Jiang S, Huang L, Liu L, Xia Z (2017) Effects of preparation methods on the morphology and properties of nanocellulose (NC) extracted from corn husk. Ind Crop Prod 109:241–247. https://doi.org/10.1016/j.indcrop.2017.08.032
Yu WD (2018) Textile material science. China Textile & Apparel Press, Beijing
Zanini M, Lavoratti A, Lazzari LK, Galiotto D, Pagnocelli M, Baldasso C, Zattera AJ (2016) Producing aerogels from silanized cellulose nanofiber suspension. Cellulose 24:769–779. https://doi.org/10.1007/s10570-016-1142-4
Zhang J, Cheng Y, Tebyetekerwa M, Meng S, Zhu M, Lu Y (2019) “Stiff–soft” binary synergistic aerogels with superflexibility and high thermal insulation performance. Adv Funct Mater 29:1806407. https://doi.org/10.1002/adfm.201806407
Zhao S, Zhang Z, Sèbe G, Wu R, Rivera Virtudazo RV, Tingaut P, Koebel MM (2015) Multiscale assembly of superinsulating silica aerogels within silylated nanocellulosic scaffolds: improved mechanical properties promoted by nanoscale chemical compatibilization. Adv Funct Mater 25:2326–2334. https://doi.org/10.1002/adfm.201404368
Zhao S, Emery O, Wohlhauser A, Koebel MM, Adlhart C, Malfait WJ (2018) Merging flexibility with superinsulation: machinable, nanofibrous pullulan-silica aerogel composites. Mater Des 160:294–302. https://doi.org/10.1016/j.matdes.2018.09.010
Zhou S, You T, Zhang X, Xu F (2018) Superhydrophobic cellulose nanofiber-assembled aerogels for highly efficient water-in-oil emulsions separation. ACS Appl Nano Mater 1:2095–2103. https://doi.org/10.1021/acsanm.8b00079
Acknowledgments
This work was supported by the National Key R&D Program of China (Project No. 2018YFC2000900), the Fundamental Research Funds for the Central Universities (Project No. 2232018A3-04) and Suzhou Science and Technology Project (Project No. ZXL2018134).
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Jiang, S., Zhang, M., Li, M. et al. Cellulose nanofibril (CNF) based aerogels prepared by a facile process and the investigation of thermal insulation performance. Cellulose 27, 6217–6233 (2020). https://doi.org/10.1007/s10570-020-03224-4
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DOI: https://doi.org/10.1007/s10570-020-03224-4