Authors :
A. Abandoh; A. C. K. Amuzu; B. Puzer; F. J. K. Adzabe; S. Anane; L. K. Labik; I. Nkrumah; E. K. K. Abavare; B. Kwakye-Awuah
Volume/Issue :
Volume 10 - 2025, Issue 10 - October
Google Scholar :
https://tinyurl.com/42tzfcf8
Scribd :
https://tinyurl.com/2ts74bjp
DOI :
https://doi.org/10.38124/ijisrt/25oct1118
Note : A published paper may take 4-5 working days from the publication date to appear in PlumX Metrics, Semantic Scholar, and ResearchGate.
Note : Google Scholar may take 30 to 40 days to display the article.
Abstract :
This study employed a facile sol-gel precipitation method to synthesize calcium silicate hydrate (CSH) at room
temperature using oyster shell-derived calcium nitrate and de-aluminated metakaolin-derived sodium silicate as
sustainable precursors. The evolution of CSH gel from an initial stoichiometric Ca/Si molar ratio of 0.68 into crystalline
phases was investigated over different aging periods (1, 3, 7, and 14 days). The microstructural characteristics of the
synthesized CSH were comprehensively analyzed using Fourier transform infrared spectroscopy (FTIR), powder X-ray
diffraction (XRD), X-ray fluorescence spectroscopy (XRF), energy-dispersive X-ray spectroscopy (EDX),
thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). XRF analysis revealed a progressive
increase in Ca/Si ratio from 0.63 (Day 1) to 0.88 (Day 14), indicating enhanced calcium incorporation during aging. FTIR
spectra confirmed the formation of hydrated silicates through characteristic functional groups (O–H, Si–O, and Si–
O(Ca)), with band intensity evolution suggesting increased silicate chain polymerization over time. XRD patterns
confirmed tobermorite-like crystalline phases at extended aging periods, correlating with improved structural ordering.
TGA analysis revealed distinct thermal decomposition profiles attributed to adsorbed water loss, CSH phase dehydration,
and decarbonation. SEM micrographs of 14-day aged CSH exhibited dense, fibrous morphology characteristic of well-
developed CSH phases, while EDX analysis confirmed silicon and calcium as the predominant elements, corroborating
XRF findings. Prolonged aging enhanced crystallinity, calcium content, and polymerization degree, aligning with
properties reported for high-performance cementitious materials. These results demonstrated the viability of utilizing
oyster shells and de-aluminated metakaolin as eco-friendly precursors for CSH synthesis. This study highlights the
potential for valorizing dealuminated metakaolin and oyster shells into advanced materials for sustainable construction
applications; and offers promising pathway for reducing environmental wastes while contributing to greener construction
material development. Future research should focus on optimizing synthesis parameters and evaluating the mechanical
and durability properties of CSH in composite systems.
Keywords :
Calcium Silicate Hydrate (CSH); C/S Ratio; Dealuminated Metakaolin, Period, Oyster-Shell.
References :
- Kumar, A., Walder, B. J., Mohamed, A. K., Hofstetter, A., Rossini, A. J., Scrivener, K., et al., (2017). The Atomic-Level Structure of Cementitious Calcium Silicate Hydrate. Journal of Physical Chemistry C, 121(32), 17188–17196. Retrieved from http://pubs.acs.org.
- Picker, A., Nicoleau, L., Burghard, Z., Bill, J., Zlotnikov, I., Labbez, C., Cölfen, H., et al., (2017). Mesocrystalline calcium silicate hydrate : A bioinspired route toward elastic concrete materials. Science Advances, 3(11), e1701216.
- Kuwahara, Y., Tamagawa, S., Fujitani, T., & Yamashita, H. (2013). A novel conversion process for waste slag: synthesis of calcium silicate hydrate from blast furnace slag and its application as a versatile adsorbent for water purificatio. Journal of Materials Chemistry A, 1, 7199–7210. https://doi.org/10.1039/c3ta11064h.
- Zeng, L., Yang, L., Wang, S., & Yang, K. (2014). Synthesis and Characterization of Different Crystalline Calcium Silicate Hydrate : Application for the Removal of Aflatoxin B1 from Aqueous Solution. Journal of Nanomaterials, 2014, 10. https://doi.org/10.1155/2014/431925.
- Kumar, A., Scrivener, P. K., & Bowen, P. P. (2015). Synthesis of nano-structured Calcium silicate hydrate Powder Technology Laboratory , École Polytechnique Fédérale de Lausanne EPFL , Switzerland. Advanced Materials. Switzerland.
- Martín-Garrido, Moisés Martínez-Ramírez, Sagrario Pérez, G. G. A. (2016). Calcium Silicate Hydrate Characterization by Spectroscopic Techniques. Madrid.
- Zhu, G., Li, H., Wang, X., Li, S., Hou, X., Wu, W., & Tang, Q. (2016). Synthesis of Calcium Silicate Hydrate in Highly Alkaline System. The American Ceramic Society,99(8),2778–2785. https://doi.org/10.1111/jace.14242.
- Estrada-Flores, S., Martiınez-Lu, evanos A., Bartolo-P´erez, P., Garc´ıa- Cerda, L. A., Flores-Guia, T. E., & Aguilera-Gonz´alez, E. N. (2018). Facile synthesis of novel calcium silicate hydrated- nylon 6/66 nanocomposites by solution mixing method. RSC Advances, 8, 41818-41827. https://doi.org/10.1039/c8ra07116k.
- Shuping, W., Xiaoqin, P., Luping, T., Lu, Z., & Cong, L A N, C. (2018). Influence of Hydrothermal Synthesis Conditions on the Formation of Calcium Silicate Hydrates : from Amorphous to Crystalline Phases. Journal of Wuhan University of Technology-Mater. Sci. Ed., 33(5), 1150–1158. https://doi.org/10.1007/s11595-018-1947-0.
- Maddalena, R., Li, K., Chater, P. A., Michalik, S., & Hamilton, A. (2019). Direct synthesis of a solid calcium silicate hydrate (C-S-H). Construction and Building Materials, 223, 554-565. https://doi.org/10.1016/j.conbuildmat.2019.06.024.
- Wang, B., Yao, W., & Stephan, D. (2019). Preparation of calcium silicate hydrate seeds by means of mechanochemical method and its effect on the early hydration of cement. Advances in Mechanical Engineering, 11(4), 1–7. https://doi.org/10.1177/1687814019840586.
- Ogur, E., Botti, R., Bortolotti, M., Colombo, P., Vakifahmetoglu, C., & Industriale, I. (2021). Synthesis and additive manufacturing of calcium silicate hydrate scaffolds. Journal of Materials Research and Technology, 11, 1142–1151. https://doi.org/10.1016/j.jmrt.2021.01.090.
- Qi, F., Zhu, G., & Zhang, Y. (2021). Effect of calcium to silica ratio on the synthesis of calcium silicate hydrate in high alkaline desilication solution. Journal of American Ceramic Society, 104(April 2020), 535–547. https://doi.org/10.1111/jace.17440.
- Harris, A. W., Manning, M. C., Tearle, W. M., & Tweed, C. J. (2002). Testing of models of the dissolution of cements – leaching of synthetic CSH gels, 32, 731-746.
- Chen, J. J., Thomas, J. J., Taylor, H. F. W., & Jennings, H. M. (2004). Solubility and structure of calcium silicate hydrate. Cement and Concrete Reasearch, 34(10), 1499–1519. https://doi.org/10.1016/j.cemconres.2004.04.034.
- Trankle, S., Jahn, D., Neumann, T., Nicoleau, L., Husing, N., & Volkmer, D. (2013). Conventional and microwave assisted hydrothermal syntheses of 11 Å tobermorite. Journal of Materials Chemistry A, 1(35), 10318–10326. https://doi.org/10.1039/c3ta11036b.
- Matsuyama, H. & Young, F. J. (1999). Synthesis of calcium silicate hydrate / polymer complexes : Part. I. Journal of Materials Research and Technology, 14(8), 3379–3388.
- Amuzu, A.C.K., Abandoh, A., Labik, L. k., Puzer, D. B., Gyening, R. O. M., Nkrumah, I., Abavare, E. K. K., & Kwakye-Awuah, B. (2025). Novel Pathway for the Synthesis of High Purity Silica from De-aluminated-metakaolin-derived Sodium Metasilicate Hydrate. International Journal of Innovative Science and Research, x(y), a-b. https://doi.org/10.5281/zenodo.12345678.
- Li, J., Zhang, W., Xu, K., & Monteiro, P. J. M. (2020). Fibrillar calcium silicate hydrate seeds from hydrated tricalcium silicate lower cement demand. Cement and Concrete Reasearch, 137(8), 106195. https://doi.org/10.1016/j.cemconres.2020.106195.
- Biagioni, C., Bonaccorsi, E., Merlino, S., & Bersani, D. (2013). Cement and Concrete Research New data on the thermal behavior of 14 Å tobermorite. Cement and Concrete Research, 49, 48–54. https://doi.org/10.1016/j.cemconres.2013.03.007.
- Yu, P. (2022). Thermal dehydration of tobermorite and jennite. Concrete Science and Engineering, 1(12), 185–191.
- Woo, S., & Choi, Y.-C. (2023). Synthesis of calcium silicate hydrate nanoparticles and their effect on cement hydration and compressive strength. Construction and Building Materials, 407, 133559.
- Augustyniak, A., Sikora, P., Jablonska, J., Cendrowski, K., John, E., Stephan, D., & Mijowska, E. (2020). The effects of calcium – silicate – hydrate ( C – S – H ) seeds on reference microorganisms. Applied Nanoscience, 10(12), 4855–4867. https://doi.org/10.1007/s13204-020-01347-5.
- Cristina, L., Alberto, R., Machado, L. B., Aparecida, L., & Motta, D. C. (2019). Industrial Crops & Products Optimization of metakaolin-based geopolymer reinforced with sisal fibers using response surface methology. Industrial Crops & Products, 139(7), 111551. https://doi.org/10.1016/j.indcrop.2019.111551.
- Kwakye-Awuah, B., Abavare, E. K. K., Ntiri-Sefa, B., Nkrumah, I., & Von-Kiti, E. (2021). Synthesis and characterization of geopolymer ‑ zeolites from Ghanaian Kaolin samples by variation of two synthesis parameters. Journal of Thermal Analysis and Calorimetry, 146(5), 18–21. https://doi.org/10.1007/s10973-021-10710-9.
- Lingyu, T., Dongpo, H., Jianing, Z., & Hongguang, W. (2021). Durability of geopolymers and geopolymer concretes : A review. Reviews on Advanced Materials Science, 60(1), 1–14. https://doi.org/10.1515/rams-2021-0002.
- Tijani, J. O., Bankole, M. T., Hussein, A., Oketoye, J. A., & Abdulkareem, A. S. (2019). Influence of Synthesis Parameters in the Preparation of Silicon (IV) Oxide Nanoparticles from Dealuminated Metakaolin and Metakaolin with Na2SiO3. Journal of Chemical Society of Nigeria, 44(6), 1143–1156.
- Bellei, P., Torres, I., & Solstad, R. (2023). Potential Use of Oyster Shell Waste in the Composition of Construction Composites : A Review. Buildings, 13, 1546. https://doi.org/10.3390/buildings13061546.
- Amaechi, P., Sunday, V., & Inderlal, N. (2023). Modified calcium oxide nanoparticles derived from oyster shells for biodiesel production from waste cooking oil. Fuel Communications, 14(January), 100085. https://doi.org/10.1016/j.jfueco.2023.100085,
- Seesanong, S., Seangarun, C., Boonchom, B., & Laohavisuti, N. (2024). Low-Cost and Eco-Friendly Calcium Oxide Prepared via Thermal Decompositions of Calcium Carbonate and Calcium Acetate. Materials, 17, 3875. https://doi.org/10.3390/ma1715387.
- Richardson, I. G. (2008). The calcium silicate hydrates. Cement and Concrete Reasearch, 38(11), 137–158. https://doi.org/10.1016/j.cemconres.2007.11.005.
- Huang, J., Fan, Y., Mejia, S., Hoyos, B., Chandler, M. Q., Peters, J. F., & Pelessone, D. (2019). Preparation of nano-calcium silicate hydrate and its application in concrete Preparation of nano-calcium silicate hydrate and its application in concrete. Materials and Engineering, 631 (022052), 0–5. https://doi.org/10.1088/1757-899X/631/2/022052.
- Elghniji, K., Virlan, C., Elaloui, E., & Pui, A. (2018). Synthesis , characterization of SiO 2 supported- industrial phosphoric acid catalyst for hydrolysis of NaBH 4 solution. Phosphorus, Sulfur, and Silicon and the Related Elements, 0(0), 1–16. https://doi.org/10.1080/10426507.2018.1515946.
- Wang, B., Yao, W., & Stephan, D. (2019). Preparation of calcium silicate hydrate seeds by means of mechanochemical method and its effect on the early hydration of cement. Advances in Mechanical Engineering, 11(4), 1–7. https://doi.org/10.1177/1687814019840586.
This study employed a facile sol-gel precipitation method to synthesize calcium silicate hydrate (CSH) at room
temperature using oyster shell-derived calcium nitrate and de-aluminated metakaolin-derived sodium silicate as
sustainable precursors. The evolution of CSH gel from an initial stoichiometric Ca/Si molar ratio of 0.68 into crystalline
phases was investigated over different aging periods (1, 3, 7, and 14 days). The microstructural characteristics of the
synthesized CSH were comprehensively analyzed using Fourier transform infrared spectroscopy (FTIR), powder X-ray
diffraction (XRD), X-ray fluorescence spectroscopy (XRF), energy-dispersive X-ray spectroscopy (EDX),
thermogravimetric analysis (TGA), and scanning electron microscopy (SEM). XRF analysis revealed a progressive
increase in Ca/Si ratio from 0.63 (Day 1) to 0.88 (Day 14), indicating enhanced calcium incorporation during aging. FTIR
spectra confirmed the formation of hydrated silicates through characteristic functional groups (O–H, Si–O, and Si–
O(Ca)), with band intensity evolution suggesting increased silicate chain polymerization over time. XRD patterns
confirmed tobermorite-like crystalline phases at extended aging periods, correlating with improved structural ordering.
TGA analysis revealed distinct thermal decomposition profiles attributed to adsorbed water loss, CSH phase dehydration,
and decarbonation. SEM micrographs of 14-day aged CSH exhibited dense, fibrous morphology characteristic of well-
developed CSH phases, while EDX analysis confirmed silicon and calcium as the predominant elements, corroborating
XRF findings. Prolonged aging enhanced crystallinity, calcium content, and polymerization degree, aligning with
properties reported for high-performance cementitious materials. These results demonstrated the viability of utilizing
oyster shells and de-aluminated metakaolin as eco-friendly precursors for CSH synthesis. This study highlights the
potential for valorizing dealuminated metakaolin and oyster shells into advanced materials for sustainable construction
applications; and offers promising pathway for reducing environmental wastes while contributing to greener construction
material development. Future research should focus on optimizing synthesis parameters and evaluating the mechanical
and durability properties of CSH in composite systems.
Keywords :
Calcium Silicate Hydrate (CSH); C/S Ratio; Dealuminated Metakaolin, Period, Oyster-Shell.