Co-Doped Hardystonite, Ca2(Zn,Co)Si2O7, a New Blue Ceramic Pigment
Raising cost, limited reserves, and toxicity make a pressing need to reduce the consumption of cobalt in the ceramic industry, trying to improve efficiency and sustainability of pigments. A novel blue colorant, based on the melilite structure, has been developed by searching for a ceramic pigment st...
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| Published in | Journal of the American Ceramic Society Vol. 94; no. 4; pp. 1025 - 1030 |
|---|---|
| Main Authors | , , , |
| Format | Journal Article |
| Language | English |
| Published |
Malden, USA
Blackwell Publishing Inc
2011
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| Subjects | |
| Online Access | Get full text |
| ISSN | 0002-7820 1551-2916 |
| DOI | 10.1111/j.1551-2916.2010.04203.x |
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| Abstract | Raising cost, limited reserves, and toxicity make a pressing need to reduce the consumption of cobalt in the ceramic industry, trying to improve efficiency and sustainability of pigments. A novel blue colorant, based on the melilite structure, has been developed by searching for a ceramic pigment stable in very aggressive media, like the calcium‐ and zinc‐rich glazes used in porous tiles (stoneware and monoporosa). Hardystonite was selected as a typical crystalline compound found in these coatings, which has just one fourfold crystallographic site where Co2+ ions can be accommodated, thus ensuring its unrivalled blue color. Five samples (Ca2Zn1−xCoxSi2O7 with x=0.05, 0.1, 0.2, 0.3, and 0.4) were prepared by a solid‐state synthesis in industrial‐like conditions (∼95% yield) and characterized by XRD, DRS, SEM–EDS, and technological testing. Increasing cobalt doping gives rise to a gradual expansion of the hardystonite unit cell, unexpected on the basis of Zn2+ and Co2+ ionic radii, attributed to a change of the covalent character of M–O bonding. Optical spectra are dominated by the strong absorption bands of Co2+ in tetrahedral coordination (crystal field strength Dq=421 cm−1, Racah B parameter=793 cm−1). The best compromise between cobalt concentration and optical response was found to be around x=0.3. The hardystonite pigment bestows a deep blue color on glazes and glassy coatings, withstanding aggressive media rich in CaO and ZnO better than industrial blue pigments (cobalt aluminate, spinel) with similar color efficiency than industrial blue dyes (cobalt silicate, olivine) but with the advantage to avoid specking defects of highly staining colorants. |
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| AbstractList | A novel blue colourant, based on the melilite structure, has been developed by searching for a ceramic pigment stable in very aggressive media, like the calcium- and zinc-rich glazes used in porous tiles. Hardystonite was selected as a typical crystalline compound found in these coatings, which has just one fourfold crystallographic site where Co2+ ions can be accommodated, thus ensuring its unrivalled blue colour. Five samples (Ca2Zn1-xCoxSi2O7 with x = 0.05, 0.1, 0.2, 0.3, and 0.4) were prepared by solid-state synthesis in industrial-like conditions (about 95% yield) and characterised by XRD, DRS, SEM-EDS, and technological testing. Increasing the cobalt doping gradually expanded the hardystonite unit cell, unexpected on the basis of Zn2+ and Co2+ ionic radii, attributed to a change in the covalent character of M-O bonding. Optical spectra were dominated by strong absorption bands of Co2+ in tetrahedral coordination. The best compromise between cobalt concentration and optical response was around x = 0.3. The hardystonite pigment bestowed a deep blue colour on the glazes and glassy coatings, withstanding aggressive media rich in CaO and ZnO better than industrial blue pigments with similar colour efficiency than industrial blue dyes but with the advantage of avoiding specking defects. Raising cost, limited reserves, and toxicity make a pressing need to reduce the consumption of cobalt in the ceramic industry, trying to improve efficiency and sustainability of pigments. A novel blue colorant, based on the melilite structure, has been developed by searching for a ceramic pigment stable in very aggressive media, like the calcium‐ and zinc‐rich glazes used in porous tiles (stoneware and monoporosa). Hardystonite was selected as a typical crystalline compound found in these coatings, which has just one fourfold crystallographic site where Co2+ ions can be accommodated, thus ensuring its unrivalled blue color. Five samples (Ca2Zn1−xCoxSi2O7 with x=0.05, 0.1, 0.2, 0.3, and 0.4) were prepared by a solid‐state synthesis in industrial‐like conditions (∼95% yield) and characterized by XRD, DRS, SEM–EDS, and technological testing. Increasing cobalt doping gives rise to a gradual expansion of the hardystonite unit cell, unexpected on the basis of Zn2+ and Co2+ ionic radii, attributed to a change of the covalent character of M–O bonding. Optical spectra are dominated by the strong absorption bands of Co2+ in tetrahedral coordination (crystal field strength Dq=421 cm−1, Racah B parameter=793 cm−1). The best compromise between cobalt concentration and optical response was found to be around x=0.3. The hardystonite pigment bestows a deep blue color on glazes and glassy coatings, withstanding aggressive media rich in CaO and ZnO better than industrial blue pigments (cobalt aluminate, spinel) with similar color efficiency than industrial blue dyes (cobalt silicate, olivine) but with the advantage to avoid specking defects of highly staining colorants. |
| Author | Zanelli, Chiara Ardit, Matteo Cruciani, Giuseppe Dondi, Michele |
| Author_xml | – sequence: 1 givenname: Michele surname: Dondi fullname: Dondi, Michele organization: Institute of Science and Technology for Ceramics (ISTEC-CNR), Via Granarolo 64, 48018 Faenza, Italy – sequence: 2 givenname: Chiara surname: Zanelli fullname: Zanelli, Chiara organization: Institute of Science and Technology for Ceramics (ISTEC-CNR), Via Granarolo 64, 48018 Faenza, Italy – sequence: 3 givenname: Matteo surname: Ardit fullname: Ardit, Matteo email: harditster@gmail.com organization: Department of Earth Sciences, University of Ferrara, Via Saragat 1, 44100 Ferrara, Italy – sequence: 4 givenname: Giuseppe surname: Cruciani fullname: Cruciani, Giuseppe organization: Department of Earth Sciences, University of Ferrara, Via Saragat 1, 44100 Ferrara, Italy |
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Monros, "Cobalt Minimisation in Willemite (CoxZn2−xSiO4) Ceramic Pigments," Green Chem., 2, 93-100 (2000). Y. Hao and Y. H. Wang, "Synthesis and Photoluminescence of New Phosphors M(Mg, Zn)Si2O7: Mn2+ (M=Ca, Sr, Ba)," Mater. Res. Bull., 42, 2219-23 (2007). M. Llusar, A. Fores, J. A. Badenés, J. Calbo, M. A. Tena, and G. Monros, "Colour Analysis of Some Cobalt-Based Blue Pigments," J. Eur. Ceram. Soc., 21, 1121-30 (2001). L. Bindi, M. Czank, F. Röthlisberger, and P. Bonazzi, "Hardystonite from Franklin Furnace: A Natural Modulated Melilite," Am. Mineral., 86, 747-51 (2001). H. Kamioka, T. Yamaguchi, M. Hirano, T. Kamiya, and H. Hosono, "Structural and Photo-Induced Properties of Eu2+-Doped Ca2ZnSi2O7: A Red Phosphor for White Light Generation by Blue Ray Excitation," J. Lumin., 122, 339-41 (2007). Italian Ceramic Society. Colour, Pigments and Colouring in Ceramics. SALA, Modena, 2003. K. Hagiya, M. Ohmasa, and K. Iishi, "The Modulated Structure of Synthetic Co-åkermanite, Ca2CoSi2O7," Acta Cryst., B49, 172-9 (1993). M. Dondi, F. Matteucci, G. Baldi, A. Barzanti, G. Cruciani, I. Zama, and C. L. Bianchi, "Gray-Blue Al2O3-MoOx Ceramic Pigments: Crystal Structure, Colouring Mechanism and Technological Performance," Dyes Pigm., 76, 179-86 (2008). K. M. Knowles and F. S. H. B. Freeman, "Microscopy and Microanalysis of Crystalline Glazes," J. Microscopy, 215, 257-70 (2004). R. A. Eppler, "Selecting Ceramic Pigments," Am. Ceram. Soc. Bull., 66, 1600-4 (1987). D. Jonynaitë, D. Jasaitis, J. Senvaitienë, and A. Kareiva, "Synthesis of CoNH4PO4 Pigment by Co-Precipitation Method," Chemija, 19, 23-6 (2008). Dry Color Manufacturer's Association. Classification and Chemical Description of the Mixed Metal Oxide Inorganic Coloured Pigments-Metal Oxides and Ceramics Colors Subcommittee, 2nd edition, DCMA, Washington, DC, 1982. G. Costa, M. J. Ribeiro, J. A. Labrincha, M. Dondi, F. Matteucci, and G. 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| References_xml | – reference: G. Monari and T. Manfredini, "Coloring Effects of Synthetic Inorganic Cobalt Pigments in Fast-Fired Porcelainized Tiles," Ceram. Eng. Sci. Proc., 17, 167-72 (1996). – reference: M. Dondi, F. Matteucci, G. Baldi, A. Barzanti, G. Cruciani, I. Zama, and C. L. Bianchi, "Gray-Blue Al2O3-MoOx Ceramic Pigments: Crystal Structure, Colouring Mechanism and Technological Performance," Dyes Pigm., 76, 179-86 (2008). – reference: A. Leite, G. Costa, W. Hajjaji, M. J. Ribeiro, M. P. Seabra, and J. A. Labrincha, "Blue Cobalt Doped-Hibonite Pigments Prepared from Industrial Sludges: Formulation and Characterization," Dyes Pigm., 81, 211-7 (2009). – reference: A. Fores, M. Llusar, J. A. Badenés, J. Calbo, M. A. Tena, and G. Monros, "Alternative Turquoise Blue Pigment for Glazes," Am. Ceram. Soc. Bull., 80, 47-52 (2001). – reference: S. Marfunin, Physics of Minerals and Inorganic Materials. Springer, Berlin, 1979. – reference: Dry Color Manufacturer's Association. Classification and Chemical Description of the Mixed Metal Oxide Inorganic Coloured Pigments-Metal Oxides and Ceramics Colors Subcommittee, 2nd edition, DCMA, Washington, DC, 1982. – reference: A. S. Bystrikov, V. V. Gorbachev, D. L. Orlov, V. N. Petrakov, and I. V. Shishkin, "Decorative Materials Based on Cobalt-Containing Akermanite," Glass Ceram., 39, 128-30 (1982). – reference: F. J. Torres, U. R. Rodríguez-Mendoza, V. Lavín, E. Ruiz de Sola, and J. Alarcón, "Evolution of the Structural and Optical Properties from Cobalt Cordierite Glass to Glass-Ceramic Based on Spinel Crystalline Phase Materials," J. Non-Cryst. Solids, 353, 4093-101 (2007). – reference: D. Gardini, M. Dondi, A. L. Costa, F. Matteucci, M. Blosi, C. Galassi, G. Baldi, and E. Cinotti, "Nano-Sized Ceramic Inks for Drop-on-Demand Ink-Jet Printing in Quadrichromy," J. Nanosci. Nanotechnol., 8, 1979-88 (2008). – reference: Italian Ceramic Society. Colour, Pigments and Colouring in Ceramics. SALA, Modena, 2003. – reference: S. Meseguer, M. A. Tena, C. Gargori, R. Galindo, J. A. Badenés, M. Llusar, and G. Monrós, "Development of Blue Ceramic Dyes from Cobalt Phosphates," Ceram. Int., 34, 1431-8 (2008). – reference: R. G. Burns, Mineralogical Applications of Crystal Field Theory, 2nd edition, Cambridge University Press, Cambridge, 1993. – reference: G. Costa, M. J. Ribeiro, J. A. Labrincha, M. Dondi, F. Matteucci, and G. Cruciani, "A New Turquoise Blue Ceramic Pigment Based on Ni-Doped Hibonite (CaAl12O19)," J. Eur. Ceram. Soc., 29, 2671-8 (2009). – reference: D. Jonynaitë, D. Jasaitis, J. Senvaitienë, and A. Kareiva, "Synthesis of CoNH4PO4 Pigment by Co-Precipitation Method," Chemija, 19, 23-6 (2008). – reference: A. C. Larson and R. B. Von Dreele, GSAS, General Structure Analysis System, pp. 86-748. Los Alamos National Laboratory, Los Alamos, NM, 1988. – reference: L. Bindi, M. Czank, F. Röthlisberger, and P. Bonazzi, "Hardystonite from Franklin Furnace: A Natural Modulated Melilite," Am. Mineral., 86, 747-51 (2001). – reference: C. Siligardi, C. Mugoni, D. Corradini, D. Venturelli, M. Montorsi, and A. P. Novaes de Oliveira, "Nova frita pertencente ao sistema CaO-ZnO-SiO2 para aplicações cerâmicas," Cerâmica Ind., 14, 20-7 (2009). – reference: M. Gaudon, A. Apheceixborde, M. Menetrier, A. Le Nestour, and A. Demourgues, "Synthesis Temperature Effect on the Structural Features and Optical Absorption of Zn1−xCoxAl2O4 Oxides," Inorg. Chem., 48, 9085-91 (2009). – reference: A. Escardino, A. Mestre, C. Feliu, P. Jodar, and L. Díaz, "Stability of (Cr)CaO.SnO2.SiO2 Pink Pigment in Ceramic Frits," Br. Ceram. Trans., 101, 213-20 (2002). – reference: P. M. T. Cavalcante, M. Dondi, G. Guarini, M. Raimondo, and G. Baldi, "Colour Performance of Ceramic Nano-Pigments," Dyes Pigm., 80, 226-32 (2009). – reference: K. Hagiya, M. Ohmasa, and K. Iishi, "The Modulated Structure of Synthetic Co-åkermanite, Ca2CoSi2O7," Acta Cryst., B49, 172-9 (1993). – reference: K. M. Knowles and F. S. H. B. Freeman, "Microscopy and Microanalysis of Crystalline Glazes," J. Microscopy, 215, 257-70 (2004). – reference: M. Dondi, F. Matteucci, I. Zama, and G. Cruciani, "High-Performance Yellow Ceramic Pigments Zr(Ti1−x−ySnx−yVyMy)O4 (M=Al, In, Y): Crystal Structure, Colouring Mechanism and Technological Properties," Mater. Res. Bull., 42, 64-79 (2007). – reference: E. Ozel, H. Yurdakul, S. Turan, M. Ardit, G. Cruciani, and M. Dondi, "Co-Doped Willemite Ceramic Pigments: Technological Behaviour, Crystal Structure and Optical Properties," J. Eur. Ceram. Soc., 30, 3319-29 (2010). – reference: S. Louisnathan, "Refinement of the Crystal Structure of Hardystonite, Ca2ZnSi2O7," Z. Kristallogr., 130, 427-37 (1969). – reference: H. Kamioka, T. Yamaguchi, M. Hirano, T. Kamiya, and H. 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| Snippet | Raising cost, limited reserves, and toxicity make a pressing need to reduce the consumption of cobalt in the ceramic industry, trying to improve efficiency and... A novel blue colourant, based on the melilite structure, has been developed by searching for a ceramic pigment stable in very aggressive media, like the... |
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| SubjectTerms | Ceramics Coatings Cobalt Color Colour Glazes Media Pigments |
| Title | Co-Doped Hardystonite, Ca2(Zn,Co)Si2O7, a New Blue Ceramic Pigment |
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