Abstract
Breakdown of porous materials by salts occurs when growing crystals exert pressure on the pore walls, inducing stress in the material that exceeds its tensile strength. In this work, we quantify the mechanical stresses caused by a particularly destructive mechanism: the dissolution of an anhydrate (thenardite, Na2SO4) followed by precipitation of a hydrated salt (mirabilite, Na2SO4·10H2O). Stresses are measured using a composite specimen consisting of a plate of glass bonded to a plate of limestone (CaCO3) whose pores are impregnated with thenardite. As water wicks into the limestone, thenardite dissolves and mirabilite precipitates. The limestone expands from the pressure exerted by the salt resulting in deflection of the composite, and the stresses can be obtained from an elastic analysis. Synchrotron x-ray diffraction reveals the dissolution–crystallization rate. Numerical modeling shows that the stresses are affected by the kinetics of crystallization and dissolution, permeability, and mechanical properties of the stone, allowing us to determine the amount of salt that causes material fracture.
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References
I.S. Evans: Salt crystallization and rock weathering. Revue de Géomorphologie dynamique 19 (4), 153 (1969).
F.J.P.M. Kwaad: Experiments on the granular disintegration of granite by salt action. Fysisch Geografisch en Bodemkundig Laboratorium 16, 67 (1970).
A.S. Goudie: Further experimental investigation of rock weathering by salt and other mechanical processes. Z. Geomorphol. Suppl. 21,1 (1974).
G.W. Scherer: Crystallization in pores. Cem. Concr. Res. 29, 1347 (1999).
C. Rodriguez-Navarro and E. Doehne: Salt weathering: Influence of evaporation rate, supersaturation and crystallization pattern. Earth Surf. Processes Landforms 24, 191 (1999).
C. Rodriguez-Navarro, E. Doehne, and E. Sebastian: How does sodium sulfate crystallize? Implications for the decay and testing of building materials. Cem. Concr. Res. 30, 1527 (2000).
R.J. Flatt: Salt damage in porous materials: How high supersaturations are generated. J. Cryst. Growth 242, 435 (2002).
G.W. Scherer: Stress from crystallization of salt. Cem. Concr. Res. 34, 1613 (2004).
O. Coussy: Deformation and stress from in-pore drying-induced crystallization of salt. J. Mech. Phys. Solids 54, 1517 (2006).
E. Ruiz-Agudo, F. Mees, P. Jacob, and C. Rodriguez-Navarro: The role of saline solution properties on porous limestone salt weathering by magnesium and sodium sulfates. Environ. Geol. 52, 269 (2007).
A. Hamilton, C. Hall, and L. Pel: Salt damage and the forgotten metastable sodium sulfate heptahydrate: Direct observation of crystallization in a porous material. J. Phys. D: Appl. Phys. 41, 212002 (2008).
M. Steiger and S. Asmussen: Crystallization of sodium sulfate phases in porous materials: The phase diagram Na2SO4–H2O and the generation of stress. Geochim. Cosmochim. Acta 72, 4291 (2008).
M. Steiger and K. Linnow: Hydration of MgSO4·H2O and generation of stress in porous materials. Cryst. Growth Des. 8, 336 (2008).
R.M. Espinosa-Marzal and G.W. Scherer: Crystallization of sodium sulfate salts in limestone. Environ. Geol. 56, 605 (2008).
R.M. Espinosa-Marzal and G.W. Scherer: Study of the pore clogging induced by salt crystallization, in Proceedings of the 11th International Congress on Deterioration and Conservation of Stone, September 15–20, 2008 (Nicolaus Copernicus University Press, Torun, Poland), p. 81.
A. Goudie and H. Viles: Salt Weathering Hazards (Wiley, Chichester, 1997).
E. Doehne: Salt weathering: A selective review, in Natural Stone, Weathering Phenomena, Conservation Strategies and Case Studies, edited by S. Siegesmund, A. Vollbrecht, and T. Weiss (Geological Society Special Publication 205, London, 2003), p. 51.
H. Loewel: Observations sur la sursaturation des dissolutions salines. Ann. Chim. Phys. 29, 62 (1850).
J. Thomson: On the disintegration of stones exposed in buildings and otherwise to atmospheric influence. Report of the Annual Meeting, British Association for the Advancement of Science, p. 35 (1862).
J. Lavalle: Research on the slow growth of crystals at ambient temperature. C. R. Acad. Sci. Paris 36, 493 (1853).
S. Taber: The growth of crystals under external pressure. Am. J. Sci. 41, 532 (1916).
C.W. Correns and W. Steinborn: Experimente zur Messung und Erklärung der sogenannten Kristallisationskraft. Z. Krist. (A) 101, 117 (1939).
C.W. Correns: Growth and dissolution of crystals under linear pressure. Discuss. Faraday Soc. 5, 267 (1949).
R.J. Flatt, M. Steiger, and G.W. Scherer: A commented translation of the paper by C.W. Correns and W. Steinborn on crystallization pressure. Environ. Geol. 52, 187 (2007).
M. Steiger: Crystal growth in porous materials I: The crystallization pressure of large crystals. J. Cryst. Growth 282, 455 (2005).
M. Steiger: Crystal growth in porous materials II: Influence of crystal size on the crystallization pressure. J. Cryst. Growth 282, 470 (2005).
R.M. Espinosa, L. Franke, and G. Deckelmann: Model for the mechanical stress due to the salt crystallization in porous materials. J. Constr. Build. Mat. 22, 1350 (2007).
S. Chatterji and A.D. Jensen: Efflorescence and breakdown of building materials. Nordic Concr. Res. 8, 56 (1989).
N. Tsui, R.J. Flatt, and G.W. Scherer: Crystallization damage by sodium sulfate. J. Cult. Herit. 4, 109 (2003).
R.U. Cooke: Laboratory simulation of salt weathering processes in arid environments. Earth Surf. Processes 4, 347 (1979).
ASTM C 88-90: Standard test method for soundness of aggregate by use of sodium sulfate or magnesium sulfate. Annu. Book ASTM Stand. 4.2, p. 37 (1997).
RILEM 1980: Recommended tests to measure the deterioration of stones and assess the effectiveness of treatment methods. Commission 25-PEM: Protection et Erosion des Monuments, p. 175 (1980).
O. Coussy: Poromechanics (John Wiley & Sons, 2004).
H. van Olphen: An Introduction to Clay Colloid Chemistry, 2nd ed. (Wiley, NY, 1977).
W. Vichit-Vadakan and G.W. Scherer: Measuring permeability of rigid materials by a beam-bending method: II. Porous vycor. J. Am. Ceram. Soc. 83, 2240 (2000). Erratum J. Am. Ceram. Soc. 87, 1614(2004).
G.W. Scherer and I. Jiménez González: Characterization of swelling in clay-bearing stone, in Stone Decay and Conservation, SP-390, edited by A.V. Turkington (Geological Society of America, Boulder, CO 2005) pp. 51–61.
T. Metzger, A. Irawan, and E. Tsotsas: Influence of pore structure on drying kinetics: A pore network study. Am. Inst. Chem. Eng. 53, 3029 (2007).
B. Haimson: Micromechanisms of borehole instability leading to breakouts in rocks. Int. J. Rock Mech. Min. Sci. 44, 157 (2007).
O. Katz, Z. Rechesa, and J.C. Roegiers: Evaluation of mechanical rock properties using a Schmidt Hammer. Int. J. Rock Mech. Min. Sci. 37, 723 (2000).
G. Dharmasena and R. Frech: The stabilization of phase III and phase I in sodium sulfate by aliovalent cation substitution. J. Chem. Phys. 99, 8929 (1993).
G.W. Scherer: Drying gels: III. Warping plate. J. Non-Cryst. Solids 91, 83 (1987).
T.P. Wangler, A. Stratulat, P. Duffus, J.-H. Prévost, and G.W. Scherer: Flaw propagation and buckling in clay-bearing sandstones. Environ. Earth Sci. (2010) doi: 10.1007/s12665-010-0732-y.
H. Hartley, B.M. Jones, and G.A. Hutchinson: The spontaneous crystallisation of sodium sulfate solutions. J. Chem. Soc. 93, 825 (1908).
S. Genkinger and A. Putnis: Crystallisation of sodium sulfate: Supersaturation and metastable phases. Environ. Geol. 52, 295 (2007).
E. Balboni, R.M. Espinosa-Marzal, E. Doehne, and G.W. Scherer: Can drying and re-wetting of magnesium sulfate salts lead to damage of stone? Env. Earth Sci. (2010), doi: 10.1007/s12665-010-0774-1.
M.C. Malin: Salt weathering on Mars. J. Geophys. Res. 79, 3888 (1974).
O. Coussy and S. Brisard: Prediction of drying shrinkage beyond the pore isodeformation assumption. J. Mech. Mater. Struct. 4, 263 (2009).
Acknowledgments
The authors thank Prof. Chris Hall for helpful advice. The authors also thank the Deutsche Forschungsgemeinschaft, the Getty Conservation Institute, the National Center for Preservation Technology & Training (NCPTT) (Grant MT-2210-09-NC-03), and the United Kingdom Engineering and Physical Sciences Research Council for financial support.
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Espinosa-Marzal, R.M., Hamilton, A., McNall, M. et al. The chemomechanics of crystallization during rewetting of limestone impregnated with sodium sulfate. Journal of Materials Research 26, 1472–1481 (2011). https://doi.org/10.1557/jmr.2011.137
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DOI: https://doi.org/10.1557/jmr.2011.137