Spectrometric Characterization of Moroccan Architectural Glazed Tiles

Spectrometric Characterization of Moroccan Architectural Glazed Tiles

Mohamed EL AMRAOUI, Mustapha HADDAD, Lahcen BEJJIT, Saadia AIT LYAZIDI, Abdelouahed BEN-NCER

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Abstract The present work relates to a multi-analytic characterization of glazed tiles consisting of green monochrome glazed ceramics used in Moroccan architecture to protect ceilings, walls and roofs from rainwater. These tiles originate from five sites and date back to different historical periods: Bou-Inania Madrasa in Meknes (14th century), Prison of Qara in Meknes (18th century), Dar El-Beida Palace in Meknes (18th century) and Al-Hibous Cemetery of Mdaghra in Errachidia (19th century). Different analysis techniques were used in view to go back to the ancient technological processes adopted (materials, coloring pigments, firing temperatures, etc..). Optical absorption spectrometry revealed two different types of chromogenic ions in green glazes, chromium Cr3+ in the case of the tiles from Dar El-Beida Palace and Prison of Qara, and copper Cu2+ in the case of the tiles from Bou-Inania Madrasa and Al-Hibous Cemetery. Raman microspectroscopy identified different coloring phases with two types of green glazes, escolaite (Cr2O3) in the case of the glazes of the Prison of Qara and copper phthalocyanine mixed with a chromium-based pigment in the case of the glazes of the Dar El-Beida Palace. However, the origin of the green color in the glazes from Bou-Inania Medersa in Meknes and Al-Hibous cemetery of Errachidia may be due to the dissolution of copper in the vitreous glazes. X-ray diffraction, supported by Raman microspectrometry, revealed the mineralogical compositions of the terracotta tiles. Quartz and calcite are the main phases, while hematite and “high temperature” phases (anorthite, gehlenite and diopside) appear as minority ones. These identified phases permit to estimate the firing temperature of the tiles at around 950 °C in an oxidizing atmosphere. The chromatic coordinates of all glazes, represented in the Lab CIE color space, made it possible to discriminate objectively all green colors. The present investigation of glazes from different historical sites allowed the exploration of the coloring materials, revealed differences in the adopted technological protocols and permitted the establishment of a color reference database to follow glazes degradation and to help while replacing missing or degraded tile pieces.

Keywords
Glazed Tiles, Spectrometric Characterization, Moroccan Historical Sites and Monuments, Colouring Phases, Crystalline Phases

Published online 3/15/2024, 12 pages
Copyright © 2024 by the author(s)
Published under license by Materials Research Forum LLC., Millersville PA, USA

Citation: Mohamed EL AMRAOUI, Mustapha HADDAD, Lahcen BEJJIT, Saadia AIT LYAZIDI, Abdelouahed BEN-NCER, Spectrometric Characterization of Moroccan Architectural Glazed Tiles, Materials Research Proceedings, Vol. 40, pp 167-178, 2024

DOI: https://doi.org/10.21741/9781644903117-18

The article was published as article 18 of the book Mediterranean Architectural Heritage

Content from this work may be used under the terms of the Creative Commons Attribution 3.0 license. Any further distribution of this work must maintain attribution to the author(s) and the title of the work, journal citation and DOI.

References
[1] M. El Amraoui, A. Azzou, M. Haddad, L. Bejjit, S. Aït Lyazidi, Y. El Amraoui, “Zelliges of Dar-El Beïda Palace (18th-century) in Meknes (Morocco): Optical Absorption and Raman Spectrometry study” Spectroscopy Letters, Volume 40, issue 5, (2007), pp. 777-783. https://doi.org/10.1080/00387010701521892
[2] A. Zucchiatti, A. Azzou, M. El Amraoui, M. Haddad, L. Bejjit, S. Aït Lyazidi, “PIXE analysis of Moroccan architectural glazed ceramics (XIV-XVIII centuries)”, International Journal of PIXE, Volume: 19, Issues: 3-4, (2009), pp. 175-187. https://doi.org/10.1142/S0129083509001862
[3] M El Amraoui., A Azzou., M Haddad., L Bejjit., Y El Amraoui., S Aït Lyazidi. “Elemental and crystalline analysis of architectural ceramics of Dar-El Beïda Palace (18th century) in Meknes (Morocco)” Minbar Al Jamiaa (7); Actes de la 1ère Rencontre Internationale sur le Patrimoine Architectural Méditerranéen (RIPAM 1) Edition de l’Université Moulay Ismaïl, (2007), p.188-194
[4] M. El Amraoui, A. Azzou, A. Zucchiatti, M. Haddad, L. Bejjit, “Analyse par PIXE de Zelliges marocains du XIVème siècle”, Actes de la 2ème Rencontre Internationale sur le Patrimoine Architectural Méditerraneen (RIPAM 2) édité par M. Haddad et M. Ibnoussina, Minbar Al Jamiaa, édition de l’Université Moulay Ismaïl, (20), (2010), pp. 212-221.
[5] A. Azzou, M Haddad., S Ait Lyazidi., L Bejjit., A Ben Amara., M. Schvoerer, 2007, “ Micro-spectrométrie Raman appliquée à la céramique ancienne de Fès (Maroc, 14ème siècle)”, MINBAR AL JAMIAA n°7, Actes de la RIPAM1-(2005), Meknes, Maroc.
[6] M.El Amraoui, 2011,“ Etudes par des techniques physiques de céramiques glaçurée de l’architecture marocaine (14ème – 20ème s), de mosaïques romaines de Volubilis et de matériels archéologiques provenant de fouille“, Thèse de Doctorat, Faculté des sciences, Université Moulay Ismaïl, Meknès, Maroc, 219 p.
[7] A. Azzou, 2005, “ céramiques glaçurée architecturales marocaines: caractéristiques physico-chimiques et techniques de fabrication des zelliges anciennes (14ème et 17ème siècle) ”, Thèse de Doctorat, Faculté des sciences, Université Moulay Ismaïl, Meknès, Maroc, 150 p.
[8] RRUFF project database. http://rruff.info
[9] T Cavaleri., A Giovagnoli. et M. Nervo, 2013, “ Pigments and mixtures identification by Visible Reflectance Spectroscopy ”, Procedia Chemistry, 8 : p.45–54. https://doi.org/10.1016/j.proche.2013.03.007
[10] A. Tournié, Analyse Raman sur site de verres et vitraux anciens : modélisation, procédure, lixiviation et caractérisation, Thèse de Doctorat, Universite Pierre et Marie Curie, 163p.
[11], Ph. Colomban, 2003, “Polymerisation Degree and Raman Identification of Ancient Glasses used for Jewellery, Ceramics Enamels and Mosaics”, Non-Crystalline Solids, 323 :p. 180-187. https://doi.org/10.1016/S0022-3093(03)00303-X
[12] Ph. Colomban, V Milande. et L Le Bihan., 2004, “ On site Raman analysis of Iznik pottery Glazes and pigments ”, J. Raman spectroscopy , 35 :p.527-535. https://doi.org/10.1002/jrs.1163
[13] Ph. Colomban, G. Sagon, A Louhichi., H Binous. N Ayed., 2001 “ Identification par Microscopie Raman des tessons et pigments de glaçures de céramiques de l’Ifriqiya (Dougga, XI-XVIIIèmes siècles)” Revue d’Archéométrie, 25 p.101-112. https://doi.org/10.3406/arsci.2001.1005
[14] Ph Colomban., F. Treppoz, 2001, “Identification and differentiation of ancient and modern European porcelains by Raman macro- and micro-spectroscopy”, Raman Spectroscopy, 32, 93–102. https://doi.org/10.1002/jrs.678
[15] L.F. Vieira Ferreira, R. Varela Gomes, M.F.C. Pereira, L.F. Santos et Ferreira Machado I., 2016, “Islamic ceramics in Portugal found at Silves Castle (8th to 13th c.): An archaeometric characterization”, Archaeological Science: Reports, 8 : p.434–443. https://doi.org/10.1016/j.jasrep.2016.06.051
[16] L.F. Vieira Ferreira, E. De Sousa, M.F.C Pereira., Guerra S. et Ferreira Machado I., 2019, “An archaeometric study of the Phoenician ceramics found at the São Jorge Castle’s hill in Lisbon”, Ceramics International. https://doi.org/10.1016/j.ceramint.2019.11.267
[17] Ph. Colomban, B. Kırmızı, B Zhao., J.B Clais., Yang Y. et Droguet V., 2020, “ Non-Invasive On-Site Raman Study of Pigments and Glassy Matrix of 17th–18th Century Painted Enamelled Chinese Metal Wares: Comparison with French Enamelling Technology”,. Coatings 2020, 10, 471. https://doi.org/10.3390/coatings10050471
[18] S.S Pawełkowicz., D Rohanová. et P Svora., 2017, “ Gothic green glazed tile from Malbork Castle: multi-analytical study”, Heritage science, 5:27. https://doi.org/10.1186/s40494-017-0141-6
[19] M.C Caggiani., A Cosentino. et A. Mangone, 2016, “Pigments Checker version 3.0, a handy set for conservation scientists: A free online Raman spectra database”, Microchemical Journal, 129:p.123–132. https://doi.org/10.1016/j.microc.2016.06.020
[20] T. Aguayo, E. Clavijo, A. villagrán , F Espinosa., F. E. sAgüés et Campos-Allette M., 2010, “Raman vibrational study of pigments with patrimonial interest for the chilean cultural heritage”, J. Chil. Chem, 55, Nº 3. https://doi.org/10.4067/S0717-97072010000300016
[21] A. Coccato, D Bersani., A. Coudray, J Sanyova., L. Moens, Vandenabeele P., 2016, ‘Raman spectroscopy of green minerals and reaction products with an application in Cultural Heritage research’ J. Raman spectroscopy. https://doi.org/10.1002/jrs.4956
[22] A. Zoppi, C Lofrumento., E.M Castellucci., M.G Migliorini., 2002, “ Micro-Raman technique for phase analysis on archaeological ceramics”, J. Raman spectroscopy, p.16–21.
[23] H. AZZOUZ, R. ALOUANI and S. TLIG “Mineralogical characterization of ceramic tiles prepared by a mixture of Cretaceous and Mio-Pliocene clays from Tunisia: factory and laboratory products” Journal of the Ceramic Society of Japan 119 [2] 93-100 2011. https://doi.org/10.2109/jcersj2.119.93
[24] G. Raja Annamalai1, R. Ravisankar, A. Chandrasekaran “Analytical investigation of archaeological pottery fragments excavated from Porunthal, Tamil Nadu, India,” Cerâmica 66 (2020) 347-353. https://doi.org/10.1590/0366-69132020663792811
[25] M. Sendova, V. Zhelyaskov, M. Scalera, M. Ramsey, J. Raman Spectrosc. 36 (2005) 829. https://doi.org/10.1002/jrs.1371