Title:
Hindered Calcium Hydroxide Nucleation and Growth as Mechanism Responsible for Tricalcium Silicate Retardation in Presence of Sucrose
Author(s):
Patrick Juilland and Emmanuel Gallucci
Publication:
Symposium Paper
Volume:
329
Issue:
Appears on pages(s):
143-154
Keywords:
retardation; sucrose; hydration; nucleation and growth; dissolution; calcium hydroxide; C-S-H; tricalcium silicate
DOI:
10.14359/51711210
Date:
9/24/2018
Abstract:
Among retarding molecules, sucrose is known since decades as probably one of the most powerful retarder of Portland cement hydration. Despite numerous studies, the underlying mechanism for this retardation remains highly speculative since unequivocal experiments are still lacking. Which process or which phase is affected and what is the nature of the interaction between sucrose and cement phases remain some of the unanswered questions. The present study lets aside the influence of sucrose on the aluminate phases and focuses on tricalcium silicate since it dominates the kinetics of hydration at early age.
The impact of sucrose on the independent basic hydration mechanisms was evaluated on the dissolution of alite (impure tricalcium silicate) by means of topological experiments and on the nucleation of its hydrates, i.e. C-S-H and calcium hydroxide, using potentiometric experiments at different pH.
Pure dissolution seems poorly affected by sucrose, if not at all, indicating that there is potentially no interaction between alite and sucrose.
The nucleation and growth of C-S-H, studied through precipitation experiments in diluted suspension showed to be affected to a very limited extent and only at high pH.
On the other hand, both the nucleation and growth of CH revealed to be extremely sensitive by the presence of sucrose, even at relatively low dosages, and at all studied pH.
Adsorption experiments on the various phases supported those observations. Thermogravimetric analysis of hydrated alite pastes further confirmed that sucrose effectively prevents the growth of calcium hydroxide and that the onset for the acceleration is subjected to this condition.
In light of those results a novel mechanism of retardation is proposed for sucrose and its implications regarding early age hydration processes are discussed.
Related References:
1. Juenger, M. C. G., and Jenningsa, H. M., “New Insights into the Effects of Sugar on the Hydration and Microstructure of Cement Pastes,” Cement and Concrete Research, V. 32, No. 3, 2002, pp. 393-399. doi: 10.1016/S0008-8846(01)00689-5
2. Cheung, J.; Jeknavorian, A.; Roberts, L.; and Silva, D., “Impact of Admixtures on the Hydration Kinetics of Portland Cement,” Cement and Concrete Research, V. 41, No. 12, 2011, pp. 1289-1309. doi: 10.1016/j.cemconres.2011.03.005
3. Marchon, D.; Juilland, P.; Gallucci, E.; Frunz, L.; and Flatt, R. J., “Molecular and Submolecular Scale Effects of Comb-Copolymers on Tri-calcium Silicate Reactivity: Toward Molecular Design,” Journal of the American Ceramic Society, V. 100, No. 3, 2017, pp. 817-841. doi: 10.1111/jace.14695
4. Pourchet, S.; Comparet, C.; Nicoleau, L.; and Nonat, A., “Influence of PC Superplasticizers on Tricalcium Silicate Hydration,” 12th International Congress on the Chemistry of Cement – ICCC 2007,” Montreal, QC, Canada, 2007, 14 pp.
5. Nicoleau, L., “Interactions physico-chimiques entre des latex et les phases principales du ciment,” thesis, University of Burgundy, Dijon, France, 2004.
6. Nachbaur, L.; Nkinamubanzi, P.-C.; Nonat, A.; and Mutin, J.-C., “Electrokinetic Properties which Control the Coagulation of Silicate Cement Suspensions during Early Age Hydration,” Journal of Colloid and Interface Science, V. 202, No. 2, 1998, pp. 261-268. doi: 10.1006/jcis.1998.5445
7. Jönsson, B.; Nonat, A.; Labbez, C.; Cabane, B.; and Wennerström, H., “Controlling the Cohesion of Cement Paste,” Langmuir, V. 21, No. 20, 2005, pp. 9211-9221. doi: 10.1021/la051048z
8. Bullard, J. W., and Flatt, R. J., “New Insights Into the Effect of Calcium Hydroxide Precipitation on the Kinetics of Tricalcium Silicate Hydration,” Journal of the American Ceramic Society, V. 93, No. 7, 2010, pp. 1894-1903.
9. Juilland, P.; Gallucci, E.; Flatt, R.; and Scrivener, K., “Dissolution Theory Applied to the Induction Period in Alite Hydration,” Cement and Concrete Research, V. 40, No. 6, 2010, pp. 831-844. doi: 10.1016/j.cemconres.2010.01.012
10. Young, J. F.; Tong, H. S.; and Berger, R. L., “Composition of Solutions in Contact with Hydrating Tricalcium Silicate Pastes,” Journal of the American Ceramic Society, V. 60, No. 5-6, 1977, pp. 193-198. doi: 10.1111/j.1151-2916.1977.tb14104.x
11. Costoya, M., “Effect of particle size on the hydration kinetics and microstructural development of tricalcium silicate,” PhD thesis, École polytechnique fédérale de Lausanne, Lausanne, Switzerland, 2008.
12. Juilland, P., and Gallucci, E., “Morpho-topological Investigation of the Mechanisms and Kinetic Regimes of Alite Dissolution,” Cement and Concrete Research, V. 76, 2015, pp. 180-191. doi: 10.1016/j.cemconres.2015.06.001
13. Kulik, D. et al., “GEM – Selektor Geochemical Modeling Package: Revised Algorithm and GEMS3K Numerical Kernel for Coupled Simulation Codes,” Computers & Geosciences, V. 17, 2013, pp. 1-24.
14. Popov, K. I.; Sultanova, N.; Rönkkömäki, H.; Hannu-Kuure, M.; Jalonen, J.; Lajunen, L. H. J.; Bugaenko, I. F.; and Tuzhilkin, V. I., “13C NMR and Electrospray Ionization Mass Spectrometric Study of Sucrose Aqueous Solutions at High pH: NMR Measurement of Sucrose Dissociation Constant,” Food Chemistry, V. 96, No. 2, 2006, pp. 248-253. doi: 10.1016/j.foodchem.2005.02.025
15. Nicoleau, L., and Nonat, A., “A New View on the Kinetics of Tricalcium Silicate Hydration,” Cement and Concrete Research, V. 86, 2016, pp. 1-11. doi: 10.1016/j.cemconres.2016.04.009
16. Galmarini, S.; Aimable, A.; Ruffray, N.; and Bowen, P., “Changes in Portlandite Morphology with Solvent Composition: Atomistic Simulations and Experiment,” Cement and Concrete Research, V. 41, No. 12, 2011, pp. 1330-1338. doi: 10.1016/j.cemconres.2011.04.009
17. Gránásy, L.; Pusztai, T.; Tegze, G.; Warren, J. A.; and Douglas, J. F., “Growth and Form of Spherulites,” Physical Review. E, V. 72, No. 1, 2005, pp. 1-15. doi: 10.1103/PhysRevE.72.011605
18. Peterson, V. K., and Juenger, M. C. G., “Hydration of Tricalcium Silicate: Effects of CaCl2 and Sucrose on Reaction Kinetics and Product Formation,” Chemistry of Materials, V. 18, No. 24, 2006, pp. 5798-5804. doi: 10.1021/cm061724y
19. Taylor, H. F. W., Cement Chemistry, Thomas Telford, 1997.
20. Zhang, J., and Scherer, G. W., “Comparison of Methods for Arresting Hydration of Cement,” Cement and Concrete Research, V. 41, No. 10, 2011, pp. 1024-1036. doi: 10.1016/j.cemconres.2011.06.003
21. Pannetier, N.; Khoukh, A.; and François, J., “Physico-Chemical Study of Sucrose and Calcium Ions Interactions in Alkaline Aqueous Solutions,” Macromolecular Symposia, V. 166, No. 1, 2001, pp. 203-208. doi: 10.1002/1521-3900(200103)166:13.0.CO;2-I