Abstract
Nanocellulose aerogel is the third generation aerogel, and its highly interconnected porous network structure makes it an extraordinary thermal insulation material. However, there are abundant hydroxyl groups on the surface of cellulose nanofibrils, which causes the nanocellulose aeogels to absorb moisture in the air and the environment easily, thereby destroying their porous network structure and damaging their original thermal insulation performance. Herein, cellulose nanofibril (CNF) aerogels were prepared by freeze-drying and then modified by a facile two-step impregnation process. Firstly, the pure CNF aerogels were impregnated in the hydrolyzed sol with methyltriethoxysilane (MTES) as the silicon source; and then the silanol polycondensed in an alkaline environment to form polysiloxane particles. The silanization modification made the CNF aerogels superhydrophobic (water contact angle up to 155.2°) while retaining their original excellent thermal insulation performance (thermal conductivity of 0.03249 Wm−1 K−1) after being exposed to water, and the thermal conductivity increased (0.03249–0.04561 Wm−1 K−1) with the increase of cellulose nanofibril concentration (2.5–4.5 wt%). Compared with previous similar studies, the method is simpler and has the advantages of low cost and low risk.
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References
Abdul Khalil HPS, Bhat AH, Ireana Yusra AF (2012) Green composites from sustainable cellulose nanofibrils: a review. Carbohyd Polym 87:963–979. https://doi.org/10.1016/j.carbpol.2011.08.078
Abitbol T et al (2016) Nanocellulose, a tiny fiber with huge applications. Curr Opin Biotechnol 39:76–88. https://doi.org/10.1016/j.copbio.2016.01.002
Ahankari S, Paliwal P, Subhedar A, Kargarzadeh H (2021) Recent developments in nanocellulose-based aerogels in thermal applications: a review. ACS Nano 15:3849–3874. https://doi.org/10.1021/acsnano.0c09678
Cai J, Liu S, Feng J, Kimura S, Wada M, Kuga S, Zhang L (2012) Cellulose-silica nanocomposite aerogels by in situ formation of silica in cellulose gel. Angew Chem Int Edit 51:2076–2079. https://doi.org/10.1002/anie.201105730
Chang C, Zhang L (2011) Cellulose-based hydrogels: present status and application prospects. Carbohyd Polym 84:40–53. https://doi.org/10.1016/j.carbpol.2010.12.023
Chen F et al (2016) A simple one-step approach to fabrication of highly hydrophobic silk fabrics. Appl Surf Sci 360:207–212. https://doi.org/10.1016/j.apsusc.2015.10.186
Chhajed M, Yadav C, Agrawal AK, Maji PK (2019) Esterified superhydrophobic nanofibrillated cellulose based aerogel for oil spill treatment. Carbohydr Polym 226:115286. https://doi.org/10.1016/j.carbpol.2019.115286
Citak E, Istanbullu B, Sakalak H, Gursoy M, Karaman M (2019) All-dry hydrophobic functionalization of paper surfaces for efficient transfer of CVD graphene. Macromol Chem Phys. https://doi.org/10.1002/macp.201900277
Cui Y, Gong H, Wang Y, Li D, Bai H (2018) A thermally insulating textile inspired by polar bear hair. Adv Mater 30:e1706807. https://doi.org/10.1002/adma.201706807
Deka MJ, Chowdhury D (2017) CVD assisted hydrophobic graphene quantum dots: fluorescence sensor for aromatic amino acids. ChemistrySelect 2:1999–2005. https://doi.org/10.1002/slct.201601737
Do NHN et al (2020a) Heat and sound insulation applications of pineapple aerogels from pineapple waste. Mater Chem Phys. https://doi.org/10.1016/j.matchemphys.2019.122267
Do NHN et al (2020b) Recycling of pineapple leaf and cotton waste fibers into heat-insulating and flexible cellulose aerogel composites. J Polym Environ. https://doi.org/10.1007/s10924-020-01955-w
Fu J, He C, Huang J, Chen Z, Wang S (2016a) Cellulose nanofibril reinforced silica aerogels: optimization of the preparation process evaluated by a response surface methodology. Rsc Adv 6:100326–100333. https://doi.org/10.1039/c6ra20986f
Fu J, Wang S, He C, Lu Z, Huang J, Chen Z (2016b) Facilitated fabrication of high strength silica aerogels using cellulose nanofibrils as scaffold. Carbohyd Polym 147:89–96. https://doi.org/10.1016/j.carbpol.2016.03.048
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
Guzel Kaya G, Deveci H (2020) Synergistic effects of silica aerogels/xerogels on properties of polymer composites: a review. J Ind Eng Chem 89:13–27. https://doi.org/10.1016/j.jiec.2020.05.019
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
Husing N, Schubert U (1998) Aerogels-airy materials: chemistry, structure, and properties. Angew Chem Int Ed Engl 37:22–45
Islam MT, Alam MM, Patrucco A, Montarsolo A, Zoccola M (2014) Preparation of Nanocellulose: A Review. Aatcc J Res https://doi.org/10.14504/ajr.1.5.3
Jaya NA, Yun-Ming L, Cheng-Yong H, Abdullah MMAB, Hussin K (2020) Correlation between pore structure, compressive strength and thermal conductivity of porous metakaolin geopolymer. Constr Build Mater. https://doi.org/10.1016/j.conbuildmat.2020.118641
Korhonen JT, Kettunen M, Ras RHA, Ikkala O (2011) Hydrophobic nanocellulose aerogels as floating, sustainable, reusable, and recyclable oil absorbents. Acs Appl Mater Inter 3:1813–1816. https://doi.org/10.1021/am200475b
Lavoine N, Bergstrom L (2017) Nanocellulose-based foams and aerogels: processing, properties, and applications. J Mater Chem A 5:16105–16117. https://doi.org/10.1039/c7ta02807e
Li X-M, Reinhoudt D, Crego-Calama M (2007) What do we need for a superhydrophobic surface? a review on the recent progress in the preparation of superhydrophobic surfaces. Chem Soc Rev 36:1529–1529. https://doi.org/10.1039/b602486f
Linhares T, de Amorim MTP, Duraes L (2019) Silica aerogel composites with embedded fibres: a review on their preparation, properties and applications. J Mater Chem A 7:22768–22802. https://doi.org/10.1039/c9ta04811a
Noroozi M et al (2019) Nanostructure of aerogels and their applications in thermal energy insulation. Acs Appl Energ Mater 2:5319–5349. https://doi.org/10.1021/acsaem.9b01157
Pierre AC, Pajonk GM (2002) Chemistry of aerogels and their applications. Chem Rev 102:4243–4265. https://doi.org/10.1021/cr0101306
Qi J et al (2019) Lightweight, flexible, thermally-stable, and thermally-insulating aerogels derived from cotton nanofibrillated cellulose. ACS Sustain Chem Eng 7:9202–9210. https://doi.org/10.1021/acssuschemeng.8b06851
Qu ZG, Fu YD, Liu Y, Zhou L (2018) Approach for predicting effective thermal conductivity of aerogel materials through a modified lattice Boltzmann method. Appl Therm Eng 132:730–739. https://doi.org/10.1016/j.applthermaleng.2018.01.013
Rafieian F, Hosseini M, Jonoobi M, Yu Q (2018) Development of hydrophobic nanocellulose-based aerogel via chemical vapor deposition for oil separation for water treatment. Cellulose 25:4695–4710. https://doi.org/10.1007/s10570-018-1867-3
Rechberger F, Niederberger M (2017) Synthesis of aerogels: from molecular routes to 3-dimensional nanoparticle assembly. Nanoscale Horiz 2:6–30. https://doi.org/10.1039/c6nh00077k
Si Y, Guo Z (2015) Superhydrophobic nanocoatings: from materials to fabrications and to applications. Nanoscale 7:5922–5946. https://doi.org/10.1039/c4nr07554d
Slosarczyk A (2017) Recent advances in research on the synthetic fiber based silica aerogel nanocomposites. Nanomaterials. https://doi.org/10.3390/nano7020044
Su L et al (2020) Anisotropic and hierarchical SiC@SiO2 nanowire aerogel with exceptional stiffness and stability for thermal superinsulation. Sci Adv. https://doi.org/10.1126/sciadv.aay6689
Sun D, Liu W, Zhou F, Tang A, Xie W (2020) Optimizing material and manufacturing process for PEGDA/CNF aerogel scaffold. J Porous Mater 27:1623–1637. https://doi.org/10.1007/s10934-020-00938-5
Sun Y, Chu Y, Wu W, Xiao H (2021) Nanocellulose-based lightweight porous materials: A review. Carbohydr Polym 255:117489. https://doi.org/10.1016/j.carbpol.2020.117489
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
Venkataraman M, Mishra R, Kotresh TM, Militky J, Jamshaid H (2016) Aerogels for thermal insulation in high-performance textiles. Text Prog 48:55–118. https://doi.org/10.1080/00405167.2016.1179477
Wang X, Lu L-L, Yu Z-L, Xu X-W, Zheng Y-R, Yu S-H (2015) Scalable template synthesis of resorcinol-formaldehyde/graphene oxide composite aerogels with tunable densities and mechanical properties. Angew Chem Int Edit 54:2397–2401. https://doi.org/10.1002/anie.201410668
Wang J, Liu X, Jin T, He H, Liu L (2019) Preparation of nanocellulose and its potential in reinforced composites: A review. J Biomater Sci Polym Ed 30:919–946. https://doi.org/10.1080/09205063.2019.1612726
Yadav C, Saini A, Zhang W, You X, Chauhan I, Mohanty P, Li X (2021) Plant-based nanocellulose: A review of routine and recent preparation methods with current progress in its applications as rheology modifier and 3D bioprinting. Int J Biol Macromol 166:1586–1616. https://doi.org/10.1016/j.ijbiomac.2020.11.038
Yamasaki S et al (2019) Nanocellulose xerogels with high porosities and large specific surface areas. Front Chem 7:316. https://doi.org/10.3389/fchem.2019.00316
Yang Y, Deng Y, Tong Z, Wang C (2014) Renewable lignin-based xerogels with self-cleaning properties and superhydrophobicity. ACS Sustain Chem Eng 2:1729–1733. https://doi.org/10.1021/sc500250b
Zhang ZH et al. (2008) Mechanical reinforcement of silica aerogel insulation with ceramic fibers. 2008 2nd Ieee International Nanoelectronics Conference, Vols 1–3:371-+. https://doi.org/10.1109/Inec.2008.4585507
Zhang ZH et al (2012) Mechanical property of silica aerogel fibers composite insulation. Rare Metal Mat Eng 41:415–418
Zhang S et al (2020) Thermal conductivities of cellulose diacetate based aerogels. Cellulose 27:4555–4564. https://doi.org/10.1007/s10570-020-03084-y
Zhou S, Apostolopoulou-Kalkavoura V, Tavares da Costa MV, Bergström L, Strømme M, Xu C (2019) Elastic aerogels of cellulose nanofibers@metal–organic frameworks for thermal insulation and fire retardancy. Nanomicro Lett. https://doi.org/10.1007/s40820-019-0343-4
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This work was financially supported by Zhejiang Sci-Tech University (No. LW-YP2020034).
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Chen, C., Li, C., Yu, D. et al. A facile method to prepare superhydrophobic nanocellulose-based aerogel with high thermal insulation performance via a two-step impregnation process. Cellulose 29, 245–257 (2022). https://doi.org/10.1007/s10570-021-04275-x
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DOI: https://doi.org/10.1007/s10570-021-04275-x