Title:
Study of Hydration Process of Cement Paste with Chemical Mapping
Author(s):
Fengjuan Liu and Zhihui Sun
Publication:
Materials Journal
Volume:
113
Issue:
5
Appears on pages(s):
609-619
Keywords:
chemical mapping; hydration; microstructure; quantitative analysis; Raman spectroscopy
DOI:
10.14359/51689106
Date:
9/1/2016
Abstract:
In the present study, chemical mapping on the hydration process of cement pastes with water-cement ratios (w/c) of 0.35 to 0.60 was implemented by Raman spectroscopy (RS) from 12 hours after mixing until 28 days. Both the cement ingredients and hydration products were quantitatively studied. From the research, the content of calcium silicates (C3S and C2S) was observed to decrease rapidly during the first 3 days and then the decreasing rate slowed down. As one of the major hydration products, calcium hydroxide increased and tended to cluster in the pore vicinity with hydration progress. It was the only compound that could be detected as a pure phase in some measured regions. Ettringite was found to form on the surface of the unreacted cement particles, which was shown as a mixed zone of ettringite and calcium silicates in the maps. The RS chemical mapping results concurred with the scanning electron microscopy images collected from the same pastes.
Related References:
1. Bullard, J. W.; Jennings, H. M.; Livingston, R. A.; Nonat, A.; Scherer, G. W.; Schweitzer, J. S.; Scrivener, K. L.; and Thomas, J. J., “Mechanisms of Cement Hydration,” Cement and Concrete Research, V. 41, No. 12, 2011, pp. 1208-1223. doi: 10.1016/j.cemconres.2010.09.011
2. Scrivener, K. L.; Fullmann, T.; Gallucci, E.; Walenta, G.; and Bermejo, E., “Quantitative Study of Portland Cement Hydration by X-Ray Diffraction/Rietveld Analysis and Independent Methods,” Cement and Concrete Research, V. 34, No. 9, 2004, pp. 1541-1547. doi: 10.1016/j.cemconres.2004.04.014
3. Korpa, A.; Kowald, T.; and Trettin, R., “Phase Development in Normal and Ultra High Performance Cementitious Systems by Quantitative X-Ray Analysis and Thermoanalytical Methods,” Cement and Concrete Research, V. 39, No. 2, 2009, pp. 69-76. doi: 10.1016/j.cemconres.2008.11.003
4. Ylmén, R.; Jaglid, U.; Steenari, B. M.; and Panas, I., “Early Hydration and Setting of Portland Cement Monitored by IR, SEM, and Vicat Technique,” Cement and Concrete Research, V. 39, No. 5, 2009, pp. 433-439. doi: 10.1016/j.cemconres.2009.01.017
5. Zingg, A.; Holzer, L.; Kaech, A.; Winnefeld, F.; Pakusch, J.; Becker, S.; and Gauckler, L., “The Microstructure of Dispersed and Non-Dispersed Fresh Cement Paste—New Insight by Cryo-Microscopy,” Cement and Concrete Research, V. 38, No. 4, 2008, pp. 522-529. doi: 10.1016/j.cemconres.2007.11.007
6. Venkiteela, G., and Sun, Z., “In-Situ Observation of Cement Particle Growth during Setting,” Cement and Concrete Composites, V. 32, No. 3, 2010, pp. 211-218. doi: 10.1016/j.cemconcomp.2009.12.003
7. Stutzman, P. E., “Scanning Electron Microscopy in Concrete Petrography,” J. Skalny, J. Gebauer, and I. Odler, eds., Material Science of Concrete, Special Volume: Calcium Hydroxide in Concrete, The American Ceramic Society, Westerville, OH, 2001, pp. 59-72.
8. Bensted, J., “Use of Raman Spectroscopy in Cement Chemistry,” Journal of the American Ceramic Society, V. 59, No. 3-4, 1976, pp. 140-143. doi: 10.1111/j.1151-2916.1976.tb09451.x
9. Conjeaud, M., and Boyer, H., “Some Possibilities of Raman Microprobe in Cement Chemistry,” Cement and Concrete Research, V. 10, No. 1, 1980, pp. 61-70. doi: 10.1016/0008-8846(80)90052-6
10. Bonen, D.; Johnson, T. J.; and Sarkar, S. L., “Characterization of Principal Clinker Materials by FT-Raman Microspectroscopy,” Cement and Concrete Research, V. 24, No. 5, 1994, pp. 959-965. doi: 10.1016/0008-8846(94)90016-7
11. Newman, S. P.; Clifford, S. J.; Coveney, P. V.; Gupta, V.; Blanchard, J. D.; Serafin, F.; Ben-Amotz, D.; and Diamond, S., “Anomalous Fluorescence in Near-Infrared Raman Spectroscopy of Cementitious Materials,” Cement and Concrete Research, V. 35, No. 8, 2005, pp. 1620-1628. doi: 10.1016/j.cemconres.2004.10.001
12. Gastaldi, D.; Boccaleri, E.; Canonico, F.; and Bianchi, M., “The Use of Raman Spectroscopy as a Versatile Characterization Tool for Calciumsulphoaluminate Cements: A Compositional and Hydration Study,” Journal of Materials Science, V. 42, No. 20, 2007, pp. 8426-8432. doi: 10.1007/s10853-007-1790-8
13. Frías, M., and Martínez-Ramírez, S., “Use of Micro-Raman Spectroscopy to Study Reaction Kinetics in Blended White Cement Pastes Containing Metakaolin,” Journal of Raman Spectroscopy, V. 40, No. 12, 2009, pp. 2063-2068. doi: 10.1002/jrs.2372
14. Torréns-Martín, D.; Fernández-Carrasco, L.; and Martínez-Ramírez, S., “Hydration of Calcium Aluminates and Calcium Sulfoaluminate Studied by Raman Spectroscopy,” Cement and Concrete Research, V. 47, May, 2013, pp. 43-50. doi: 10.1016/j.cemconres.2013.01.015
15. Garbev, K.; Stemmermann, P.; Black, L.; Breen, C.; Yarwood, J.; and Gasharova, B., “Structural Features of C-S-H (I) and its Carbonation in Air—A Raman Spectroscopic Study. Part I: Fresh Phases,” Journal of the American Ceramic Society, V. 90, No. 3, 2007, pp. 900-907. doi: 10.1111/j.1551-2916.2006.01428.x
16. Kirkpatrick, R. J.; Yarger, J. L.; McMillan, P. F.; Ping, Y.; and Cong, X., “Raman Spectroscopy of C-S-H, Tobermorite, and Jennite,” Advanced Cement Based Materials, V. 5, No. 3-4, 1997, pp. 93-99. doi: 10.1016/S1065-7355(97)00001-1
17. Black, L.; Breen, C.; Yarwood, J.; Garbev, K.; Stemmermann, P.; and Gasharova, B., “Structural Features of C-S-H (I) and its Carbonation in Air—A Raman Spectroscopic Study. Part II: Carbonated Phases,” Journal of the American Ceramic Society, V. 90, No. 3, 2007, pp. 908-917. doi: 10.1111/j.1551-2916.2006.01429.x
18. Liu, F.; Sun, Z.; and Qi, C., “Raman Spectroscopy of the Dehydration Process of Gypsums,” Advances in Cement Research, V. 27, No. 8, 2015, pp. 434-446. doi: 10.1680/jadcr.14.00086
19. Tarrida, M.; Madon, M.; Le Rolland, B.; and Colombet, P., “An In-Situ Raman Spectroscopy Study of the Hydration of Tricalcium Silicate,” Advanced Cement Based Materials, V. 2, No. 1, 1995, pp. 15-20. doi: 10.1016/1065-7355(95)90035-7
20. Black, L.; Breen, C.; Yarwood, J.; Deng, C.-S.; Phipps, J.; and Maitland, G., “Hydration of Tricalcium Aluminate (C3A) in the Presence and Absence of Gypsum—Studied by Raman Spectroscopy and X-Ray Diffraction,” Journal of Materials Chemistry, V. 16, No. 13, 2006, pp. 1263-1272. doi: 10.1039/b509904h
21. Garg, N.; Wang, K.; and Martin, S. W., “A Raman Spectroscopic Study of Evolution of Sulfates and Hydroxides in Cement-Fly Ash Pastes,” Cement and Concrete Research, V. 53, Nov, 2013, pp. 91-103. doi: 10.1016/j.cemconres.2013.06.009
22. Liu, F., and Sun, Z., “Feasibility Study of Using Raman Spectroscopy to Detect Hydration in Wet Paste,” ACI Materials Journal, V. 110, No. 6, Nov.-Dec. 2013, pp. 611-618.
23. Liu, F.; Sun, Z.; and Qi, C., “Raman Spectroscopy Study on the Hydration Behaviors of Portland Cement Pastes during Setting,” Journal of Materials in Civil Engineering, ASCE, V. 27, No. 8, 2015, p. 04014223 doi: 10.1061/(ASCE)MT.1943-5533.0001189
24. Zhang, L.; Henson, M. J.; and Sekulic, S. S., “Multivariate Data Analysis for Raman Imaging of a Model Pharmaceutical Tablet,” Analytica Chimica Acta, V. 545, No. 2, 2005, pp. 262-278. doi: 10.1016/j.aca.2005.04.080
25. Belu, A.; Mahoney, C.; and Wormuth, K., “Chemical Imaging of Drug Eluting Coatings: Combining Surface Analysis and Confocal Raman Microscopy,” Journal of Controlled Release, V. 126, No. 2, 2008, pp. 111-121. doi: 10.1016/j.jconrel.2007.11.015
26. Fischer, H.; Ibach, W.; Dampel, H.; and Sanchen, D., “A Confocal Raman Imaging Study on Emulsions,” Imaging & Microscopy, V. 11, No. 4, 2009, pp. 35-38. doi: 10.1002/imic.200990085
27. Gordon, K. C., and McGoverin, C. M., “Raman Mapping of Pharmaceuticals,” International Journal of Pharmaceutics, V. 417, No. 1-2, 2011, pp. 151-162. doi: 10.1016/j.ijpharm.2010.12.030
28. Jallad, K. N.; Santhanam, M.; Cohen, M. D.; and Ben-Amotz, D., “Chemical Mapping of Thaumasite Formed in Sulfate-Attacked Cement Mortar using Near-Infrared Raman Imaging Microscopy,” Cement and Concrete Research, V. 31, No. 6, 2001, pp. 953-958. doi: 10.1016/S0008-8846(01)00514-2
29. Taylor, H. F. W., Cement Chemistry, second edition, Thomas Telford, London, UK, 1997, 459 pp.
30. Feldman, R. F., and Beaudoin, J. J., “Pretreatment of Hardened Hydrated Cement Pastes for Mercury Intrusion Measurements,” Cement and Concrete Research, V. 21, No. 2-3, 1991, pp. 297-308. doi: 10.1016/0008-8846(91)90011-6
31. Konecny, L., and Naqvi, S. J., “The Effect of Different Drying Techniques on the Pore Size Distribution of Blended Cement Mortars,” Cement and Concrete Research, V. 23, No. 5, 1993, pp. 1223-1228. doi: 10.1016/0008-8846(93)90183-A
32. Collier, N. C.; Sharp, J. H.; Milestone, N. B.; Hill, J.; and Godfrey, I. H., “The Influence of Water Removal Techniques on the Composition and Microstructure of Hardened Cement Pastes,” Cement and Concrete Research, V. 38, No. 6, 2008, pp. 737-744. doi: 10.1016/j.cemconres.2008.02.012
33. Kontoyannis, C. G.; Bouropoulos, N.; and Koutsoukos, P. G., “Raman Spectroscopy: A Tool for the Quantitative Analysis of Mineral Components of Solid Mixtures. The Case of Calcium Oxalate Monohydrate and Hydroxyapatite,” Vibrational Spectroscopy, V. 15, No. 1, 1997, pp. 53-60. doi: 10.1016/S0924-2031(97)00025-8
34. Scrivener, K. L., “Backscattered Electron Imaging of Cementitious Microstructures: Understanding and Quantification,” Cement and Concrete Composites, V. 26, No. 8, 2004, pp. 935-945. doi: 10.1016/j.cemconcomp.2004.02.029
35. Kjellsen, K. O., and Justnes, H., “Revisiting the Microstructure of Hydrated Tricalcium Silicate—A Comparison to Portland Cement,” Cement and Concrete Composites, V. 26, No. 8, 2004, pp. 947-956. doi: 10.1016/j.cemconcomp.2004.02.030
36. Carino, N. J., “Maturity Functions for Concrete,” Proceedings of International Conference on Concrete at Early Ages, RILEM, Paris, France, V. 1, 1982, pp. 123-128.
37. Eren, O., “Strength Development of Concretes with Ordinary Portland Cement, Slag or Fly Ash Cured at Different Temperatures,” Materials and Structures, V. 35, No. 9, 2002, pp. 536-540. doi: 10.1007/BF02483121
38. Thomas, J. J.; Biernacki, J. J.; Bullard, J. W.; Bishnoi, S.; Dolado, J. S.; Scherer, G. W.; and Luttge, A., “Modeling and Simulation of Cement Hydration Kinetics and Microstructure Development,” Cement and Concrete Research, V. 41, No. 12, 2011, pp. 1257-1278. doi: 10.1016/j.cemconres.2010.10.004
39. Abd elaty, M., “Compressive Strength Prediction of Portland Cement Concrete with Age Using a New Model,” HBRC Journal, V. 10, No. 2, 2014, pp. 145-155. doi: 10.1016/j.hbrcj.2013.09.005