Degradation of C–S–H(I) at different decalcification degrees
Source abstract
Abstract
The deterioration of cement-basted materials serviced in leaching environments is strongly dependent on the decalcification behavior of calcium silicate hydrates after complete dissolution of calcium hydroxide. This paper examines the deteriorating condition of calcium silicate hydrates (hereinafter referred to C–S–H(I)) samples with the decalcification degree which is controlled by immersing samples into leaching solutions with different NH4Cl concentrations. The composition, chemical structure, micromorphology and pore structure of un-leached and leached C–S–H(I) samples were determined using XRD, TG, FTIR, 29Si NMR, SEM, TEM and N2 adsorption–desorption measurements. Results reveal that the decalcification degree of C–S–H(I) samples increases with the increasing NH4Cl concentration with the Ca/Si atomic ratio decreasing from 0.91 to 0.02. The area of flocculent micromorphology of C–S–H(I) samples increases with the decalcification degree due to the continuous generation of cross-linking C–S–H(I) and amorphous silica gel. In addition, the decalcification behavior damages the crystallinity, coarsens the pore structure and decreases the chemically-bound water content of C–S–H(I) samples. Molecular dynamics simulations prove that increasing NH4Cl content results in weaker connectivity stability and more breakage of Ca–O bond in C–S–H(I) molecules.
Source: expertdata · Quality: candidate unverified · Source record ↗
Research context
OpenAlex topics: Concrete and Cement Materials Research · Building materials and conservation · CO2 Sequestration and Geologic Interactions
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
References (59)
Show source-provided references
1. Rosenqvist M, Bertron A, Fridh K, Hassanzadeh M (2017) Concrete alteration due to 55years of exposure to river water: chemical and mineralogical characterisation. Cem Concr Res 92:110. https://doi.org/10.1016/j.cemconres.2016.11.01210.1016/j.cemconres.2016.11.012 ↗
2. Neumann C, Faria EF, dos Santos ACP (2021) Concrete leaching of a hydroelectric powerhouse due to 40 years of exposure to river water. Constr Build Mater 302:124253. https://doi.org/10.1016/j.conbuildmat.2021.12425310.1016/j.conbuildmat.2021.124253 ↗
3. Gérard B, Le Bellego C, Bernard O (2002) Simplified modelling of calcium leaching of concrete in various environments. Mater Struct 35:632. https://doi.org/10.1007/BF0248035610.1007/BF02480356 ↗
4. Jain J, Neithalath N (2009) Analysis of calcium leaching behavior of plain and modified cement pastes in pure water. Cem Concr Comp 31:176. https://doi.org/10.1016/j.cemconcomp.2009.01.00310.1016/j.cemconcomp.2009.01.003 ↗
5. Bossa N, Chaurand P, Vicente J et al (2015) Micro- and nano-X-ray computed-tomography: a step forward in the characterization of the pore network of a leached cement paste. Cem Concr Res 67:138. https://doi.org/10.1016/j.cemconres.2014.08.00710.1016/j.cemconres.2014.08.007 ↗
6. Garcia-Lodeiro I, Goracci G, Dolado JS, Blanco-Varela MT (2021) Mineralogical and microstructural alterations in a portland cement paste after an accelerated decalcification process. Cem Concr Res 140. https://doi.org/10.1016/j.cemconres.2020.10631210.1016/j.cemconres.2020.106312 ↗
7. Jiang C, Jiang L, Tang X, Gong J, Chu H (2021) Impact of calcium leaching on mechanical and physical behaviors of high belite cement pastes. Constr Build Mater 286:122983. https://doi.org/10.1016/j.conbuildmat.2021.12298310.1016/j.conbuildmat.2021.122983 ↗
8. Jiang C, Yu L, Tang X, Chu H, Jiang L (2021) Deterioration process of high belite cement paste exposed to sulfate attack, calcium leaching and the dual actions. J Mater Res Tech 15:2982. https://doi.org/10.1016/j.jmrt.2021.09.12510.1016/j.jmrt.2021.09.125 ↗
9. Liu L, Wang X, Zhou J et al (2018) Investigation of pore structure and mechanical property of cement paste subjected to the coupled action of freezing/thawing and calcium leaching. Cem Concr Res 109:133. https://doi.org/10.1016/j.cemconres.2018.04.01510.1016/j.cemconres.2018.04.015 ↗
10. Kumar A, Walder BJ, Mohamed AK et al (2017) The atomic-level structure of cementitious calcium silicate hydrate. J Phys Chem C 121:17188. https://doi.org/10.1021/acs.jpcc.7b0243910.1021/acs.jpcc.7b02439 ↗
11. NCM Marty, S Grangeon, F Warmont, C Lerouge (2018) Alteration of nanocrystalline calcium silicate hydrate (C-S-H) at pH 9.2 and room temperature: a combined mineralogical and chemical study. Mineral Mag 79: 437. https://doi.org/10.1180/minmag.2015.079.2.2010.1180/minmag.2015.079.2.20 ↗
12. Liu H, Chen W, Pan R et al (2020) From molten calcium aluminates through phase transitions to cement phases. Adv Sci 7:1902209. https://doi.org/10.1002/advs.20190220910.1002/advs.201902209 ↗
13. Zhou Y, Zheng H, Li W, Ma T, Miao C (2022) A deep learning potential applied in tobermorite phases and extended to calcium silicate hydrates. Cem Concr Res 152:106685. https://doi.org/10.1016/j.cemconres.2021.10668510.1016/j.cemconres.2021.106685 ↗
14. Trapote-Barreira A, Cama J, Soler JM (2014) Dissolution kinetics of C-S–H gel: Flow-through experiments. Phys Chem Earth A/B/C 70–71:17. https://doi.org/10.1016/j.pce.2013.11.00310.1016/j.pce.2013.11.003 ↗
15. Chen T, Gao X (2019) How carbonation curing influences ca leaching of Portland cement paste: mechanism and mathematical modeling. J Am Ceram Soc 102:7755. https://doi.org/10.1111/jace.1668410.1111/jace.16684 ↗
16. Choi YS, Yang EI (2013) Effect of calcium leaching on the pore structure, strength, and chloride penetration resistance in concrete specimens. Nucl Eng Des 259:126. https://doi.org/10.1016/j.nucengdes.2013.02.04910.1016/j.nucengdes.2013.02.049 ↗
17. Constantinides G, Ulm F-J (2004) The effect of two types of C-S-H on the elasticity of cement-based materials: results from nanoindentation and micromechanical modeling. Cem Concr Res 34:67. https://doi.org/10.1016/s0008-8846(03)00230-810.1016/s0008-8846(03)00230-8 ↗
18. Chen JJ, Thomas JJ, Jennings HM (2006) Decalcification shrinkage of cement paste. Cem Concr Res 36:801. https://doi.org/10.1016/j.cemconres.2005.11.00310.1016/j.cemconres.2005.11.003 ↗
19. Hou D, Li H, Zhang L, Zhang J (2018) Nano-scale mechanical properties investigation of C-S-H from hydrated tri-calcium silicate by nano-indentation and molecular dynamics simulation. Constr Build Mater 189:265. https://doi.org/10.1016/j.conbuildmat.2018.08.21510.1016/j.conbuildmat.2018.08.215 ↗
20. IG Richardson (2014) Model structures for C-(A)-S-H(I). Acta Crystallog B Struct Sci Cryst Eng Mater 70: 903. https://doi.org/10.1107/S205252061402198210.1107/S2052520614021982 ↗
21. Allen AJ, Thomas JJ, Jennings HM (2007) Composition and density of nanoscale calcium-silicate-hydrate in cement. Nat Mater 6:311. https://doi.org/10.1038/nmat187110.1038/nmat1871 ↗
22. Richardson IG (1999) The nature of C-S-H in hardened cements. Cem Concr Res 29:1131. https://doi.org/10.1016/S0008-8846(99)00168-410.1016/S0008-8846(99)00168-4 ↗
23. MCM AW, Harris WM, Tearle CJ Tweed (2002) Testing of models of the dissolution of cements—leaching of synthetic CSH gels. Cem Concr Res10.1016/S0008-8846(01)00748-7 ↗
24. Liu X, Feng P, Li W et al (2021) Effects of pH on the nano/micro structure of calcium silicate hydrate (C-S-H) under sulfate attack. Cem Concr Res 140:106306. https://doi.org/10.1016/j.cemconres.2020.10630610.1016/j.cemconres.2020.106306 ↗
25. Liu L, Sun C, Geng G, Feng P, Li J, Dähn R (2019) Influence of decalcification on structural and mechanical properties of synthetic calcium silicate hydrate (C-S-H). Cem Concr Res 123:105793. https://doi.org/10.1016/j.cemconres.2019.10579310.1016/j.cemconres.2019.105793 ↗
26. Hu Z, Wyrzykowski M, Griffa M, Scrivener K, Lura P (2020) Young’s modulus and creep of calcium-silicate-hydrate compacts measured by microindentation. Cem Concr Res 134:106104. https://doi.org/10.1016/j.cemconres.2020.10610410.1016/j.cemconres.2020.106104 ↗
27. Brunauer S, Emmett PH, Teller E (1938) Adsorption of gases in multimolecular layers. J Am Chem Soc 60:30910.1021/ja01269a023 ↗
28. Pellenq RJ, Kushima A, Shahsavari R et al (2009) A realistic molecular model of cement hydrates. Proc Natl Acad Sci 106:16102. https://doi.org/10.1073/pnas.090218010610.1073/pnas.0902180106 ↗
29. Kalinichev AG, Kirkpatrick RJ (2002) Molecular dynamics modeling of chloride binding to the surfaces of calcium hydroxide, hydrated calcium aluminate, and calcium silicate phases. Chem Mater 14:353910.1021/cm0107070 ↗
30. Kalinichev AG, Wang J, Kirkpatrick RJ (2007) Molecular dynamics modeling of the structure, dynamics and energetics of mineral–water interfaces: Application to cement materials. Cem Concr Res 37:33710.1016/j.cemconres.2006.07.004 ↗
31. Richard T, Mercury L, Poulet F, d’Hendecourt L (2006) Diffuse reflectance infrared Fourier transform spectroscopy as a tool to characterise water in adsorption/confinement situations. J Colloid Interface Sci 304:125. https://doi.org/10.1016/j.jcis.2006.08.03610.1016/j.jcis.2006.08.036 ↗
32. Yu P, Kirkpatrick RJ, Poe B, McMillan PF, Cong XD (1999) Structure of calcium silicate hydrate (C-S-H): Near-, mid-, and far-infrared spectroscopy. J Am Ceram Soc 82:74210.1111/j.1151-2916.1999.tb01826.x ↗
33. García Lodeiro I, Macphee DE, Palomo A, Fernández-Jiménez A (2009) Effect of alkalis on fresh C-S–H gels. FTIR analysis Cem Concr Res 39:147. https://doi.org/10.1016/j.cemconres.2009.01.00310.1016/j.cemconres.2009.01.003 ↗
34. Mollah MY, Kesmez M, Cocke DL (2004) An X-ray diffraction (XRD) and Fourier transform infrared spectroscopic (FT-IR) investigation of the long-term effect on the solidification/stabilization (S/S) of arsenic(V) in Portland cement type-V. Sci Total Environ 325:255. https://doi.org/10.1016/j.scitotenv.2003.09.01210.1016/j.scitotenv.2003.09.012 ↗
35. Kurumisawa K, Nawa T, Owada H, Shibata M (2013) Deteriorated hardened cement paste structure analyzed by XPS and 29Si NMR techniques. Cem Concr Res 52:190. https://doi.org/10.1016/j.cemconres.2013.07.00310.1016/j.cemconres.2013.07.003 ↗
36. Ibrahim DM, El-Hemaly SA, Abdel-Kerim FM (1980) Study of rice-husk ash silica by infrared spectroscopy. Thermochim Acta 37:307. https://doi.org/10.1016/0040-6031(80)87160-710.1016/0040-6031(80)87160-7 ↗
37. Pustovgar E, Sangodkar RP, Andreev AS et al (2016) Understanding silicate hydration from quantitative analyses of hydrating tricalcium silicates. Nat Commun 7:10952. https://doi.org/10.1038/ncomms1095210.1038/ncomms10952 ↗
38. Kanchanason V, Plank J (2017) Role of pH on the structure, composition and morphology of C-S-H–PCE nanocomposites and their effect on early strength development of Portland cement. Cem Concr Res 102:90. https://doi.org/10.1016/j.cemconres.2017.09.00210.1016/j.cemconres.2017.09.002 ↗
39. Yang M, Zheng Y, Li X, Yang X, Rao F, Zhong L (2022) Durability of alkali-activated materials with different C-S–H and N-A-S-H gels in acid and alkaline environment. J Mater Res Tech 16:619. https://doi.org/10.1016/j.jmrt.2021.12.03110.1016/j.jmrt.2021.12.031 ↗
40. Gaboreau S, Grangeon S, Claret F et al (2020) Hydration properties and interlayer organization in synthetic C-S-H. Langmuir 36:9449. https://doi.org/10.1021/acs.langmuir.0c0133510.1021/acs.langmuir.0c01335 ↗
41. Li J, Yu Q, Huang H, Yin S (2019) Effects of Ca/Si ratio, aluminum and magnesium on the carbonation behavior of calcium silicate hydrate. Materials (Basel) 12. https://doi.org/10.3390/ma1208126810.3390/ma12081268 ↗
42. Zhu X, Qian C, He B, Chen Q, Jiang Z (2020) Experimental study on the stability of C-S-H nanostructures with varying bulk CaO/SiO2 ratios under cryogenic attack. Cem Concr Res 135:106114. https://doi.org/10.1016/j.cemconres.2020.10611410.1016/j.cemconres.2020.106114 ↗
43. Tajuelo Rodriguez E, Garbev K, Merz D, Black L, Richardson IG (2017) Thermal stability of C-S-H phases and applicability of Richardson and Groves’ and Richardson C-(A)-S-H(I) models to synthetic C-S-H. Cem Concr Res 93:45. https://doi.org/10.1016/j.cemconres.2016.12.00510.1016/j.cemconres.2016.12.005 ↗
44. Liu X, Feng P, Cai Y, Yu X, Yu C, Ran Q (2022) Carbonation behavior of calcium silicate hydrate (C-S-H): Its potential for CO2 capture. Chem Eng J 431. https://doi.org/10.1016/j.cej.2021.13424310.1016/j.cej.2021.134243 ↗
45. Kangni-Foli E, Poyet S, Le Bescop P et al (2021) Carbonation of model cement pastes: The mineralogical origin of microstructural changes and shrinkage. Cem Concr Res 144:106446. https://doi.org/10.1016/j.cemconres.2021.10644610.1016/j.cemconres.2021.106446 ↗
46. Alarcon-Ruiz L, Platret G, Massieu E, Ehrlacher A (2005) The use of thermal analysis in assessing the effect of temperature on a cement paste. Cem Concr Res 35:609. https://doi.org/10.1016/j.cemconres.2004.06.01510.1016/j.cemconres.2004.06.015 ↗
47. Roosz C, Gaboreau S, Grangeon S et al (2016) Distribution of water in synthetic calcium silicate hydrates. Langmuir 32:6794. https://doi.org/10.1021/acs.langmuir.6b0087810.1021/acs.langmuir.6b00878 ↗
48. Maruyama I, Ohkubo T, Haji T, Kurihara R (2019) Dynamic microstructural evolution of hardened cement paste during first drying monitored by 1H NMR relaxometry. Cem Concr Res 122:107. https://doi.org/10.1016/j.cemconres.2019.04.01710.1016/j.cemconres.2019.04.017 ↗
49. Tajuelo Rodriguez E, Richardson IG, Black L, Boehm-Courjault E, Nonat A, Skibsted J (2015) Composition, silicate anion structure and morphology of calcium silicate hydrates (C-S-H) synthesised by silica-lime reaction and by controlled hydration of tricalcium silicate (C3S). Adv Appl Ceram 114:362. https://doi.org/10.1179/1743676115y.000000003810.1179/1743676115y.0000000038 ↗
50. Zheng Q, Jiang J, Li X, Bustillo KC, Zheng H (2021) In situ TEM observation of calcium silicate hydrate nanostructure at high temperatures. Cem Concr Res 149. https://doi.org/10.1016/j.cemconres.2021.10657910.1016/j.cemconres.2021.106579 ↗
51. Sevelsted TF, Skibsted J (2015) Carbonation of C-S–H and C–A–S–H samples studied by 13 C, 27 Al and 29 Si MAS NMR spectroscopy. Cem Concr Res 71:56. https://doi.org/10.1016/j.cemconres.2015.01.01910.1016/j.cemconres.2015.01.019 ↗
52. Dambrauskas T, Davidoviciene D, Baltakys K et al (2022) Effect of intercalated metal ions on the specific surface area and porosity of dibasic calcium silicate hydrate. Surfaces and Interfaces 33. https://doi.org/10.1016/j.surfin.2022.10224310.1016/j.surfin.2022.102243 ↗
53. Zhu X, He B, Xie M, Zhang Y, Jiang Z (2021) A comprehensive nitrogen adsorption measurement on the pore structure of calcium-silicate-hydrate subjected to cryogenic attack. Measurement 184. https://doi.org/10.1016/j.measurement.2021.10994110.1016/j.measurement.2021.109941 ↗
54. Dambrauskas T, Baltakys K, Eisinas A, Kitrys S (2019) The specific surface area and porosity of synthetic and calcined α-C2SH, kilchoanite and hydroxyledgrewite. Powder Technol 355:504. https://doi.org/10.1016/j.powtec.2019.07.07810.1016/j.powtec.2019.07.078 ↗
55. Thommes M, Kaneko K, Neimark AV et al (2015) Physisorption of gases, with special reference to the evaluation of surface area and pore size distribution (IUPAC Technical Report). Pure Appl Chem 87:1051. https://doi.org/10.1515/pac-2014-111710.1515/pac-2014-1117 ↗
56. JJ Chen, JJ Thomas, HM Jennings (2015) Preparation of single-phase CSH specimens from hydrated tricalcium silicate pastes. Civil Northwestern Edu, 1.
57. Hay R, Li J, Celik K (2022) Phase evolution, micromechanical properties, and morphology of calcium (alumino)silicate hydrates C-(A-)S-H under carbonation. Cem Concr Res 152. https://doi.org/10.1016/j.cemconres.2021.10668310.1016/j.cemconres.2021.106683 ↗
58. Luzar A, Chandler D (1996) Hydrogen-bond kinetics in liquid water. Nature 379:5510.1038/379055a0 ↗
59. Zhou Y, Hou D, Manzano H et al (2017) Interfacial connection mechanisms in calcium-silicate-hydrates/polymer nanocomposites: a molecular dynamics study. ACS Appl Mater Interfaces 9:41014. https://doi.org/10.1021/acsami.7b1279510.1021/acsami.7b12795 ↗