Ultramarine blue pigment degradation in cementitious materials: a new approach to the phenomenon

G.  Rodríguez de Sensale; S. Chinchón-Payá; V. de Lima; A. Aguado; Ignacio Segura

doi:10.3989/mc.2024.357623

Authors

G. Rodríguez de Sensale Instituto de la Construcción, Universidad de la República - Instituto de Ensayo de Materiales, Universidad de la República https://orcid.org/0000-0003-4017-4163
S. Chinchón-Payá Instituto de Ciencias de la Construcción Eduardo Torroja (IETcc-CSIC) https://orcid.org/0000-0002-2649-7188
V. de Lima Instituto de la Construcción, Universidad de la República https://orcid.org/0009-0002-8651-2527
A. Aguado Departamento de Ingeniería Civil y Ambiental, Universidad Politécnica de Cataluña https://orcid.org/0000-0001-5542-6365
Ignacio Segura Departamento de Ingeniería Civil y Ambiental, Universidad Politécnica de Cataluña https://orcid.org/0000-0001-6519-9899

DOI:

https://doi.org/10.3989/mc.2024.357623

Keywords:

Ultramarine blue pigment, Degradation, Cement, Cement paste

Abstract

The paper analyses the degradation process of commercial ultramarine blue pigments in cementitious materials. For this purpose, two commercial pigments (with and without a protective coating) in different solutions and cement pastes are studied incrementally. The results show that pigment degradation occurs due to an ion exchange phenomenon; during hydration high ion contents are released, calcium and potassium being the most aggressive for the pigment. Calcium distorts the unit cell; between the sodium of the pigment and the potassium in the medium a cation exchange phenomenon takes place. Both processes lead to the diffusion of sulphate and sulphide ions from the pigment to the medium causing loss of colour and the formation of ettringite.

Downloads

Download data is not yet available.

References

Osticioli Y, Mendes NFC, Nevin A, Gil PSC, Becucci M, Castelluci E. 2009. Analysis of natural and artificial ultramarine blue pigments using laser induced breakdown and pulsed Raman spectroscopy, statistical analysis and light microscopy. Spectrochim. Acta Part A. Mol. Biomolec. Spectros. 73(3): 525-531. https://doi.org/10.1016/j.saa.2008.11.028 PMid:19129003

Plesters J. 1966. Identification of materials of paintings: II. Ultramarine blue, natural and artificial. Studies in conservation. 11(2): 76-91. https://doi.org/10.1179/sic.1966.010

Landman AA. 2003. The role sulphur plays in the formation of ultramarine blue, in: University of Pretoria ed., Aspects of solid-state chemistry of fly ash and ultramarine pigments, PhD These, Chapter 4, Pretoria, 65-76.

Arieli D, Vaughan DEW, Golfarb D. 2004. New synthesis and insight into the structure of blue ultramarine pigments. J. Amer. Chem. Soc. 126(18): 5776-5788. https://doi.org/10.1021/ja0320121 PMid:15125670

Miliani C, Daveri A, Brunetto BG, Sgamellotti A. 2008. CO2 entrapment in natural ultra-marine blue. Chem. Phys. Lett. 466(4-6): 148-151. https://doi.org/10.1016/j.cplett.2008.10.038

Cato E, Rossi A, Scherrer N, Ferreira ESB. 2018. An XPS study into sulphur speciation in blue and green ultramarine. J. Cult. Herit. 29: 30-35. https://doi.org/10.1016/j.culher.2017.09.005

Climent-Pascual E, Sáez-Puche R, Gómez-Herrero A, Romero J. 2008. Cluster ordering in synthetic ultramarine pigments. Micropor. Mesopor. Mater. 116 (1-3): 344-351. https://doi.org/10.1016/j.micromeso.2008.04.026

Booth DG, Dann SE, Weller MT. 2003. The effect of the cation composition on the synthesis and properties of ultramarine blue. Dyes Pigmen. 58 (1): 73-82. https://doi.org/10.1016/S0143-7208(03)00037-8

Cato E, Borca C, Huthwelker T, Ferreira ESB. 2016. Aluminium X-ray absorption near-edge spectroscopy analysis of discoloured ultramarine blue in 20th century oil paintings. Microchem. J. 126: 18-24. https://doi.org/10.1016/j.microc.2015.11.021

Plesters J. 1993. Ultramarine blue, natural and artificial, in: ashok roy ed., artists pigments: a handbook of their history and characteristics, vol. 2, National Gallery of Art, Washington, 37-65.

Del Federico E, Newman J, Tyne L, O'Hern C, Isolani L, Jerschow A. 2006. Solid-state NMR studies of ultramarine pigments discoloration. MRS Online Proceedings Library Archive 984, 713. https://doi.org/10.1557/PROC-984-0984-MM07-13

Del Federico E, Shöfberger W, Schelvis J, Kapetanaki S, Tyne L, Jerschow A. 2006. Insight into framework destruction in ultramarine pigments. Inorg. Chem. 45(3): 1270-1276. https://doi.org/10.1021/ic050903z PMid:16441139

De la Rie ER, Michelin A, Ngako M, Del Federico E, Del Grosso C. 2017. Photo-catalytic degradation of binding media of ultramarine blue containing paint layers: A new perspective on the phenomenon of "ultramarine disease" in paintings. Polym. Degrad. Stab. 144: 43-52. https://doi.org/10.1016/j.polymdegradstab.2017.08.002

Cato E, Scherrer N, Ferreira ESB. 2017. Raman mapping of the S3-chromophore in degraded ultramarine blue paints. J. Raman Spectros. 48 (12): 1789-1798. https://doi.org/10.1002/jrs.5256

Gobeltz N, Demortier A, Lelieur JP, Duhayon C. 1998. Encapsulation of the chromophores into the sodalite structure during the synthesis of the blue ultramarine pigment. J. Chemic. Soc. Farad. Transac. 94 (15): 2257-2260. https://doi.org/10.1039/a801526k

Liu QX, Xu ZH, Finch JA, Egerton RA. 1998. A novel two-step silica coating process for engineering magnetic nanocomposites. Chem. Mater. 10 (12): 3936-3940. https://doi.org/10.1021/cm980370a

Li S, Liu M, Sun I. 2011. Preparation of acid-resisting ultramarine blue by novel two-step silica coating process. Industr. Engineer. Chem. Res. 50 (12): 7326-7331. https://doi.org/10.1021/ie200343k

Liu M, Li S, Umereweneza D. 2011. Enhancement of acid resistance for ultramarine blue by silica coatings. Advanc. Mater. Res. 291-294: 163-166. https://doi.org/10.4028/www.scientific.net/AMR.291-294.163

Aranzabe E, Villasante PM, March R, Arriortua MI, Vadillo J, Larrañaga A, Aranzabe A. 2016. Preparation and characterization of NIR reflective pigments based in ultramarine blue. Ener. Build. 126:170-176. https://doi.org/10.1016/j.enbuild.2016.05.011

Kroone B. 1968. The reaction between hydrating Portland cement and ultramarine blue. Chemistry and Industry. London, 287-288.

Posada N, Sanmartín R, Restrepo O. 2003. Coloración de cemento con pigmento azul ultramar. DYNA 70(139):35-45. Retrieved from https://www.redalyc.org/articulo.oa?id=49613905.

Restrepo J, Restrepo O, Tobón O. 2009. Evaluación del desempeño mecánico del cemento blanco coloreado con pigmento azul ultramar. DYNA 76(157):225-231. Retrieved from https://revistas.unal.edu.co/index.php/dyna/article/view/9571/11501

Giraldo C, Tobón JI, Restrepo OJ. 2012. Ultramarine blue-pigment: A non-conventional pozzolan. Constr. Build. Mater. 36: 305-310. https://doi.org/10.1016/j.conbuildmat.2012.04.011

Chinchón-Payá S, Aguado A, Chinchón S. 2012. A comparative investigation of the degradation of pyrite and pyrrhotite under simulated laboratory conditions. Engineer. Geol. 127: 75-80. https://doi.org/10.1016/j.enggeo.2011.12.003

Salvador RP, Cavalaro SHP, Segura I, Figueiredo AD, Pérez J. 2016. Early age hydration of cement pastes with alkaline and alkali-free accelerators for sprayed concrete. Constr. Build. Mater. 111: 386-398. https://doi.org/10.1016/j.conbuildmat.2016.02.101

Teichmann G. 1990. The use of colorimetric methods in the concrete industry. Beton. Fertig.-Tech./Concr. Precast. Plant Technol. 10:58-73.

López A, Guzmán GA, Di Sarli AR. 2016. Colour stability in mortars and concretes. Part 1: Study on architectural mortars, Constr. Build. Mater. 120: 617-622. https://doi.org/10.1016/j.conbuildmat.2016.05.133

López A, Di Sarli AR. 2020. Measurements number in cementitious mixtures to define the colour and its homogeneity. Constr. Build. Mater. 238: 117636. https://doi.org/10.1016/j.conbuildmat.2019.117636

López A, Tobes JM, Giaccio G, Zerbino R. 2009. Advantages of mortar-based design for coloured self-compacting concrete. Cem. Concr. Compos. 31(10):754-761. https://doi.org/10.1016/j.cemconcomp.2009.07.005

Afremow LC, Vanderberg JT. 1966. High resolution spectra of inorganic pigments and extenders in the mid-infrared region from 1500 cm-1 to 200 cm-1. J. Paint. Technol. 38(495):169-202.

Sancho JP, Restrepo OJ, García P, Ayala J, Fernández B, Verdeja LF. 2008. Ultramarine blue from Asturian "hard" kaolins. Appl. Clay Sci. 41 (3-4): 133-142. https://doi.org/10.1016/j.clay.2007.10.005

Landman A, de Waal D. 2004. Fly ash as a potential starting reagent for the synthesis of ultramarine blue. Mater. Res. Bull. 39 (4-5): 655-667. https://doi.org/10.1016/j.materresbull.2003.12.002

Jakobsson S. 2002. Determination of Si/Al ratios in semicrystalline aluminosilicates by FT-IR spectroscopy. J. Appl. Spectros. 56 (6): 797-799. https://doi.org/10.1366/000370202760077559