Technical Papers
Apr 3, 2023

Dispersion of Sonicated Sulfated Cellulose Nanocrystals and Their Effect on the Mechanical Properties of Cement Mortars

Publication: Journal of Materials in Civil Engineering
Volume 35, Issue 6

Abstract

Nanocellulose extracted from lignocellulosic biomass not only provides a promising way to deal with lignocellulosic biomass wastes but also contributes to the performance of cementitious materials. In this study, sulfated cellulose nanocrystals (CNCs) were selected as nanoreinforcement for cement mortars to improve their mechanical properties, especially the flexural strength. Three different sonication procedures were applied to CNC suspensions with CNC dosages of 0.01%, 0.05%, and 0.1% to improve their dispersion. The sonicated suspensions then were incorporated into the mortars. The effects of the sonication procedure and the CNC dosage on the particle dispersion of CNC suspension and the mechanical properties of mortars were examined in detail. The result showed that increasing the sonication energy from 7,835 to 37,587  J or lowering the CNC dosage from 0.1% to 0.01% could eliminate the aggregation of CNCs and increase the magnitude of the zeta potential of the CNC suspension, resulting in better dispersion (less aggregation in water). When continuous sonication for 12 min was used, the flexural strength of mortars with 0.01% CNC dosage improved the most, about 10%; however, an unexpectedly obvious decrease occurred when the CNC dosage was increased to 0.05% or 0.1%, which was due mainly to the reduced cement hydration degree and the more porous microstructure of the mortars. Thus, the optimum sonication energy needs to be adjusted for different dosages of CNC used; otherwise the CNC may have a negative effect on the performance of cement mortars. Given the same sonication procedure, the compressive strength of specimens did not change too much with the variation of CNC dosage; however, the flexural strength varied. For 3- and 28-day specimens, the flexural strength had maximum values for 0.05% and 0.01% CNC dosages, respectively. In addition, this study indicated that the improved dispersion of CNCs in water cannot ensure the significant strength improvement of mortars.

Get full access to this article

View all available purchase options and get full access to this article.

Data Availability Statement

Some or all data, models, or code that support the findings of this study are available from the corresponding author upon reasonable request.

Acknowledgments

The authors acknowledge the National Natural Science Foundation of China (Grant No. 52208295), the China Postdoctoral Science Foundation (Grant No. 2021M702954), and the Natural Science Foundation of Henan Province (Grant No. 222300420314). The authors acknowledge the support from School of Civil Engineering at Zhengzhou University and Civil and Environmental Engineering Department and Chemical Engineering Department at University of Louisville. This work was performed in part at the Conn Center for Renewable Energy Research at the University of Louisville.

References

Abd Hamid, S. B., S. K. Zain, R. Das, and G. Centi. 2016. “Synergic effect of tungstophosphoric acid and sonication for rapid synthesis of crystalline nanocellulose.” Carbohydr. Polym. 138 (Mar): 349–355. https://doi.org/10.1016/j.carbpol.2015.10.023.
Abitbol, T., A. Rivkin, Y. Cao, Y. Nevo, E. Abraham, T. Ben-Shalom, S. Lapidot, and O. Shoseyov. 2016. “Nanocellulose, a tiny fiber with huge applications.” Curr. Opin. Biotechnol. 39 (Jun): 76–88. https://doi.org/10.1016/j.copbio.2016.01.002.
Balea, A., E. Fuente, A. Blanco, and C. Negro. 2019. “Nanocelluloses: Natural-based materials for fiber-reinforced cement composites. A critical review.” Polymers 11 (3): 518. https://doi.org/10.3390/polym11030518.
Barnat-Hunek, D., M. Szymańska-Chargot, M. Jarosz-Hadam, and G. Łagód. 2019. “Effect of cellulose nanofibrils and nanocrystals on physical properties of concrete.” Constr. Build. Mater. 223: 1–23. https://doi.og/10.1016/j.conbuildmat.2019.06.145.
Benini, K. C. C. C., H. J. C. Voorwald, M. O. H. Cioffi, M. C. Rezende, and V. Arantes. 2018. “Preparation of nanocellulose from Imperata brasiliensis grass using Taguchi method.” Carbohydr. Polym. 192 (Jul): 337–346. https://doi.org/10.1016/j.carbpol.2018.03.055.
Björnström, J., and S. Chandra. 2003. “Effect of superplasticizers on the rheological properties of cements.” Mater. Struct. 36 (10): 685–692. https://doi.org/10.1007/BF02479503.
Cao, Y., J. Weiss, J. Youngblood, R. Moon, and P. Zavattieri. 2013. “Performance-enhanced cementitious materials by cellulose nanocrystal additions.” In Production and applications of cellulose nanomaterials, 2. Peachtree Corners, GA: TAPPI Press.
Cao, Y., P. Zavaterri, J. Youngblood, R. Moon, and J. Weiss. 2015. “The influence of cellulose nanocrystal additions on the performance of cement paste.” Cem. Concr. Compos. 56 (Feb): 73–83. https://doi.org/10.1016/j.cemconcomp.2014.11.008.
Cao, Y., P. Zavattieri, J. Youngblood, R. Moon, and J. Weiss. 2016. “The relationship between cellulose nanocrystal dispersion and strength.” Constr. Build. Mater. 119 (Aug): 71–79. https://doi.org/10.1016/j.conbuildmat.2016.03.077.
Chi, K., and J. M. Catchmark. 2017. “Enhanced dispersion and interface compatibilization of crystalline nanocellulose in polylactide by surfactant adsorption.” Cellulose 24 (11): 4845–4860. https://doi.org/10.1007/s10570-017-1479-3.
Chu, Y., Y. Sun, W. Wu, and H. Xiao. 2020. “Dispersion properties of nanocellulose: A review.” Carbohydr. Polym. 250 (Dec): 116892. https://doi.org/10.1016/j.carbpol.2020.116892.
Claramunt, J., H. Ventura, R. D. Toledo Filho, and M. Ardanuy. 2019. “Effect of nanocelluloses on the microstructure and mechanical performance of CAC cementitious matrices.” Cem. Concr. Res. 119 (May): 64–76. https://doi.org/10.1016/j.cemconres.2019.02.006.
Csiszar, E., P. Kalic, A. Kobol, and E. de Paulo Ferreira. 2016. “The effect of low frequency ultrasound on the production and properties of nanocrystalline cellulose suspensions and films.” Ultrason. Sonochem. 31 (Jul): 473–480. https://doi.org/10.1016/j.ultsonch.2016.01.028.
Ding, S., J. Ou, J. Wang, and B. Han. 2019. Nano-engineered cementitious composites: Principles and practices. Singapore: Springer.
Dousti, M. R., Y. Boluk, and V. Bindiganavile. 2019. “The effect of cellulose nanocrystal (CNC) particles on the porosity and strength development in oil well cement paste.” Constr. Build. Mater. 205: 456–462. https://doi.org/10.1016/j.conbuildmat.2019.01.073.
EN (British Standard). 2011. 197-1. Cement–Part 1: Composition, specifications and conformity criteria for common cements. London, UK: European Committee For Standardisation.
Feng, X., E. J. Garboczi, D. P. Bentz, P. E. Stutzman, and T. O. Mason. 2004. “Estimation of the degree of hydration of blended cement pastes by a scanning electron microscope point-counting procedure.” Cem. Concr. Res. 34 (10): 1787–1793. https://doi.org/10.1016/j.cemconres.2004.01.014.
Flores, J., M. Kamali, and A. Ghahremaninezhad. 2017. “An investigation into the properties and microstructure of cement mixtures modified with cellulose nanocrystal.” Materials 10 (5): 498. https://doi.org/10.3390/ma10050498.
Fu, T., R. J. Moon, P. Zavattieri, J. Youngblood, and W. J. Weiss. 2017. “Cellulose nanomaterials as additives for cementitious materials.” In Cellulose-reinforced nanofibre composites, 455–482. Amsterdam, Netherlands: Elsevier.
Ghahari, S., L. N. Assi, A. Alsalman, and K. E. Alyamaç. 2020. “Fracture properties evaluation of cellulose nanocrystals cement paste.” Materials 13 (11): 2507. https://doi.org/10.3390/ma13112507.
Guo, A., Z. Sun, C. Qi, and N. Sathitsuksanoh. 2020a. “Hydration of portland cement pastes containing untreated and treated hemp powders.” J. Mater. Civ. Eng. 32 (6): 04020148. https://doi.org/10.1061/(ASCE)MT.1943-5533.0003209.
Guo, A., Z. Sun, N. Sathitsuksanoh, and H. Feng. 2020b. “A review on the application of nanocellulose in cementitious materials.” Nanomaterials 10 (12): 2476. https://doi.org/10.3390/nano10122476.
Guo, A., Z. Sun, and J. Satyavolu. 2019. “Impact of chemical treatment on the physiochemical and mechanical properties of kenaf fibers.” Ind. Crops Prod. 141 (Dec): 111726. https://doi.org/10.1016/j.indcrop.2019.111726.
Haddad Kolour, H., W. Ashraf, and E. N. Landis. 2021. “Hydration and early age properties of cement pastes modified with cellulose nanofibrils.” Transp. Res. Rec. 2675 (9): 38–46. https://doi.org/10.1177/0361198120945993.
Han, B., S. Ding, J. Wang, and J. Ou. 2019. Nano-engineered cementitious composites: Principles and practices. Singapore: Springer.
Han, B., L. Zhang, S. Zeng, S. Dong, X. Yu, R. Yang, and J. Ou. 2017. “Nano-core effect in nano-engineered cementitious composites.” Composites, Part A 95 (Apr): 100–109. https://doi.org/10.1016/j.compositesa.2017.01.008.
Hasani, M., E. D. Cranston, G. Westman, and D. G. Gray. 2008. “Cationic surface functionalization of cellulose nanocrystals.” Soft Matter 4 (11): 2238–2244. https://doi.org/10.1039/B806789A.
Hisseine, O. A., N. Basic, A. F. Omran, and A. Tagnit-Hamou. 2018. “Feasibility of using cellulose filaments as a viscosity modifying agent in self-consolidating concrete.” Cem. Concr. Compos. 94 (Nov): 327–340. https://doi.org/10.1016/j.cemconcomp.2018.09.009.
Hisseine, O. A., and A. Tagnit-Hamou. 2020. “Nanocellulose for ecological nanoengineered strain-hardening cementitious composites incorporating high-volume ground-glass pozzolans.” Cem. Concr. Compos. 112 (Sep): 103662. https://doi.org/10.1016/j.cemconcomp.2020.103662.
ISO. 2017. Particle size analysis - Dynamic light scattering (DLS). ISO 22412:2017. Geneva: ISO.
Izzat, A. M., A. M. M. Al Bakri, H. Kamarudin, A. V. Sandu, G. C. M. Ruzaidi, M. T. M. Faheem, and L. M. Moga. 2013. “Sulfuric acid attack on ordinary Portland cement and geopolymer material.” Rev. Chim. 64 (9): 1011–1014.
Jakubek, Z. J., M. Chen, M. Couillard, T. Leng, L. Liu, S. Zou, U. Baxa, J. D. Clogston, W. Y. Hamad, and L. J. Johnston. 2018. “Characterization challenges for a cellulose nanocrystal reference material: Dispersion and particle size distributions.” J. Nanopart. Res. 20 (4): 1–16. https://doi.org/10.1007/s11051-018-4194-6.
Jordan, J. H., M. W. Easson, and B. D. Condon. 2019. “Alkali hydrolysis of sulfated cellulose nanocrystals: Optimization of reaction conditions and tailored surface charge.” Nanomaterials 9 (9): 1232. https://doi.org/10.3390/nano9091232.
Kaszuba, M., D. McKnight, M. T. Connah, F. K. McNeil-Watson, and U. Nobbmann. 2008. “Measuring sub nanometre sizes using dynamic light scattering.” J. Nanopart. Res. 10 (5): 823–829. https://doi.org/10.1007/s11051-007-9317-4.
Lee, H.-J., S.-K. Kim, H.-S. Lee, and W. Kim. 2019a. “A study on the drying shrinkage and mechanical properties of fiber reinforced cement composites using cellulose nanocrystals.” Int. J. Concr. Struct. Mater. 13 (1): 1–11. https://doi.org/10.1186/s40069-019-0351-2.
Lee, H.-J., and W. Kim. 2020. “Long-term durability evaluation of fiber-reinforced ECC using wood-based cellulose nanocrystals.” Constr. Build. Mater. 238 (Mar): 117754. https://doi.org/10.1016/j.conbuildmat.2019.117754.
Lee, H.-J., H.-S. Lee, J. Seo, Y.-H. Kang, W. Kim, and T. H.-K. Kang. 2019b. “State-of-the-art of cellulose nanocrystals and optimal method for their dispersion for construction-related applications.” Appl. Sci. 9 (3): 426. https://doi.org/10.3390/app9030426.
Lin, N., and A. Dufresne. 2014. “Surface chemistry, morphological analysis and properties of cellulose nanocrystals with gradiented sulfation degrees.” Nanoscale 6 (10): 5384–5393. https://doi.org/10.1039/C3NR06761K.
Lokanathan, A. R., K. M. A. Uddin, O. J. Rojas, and J. Laine. 2014. “Cellulose nanocrystal-mediated synthesis of silver nanoparticles: Role of sulfate groups in nucleation phenomena.” Biomacromolecules 15 (1): 373–379. https://doi.org/10.1021/bm401613h.
Malvern. 2013. Zetasizer nano series user manual. Worcestershire, UK: Malvern Instruments.
Mazlan, D., M. Din, C. Tokoro, and I. Ibrahim. 2016. “Cellulose nanocrystals addition effects on cement mortar matrix properties.” Int. J. Adv. Mech. Civ. Eng. 3 (1): 44–48.
Mazlan, D., S. Krishnan, M. F. M. Din, C. Tokoro, N. H. A. Khalid, I. S. Ibrahim, H. Takahashi, and D. Komori. 2020. “Effect of cellulose nanocrystals extracted from oil palm empty fruit bunch as green admixture for mortar.” Sci. Rep. 10 (1): 1–11. https://doi.org/10.1038/s41598-020-63575-7.
Moon, R., S. Beck, and A. Rudie. 2013. “Cellulose nanocrystals—A material with unique properties and many potential applications.” In Production and applications of cellulose nanomaterials, 9. Peachtree Corners, GA : TAPPI Press.
Mwaikambo, L. Y., and M. P. Ansell. 2002. “Chemical modification of hemp, sisal, jute, and kapok fibers by alkalization.” J. Appl. Polym. Sci. 84 (12): 2222–2234. https://doi.org/10.1002/app.10460.
Neubauer, C. M., M. Yang, and H. M. Jennings. 1998. “Interparticle potential and sedimentation behavior of cement suspensions: Effects of admixtures.” Adv. Cem. Based Mater. 8 (1): 17–27. https://doi.org/10.1016/S1065-7355(98)00005-4.
Pane, I., and W. Hansen. 2005. “Investigation of blended cement hydration by isothermal calorimetry and thermal analysis.” Cem. Concr. Res. 35 (6): 1155–1164. https://doi.org/10.1016/j.cemconres.2004.10.027.
Pei, A., Q. Zhou, and L. A. Berglund. 2010. “Functionalized cellulose nanocrystals as biobased nucleation agents in poly (l-lactide)(PLLA)–Crystallization and mechanical property effects.” Compos. Sci. Technol. 70 (5): 815–821. https://doi.org/10.1016/j.compscitech.2010.01.018.
Ramezani, M., Y. H. Kim, and Z. Sun. 2019. “Modeling the mechanical properties of cementitious materials containing CNTs.” Cem. Concr. Compos. 104 (Nov): 103347. https://doi.org/10.1016/j.cemconcomp.2019.103347.
Shang, H., and Z. Sun. 2019. “PAHs (naphthalene) removal from stormwater runoff by organoclay amended pervious concrete.” Constr. Build. Mater. 200 (Mar): 170–180. https://doi.org/10.1016/j.conbuildmat.2018.12.096.
Shojaeiarani, J., D. Bajwa, and G. Holt. 2020. “Sonication amplitude and processing time influence the cellulose nanocrystals morphology and dispersion.” Nanocomposites 6 (1): 41–46. https://doi.org/10.1080/20550324.2019.1710974.
Termkhajornkit, P., and T. Nawa. 2004. “The fluidity of fly ash–cement paste containing naphthalene sulfonate superplasticizer.” Cem. Concr. Res. 34 (6): 1017–1024. https://doi.org/10.1016/j.cemconres.2003.11.017.
Thomas, B., M. C. Raj, K. B. Athira, M. H. Rubiyah, J. Joy, A. Moores, G. L. Drisko, and C. Sanchez. 2018. “Nanocellulose, a versatile green platform: From biosources to materials and their applications.” Chem. Rev. 118 (24): 11575–11625. https://doi.org/10.1021/acs.chemrev.7b00627.
Trache, D., A. F. Tarchoun, M. Derradji, T. S. Hamidon, N. Masruchin, N. Brosse, and M. H. Hussin. 2020. “Nanocellulose: From fundamentals to advanced applications.” Front. Chem. 8 (May): 392. https://doi.org/10.3389/fchem.2020.00392.
Vanin, D. V. F., V. D. Andrade, T. A. Fiorentin, D. O. S. Recouvreux, C. A. Carminatti, and H. A. Al-Qureshi. 2020. “Cement pastes modified by cellulose nanocrystals: A dynamic moduli evolution assessment by the Impulse Excitation Technique.” Mater. Chem. Phys. 239 (Jan): 122038. https://doi.org/10.1016/j.matchemphys.2019.122038.
Wang, X., S. Dong, A. Ashour, W. Zhang, and B. Han. 2020. “Effect and mechanisms of nanomaterials on interface between aggregates and cement mortars.” Constr. Build. Mater. 240 (Apr): 117942. https://doi.org/10.1016/j.conbuildmat.2019.117942.
Wei, L., U. P. Agarwal, K. C. Hirth, L. M. Matuana, R. C. Sabo, and N. M. Stark. 2017. “Chemical modification of nanocellulose with canola oil fatty acid methyl ester.” Carbohydr. Polym. 169 (Aug): 108–116. https://doi.org/10.1016/j.carbpol.2017.04.008.
Xu, X., F. Liu, L. Jiang, J. Zhu, D. Haagenson, and D. P. Wiesenborn. 2013. “Cellulose nanocrystals vs. cellulose nanofibrils: A comparative study on their microstructures and effects as polymer reinforcing agents.” ACS Appl. Mater. Interfaces 5 (8): 2999–3009. https://doi.org/10.1021/am302624t.

Information & Authors

Information

Published In

Go to Journal of Materials in Civil Engineering
Journal of Materials in Civil Engineering
Volume 35Issue 6June 2023

History

Received: Jun 27, 2022
Accepted: Sep 30, 2022
Published online: Apr 3, 2023
Published in print: Jun 1, 2023
Discussion open until: Sep 3, 2023

Permissions

Request permissions for this article.

Authors

Affiliations

Associate Research Professor, School of Civil Engineering, Zhengzhou Univ., Henan 450001, China (corresponding author). ORCID: https://orcid.org/0000-0002-0425-9998. Email: [email protected]
Winnia Professor and Chair, Dept. of Civil and Environmental Engineering, Univ. of Louisville, Louisville, KY 40292. ORCID: https://orcid.org/0000-0002-5905-1414. Email: [email protected]
Noppadon Sathitsuksanoh [email protected]
Assistant Professor, Dept. of Chemical Engineering, Univ. of Louisville, Louisville, KY 40292. Email: [email protected]
Hong Shang, M.ASCE [email protected]
Senior Staff Engineer, Terracon Consultants Inc., 13050 Eastgage Park Way Ste 101, Louisville, KY 40223-3915. Email: [email protected]

Metrics & Citations

Metrics

Citations

Download citation

If you have the appropriate software installed, you can download article citation data to the citation manager of your choice. Simply select your manager software from the list below and click Download.

View Options

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Get Access

Access content

Please select your options to get access

Log in/Register Log in via your institution (Shibboleth)
ASCE Members: Please log in to see member pricing

Purchase

Save for later Information on ASCE Library Cards
ASCE Library Cards let you download journal articles, proceedings papers, and available book chapters across the entire ASCE Library platform. ASCE Library Cards remain active for 24 months or until all downloads are used. Note: This content will be debited as one download at time of checkout.

Terms of Use: ASCE Library Cards are for individual, personal use only. Reselling, republishing, or forwarding the materials to libraries or reading rooms is prohibited.
ASCE Library Card (5 downloads)
$105.00
Add to cart
ASCE Library Card (20 downloads)
$280.00
Add to cart
Buy Single Article
$35.00
Add to cart

Media

Figures

Other

Tables

Share

Share

Copy the content Link

Share with email

Email a colleague

Share