Sains Malaysiana 47(3)(2018): 581–587
http://dx.doi.org/10.17576/jsm-2018-4703-19
Sol-gel Synthesis and Optical Properties
of Malayaite Ceramic Colour Pigments
(Sintesis Sol-gel dan Sifat Optik Pigmen Warna
Seramik Malayait)
N. YONGVANICH*, N. WANGWANICH
& N. PHOMWANA
Department of Materials
Science and Engineering, Silpakorn University, Thailand
Received: 30 August
2016/Accepted: 13 October 2017
ABSTRACT
Ceramic colour pigments based on the
malayaite structure was synthesized by sol-gel with an aim to obtain
homogeneous powder systems. The formulation was Ca(Sn1-xCrx)SiO5 where
x = 0, 0.02 and 0.05. Thermogravimetric analysis and infrared spectroscopy
suggested suitable calcination temperatures to be > 1000°C. Formation of
malayaite phase was found to be very difficult; high calcination temperatures
up to 1400°C was required which was typical for this particular phase.
Nevertheless, small amounts of impurities were still present and were found to be
both wollastonite (CaSiO3) and cassiterite (SnO2).
The oxidation state of chromium was found to be mainly 4+. The obtained pigment
particles were in the range of 1-5 micron with a high degree of agglomeration
due to sintering. UV-vis spectra demonstrated broad
absorbance peak in the 550-600 nm range which could be attributed to both Cr(III) and Cr(IV). The colour parameters in the CIELab
system showed a red tone (more positive a* values whereas b* remained
relatively constant) when chromium was doped into the malayaite host.
Preliminary interaction testing with a low-fire glaze displayed an even
improvement in the a* parameter (getting more red
tone). Microscopic studies showed a certain degree of chromium diffusion out of
the pigment powders toward the glaze matrix. These results have demonstrated a
great potential for this refractory colour pigments to be possibly utilized in
other kinds of glazes as well.
Keywords: Ceramics; colour;
malayaite; pigment; sol-gel
ABSTRAK
Pigmen warna
seramik berdasarkan struktur malayait disintesis oleh sol-gel
dengan matlamat untuk mendapatkan sistem serbuk homogen. Rumusannya
ialah Ca(Sn1-xCrx) SiO5
dengan x = 0, 0.02 dan 0.05. Analisis termogravimetri
dan spektroskopi inframerah dicadangkan sesuai untuk pengkalsinan
bagi suhu >1000°C. Pembentukan fasa malayait didapati
sangat sukar; suhu kalsinasi yang tinggi sehingga 1400°C
diperlukan secara tipikal pada fasa ini. Walau
bagaimanapun, sejumlah kecil kekotoran masih ada dan didapati
pada kedua-dua wolastonit (CaSiO3)
dan kasiterit (SnO2). Keadaan
pengoksidaan kromium didapati 4+ terutamanya. Zarah
pigmen yang diperoleh berada dalam lingkungan 1-5 mikron dengan
aglomerasi yang tinggi kerana sinteran. Spektrum sinar
UV menunjukkan
puncak penyerapan luas dalam lingkungan 550-600 nm yang boleh
dikaitkan dengan kedua-dua Cr(III)
dan Cr(IV). Parameter warna dalam sistem
CIELab menunjukkan nada merah (lebih
nilai positif a* sedangkan b* kekal agak berterusan) apabila
kromium terdop ke dalam perumah malayait. Ujian interaksi
awal dengan api kecil memaparkan
peningkatan yang lebih baik dalam parameter a* (mendapatkan
lebih banyak nada merah). Kajian mikroskopik
mendedahkan penyerapan darjah tertentu kromium daripada serbuk
pigmen ke arah matriks glas. Keputusan ini telah menunjukkan
potensi yang besar untuk pigmen warna refraktori ini yang mungkin
digunakan dalam jenis glas lain juga.
Kata
kunci: Malayait; pigmen; sol-gel; seramik; warna
REFERENCES
Biesinger,
M.C., Brown, C., Mycroft, J.R., Davidson, R.D. & McIntyre, N.S. 2004. X-ray photoelectron
spectroscopy studies of chromium compounds. Surface and Interface
Analysis 36: 1550-1563.
Faurel, X., Vanderperre,
A. & Colomban, P. 2003. Pink pigment optimization by resonance Raman
spectroscopy. Journal of Raman Spectroscopy 34: 290-294.
Halefoglua, Y.Z. &
Kusvuran, E. 2010. Preparation of ceramic pigments by sol-gel
and combustion methods. Journal of Ceramic Processing Research 11(1):
92-95.
Harisanov,
V., Pavlov, R.S., Marinova, I.T., Kozhukharov, V. & Carda, J.B. 2003. Influence of
crystallinity on chromatic parameters of enamels coloured with malayaite pink
pigments. Journal of the European Ceramic Society 23: 429-435.
Ibrahim, N.B., Baqiah,
H. & Abdullah, M.H. 2013. High transparency iron doped indium oxide (In2-xFexO3,
x = 0.0, 0.05, 0.25, 0.35 and 0.45) films prepared by the sol-gel method. Sains
Malaysiana 42(7): 961-966.
Kwoka,
M., Ottaviano, L., Passacantando, M., Santucci, S., Czempik, G. & Szuber,
J. 2005. XPS study of the surface chemistry of L-CVD SnO2 thin
films after oxidation. Thin Solid Films 490: 36-42.
Lee,
H.S. & Lee, B.H. 2008a. Colouring effect of malayaite
formation and synthesis sphene-pink pigment. Journal of Korean
Ceramic Society 45(3): 172-178.
Lee,
H.S. & Lee, B.H. 2008b. The development of a chromium
pink glaze coloring. Journal of Ceramic Processing Research 9(3):
286-291.
Lee, H.S. & Lee,
B.H. 2009. Synthesis of sphene (CaSnSiO5)-
pink pigments with CrCl3. Journal of Korean Ceramic
Society 46(4): 405-412.
Lopez-Navarrete,
E. & Ocaña, M. 2002. A simple procedure for the preparation of Cr-doped tin
sphene pigments in the absence of fluxes. Journal of the European Ceramic
Society 22: 353-359.
Lopez-Navarrete,
E., Caballero, A., Orera, V.M., Lazaro, F.J. & Ocana, M. 2003. Oxidation
state and localization of chromium ions in Cr-doped cassiterite and Cr-doped
malayaite. Acta Materialia 51: 2371-2381.
Ou-benmmou, I.,
Ahamdane, H., El idrissi Raghni, M.A., Bensamka, F., Mosset, A., El Idrissi
Moubtasim, M.L. & Jumas, J.C. 2000. Tin sphene micron-sized powders. Journal
of the European Ceramic Society 20: 2159-2163
Piña,
C., Arriola, H. & Nava, N. 2005. Study of malayaite and
malayaite cobalt pigment. Hyperfine Interaction 161: 93-97.
Shannon, R.D. 1976.
Revised effective ionic radii and systematic studies of interatomic distances
in halides and chalcogenides. Acta Crystallographica A32: 751-767.
Zhang, L., Pi, Z., Yang,
C., Tian, X. & Zhang, S. 2010. Synthesis of chromium-doped malayaite
pigments from wastewater containing low chromium(VI). Journal
of the Air and Waste Management Association 60: 1257-1261.
*Corresponding author; email: niti.yongvanich@gmail.com