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Thermal Expansion of New Arsenate Minerals, Bradaczekite, Nacu4(Aso4)3, and Urusovite, Cu(Asalo5) S

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Thermal Expansion of New Arsenate Minerals, Bradaczekite, Nacu4(Aso4)3, and Urusovite, Cu(Asalo5) S ISSN 1075-7015, Geology of Ore Deposits, 2009, Vol. 51, No. 8, pp. 827–832. © Pleiades Publishing, Ltd., 2009. Original Russian Text © S.K. Filatov, D.S. Rybin, S.V. Krivovichev, L.P. Vergasova, 2009, published in Zapiski RMO (Proceedings of the Russian Mineralogical Society), 2009, Pt. CXXXVII, No. 1, pp. 136–143. MINERALOGICAL CRYSTALLOGRAPHY Thermal Expansion of New Arsenate Minerals, Bradaczekite, NaCu4(AsO4)3, and Urusovite, Cu(AsAlO5) S. K. Filatova, D. S. Rybina, S. V. Krivovicheva, and L. P. Vergasovab a Faculty of Geology, St. Petersburg State University, Universitetskaya nab. 7/9, St. Petersburg, 199034 Russia b Institute of Volcanology, Far East Division, Russian Academy of Sciences, Boulevard Piipa, 9, Petropavlovsk-Kamchatsky, 683006 Russia Received December 19, 2007 Abstract—Thermal behavior of two new exhalation copper-bearing minerals, bradaczekite and urusovite, from the Great Tolbachik Fissure Eruption (1975–1976, Kamchatka Peninsula, Russia) has been studied by X-ray thermal analysis within the range 20–700°C in air. The following major values of the thermal expansion tensor α α α α α × –6° –1 μ α ° have been calculated for urusovite: 11 = 10, 22 = b = 7, 33 = 4, V = 21 10 C , = c^ 33 = 49 and α α α × –6° –1 μ α ° bradaczekite: 11aver = 23, 22 = 8, 33aver = 6 10 C , (c^ 33) = 73 . The sharp anisotropy of thermal deformations of these minerals, absences of phase transitions, and stability of the minerals in the selected tem- perature range corresponding to conditions of their formation and alteration during the posteruption period of the volcanic activity are established. DOI: 10.1134/S1075701509080169 INTRODUCTION established that there is a synthetic analogue, NaCu4(AsO4)3, synthesized by Pertlik (1987) under The Great Tolbachik Fissure Eruption (GTFE 1975– hydrothermal conditions. The mineral was named in 1976, Kamchatka Peninsula, Russia) is among the six most honor of Hans Bradazcek, a professor of Free Berlin famous fissure eruptions in human history. In addition, it is one of the most studied eruptions (The Great …, 1984). In University (Filatov et al., 2001). the 30 years since the eruption, posteruption mineral for- Urusovite, Cu(AlAsO5). The mineral is light green, mation has been regularly monitored at the newly formed with adamantine luster; streak is white; cleavage is per- Tolbachik volcanoes. For this time, 30 new minerals have fect parallel to (001). It occurs as clusters of plates been described, among which are a number of arsenates: extending parallel to [001] and intergrown along elon- lammerite, Cu3[(P,As)O4]2; alarsite, AlAsO4; coparsite, gation. The temperature at the sampling locality was Cu4O2[(As,V)O4]Cl, johillerite, Na(Mg,Zn)3Cu(AsO4)3; 400°C. The microhardness VHN is 378 kg/mm2; the urusovite, Cu[AlAsO5]; bradaczekite, NaCu4(AsO4)3; and Mohs hardness is 5. Urusovite is pleochroic in light filatovite, K[(Al,Zn)2(As,Si)2O8]. Except for lammerite and johillerite, the listed mineral species are new. green tints. It was named in honor of Academician V.S. Urusov (Vergasova et al., 2002). Bradaczekite and urusovite examined in this study were found, among products of volcanic exhalations at The crystallochemical and mineralogical character- the second cinder cone of the North break of the GTFE, istics of bradaczekite and urusovite are given in the to be intimately associated with hematite, tenorite, table. orthoclase, johillerite Na(Mg,Zn)3Cu(AsO4)3, pono- marevite K Cu OCl , piypite K Cu O (SO ) MeCl, It can be concluded that bradaczekite and urusovite 4 4 10 4 4 2 4 4 as exhalative minerals are formed at high temperatures sylvite, dolerophanite Cu2OSO4, and euchlorine KNaCu O(SO ) . and occur at high temperatures and atmospheric pres- 3 4 3 sures on cooling volcanoes for a certain time after for- Bradaczekite, NaCu4(AsO4)3. The mineral is dark mation. Therefore, the aim of this article is to study the blue, with adamantine luster; streak ranges from pale thermal behavior of these minerals by X-ray thermal sky blue to white; cleavage is not observed. Bradacze- analysis under conditions close to natural. The occur- kite occurs as clusters of dark blue plates. The mineral rence of such toxic elements as arsenic in the studied is stable in air and almost insoluble in water and alco- minerals attaches special importance to this work. The hol. The calculated density is 4.77(1) g/cm3. Lumines- cence was not displayed in short- or longwave UV probable release of As from the crystal structure of light. Shortly after discovery of the mineral, it was these minerals and its migration in the biosphere is a subject of doubtless concern. Rybin et al. (2007) and Corresponding author: S.K. Filatov. E-mail: filatov@crystal- Filatov et al. (2007) reported the preliminary results of spb.com this study. 827 828 FILATOV et al. α × –6 × –9 × Crystallochemical and mineralogical characteristics of bradacze- follows: a = 8.4 10 + 16.4 10 T (average ° α α × kite and urusovite value in the range 20–700 C; a average = 14.0), b = 8.0 –6 α × –6 × –9 × α 10 , c = 13.9 10 + 21.6 10 T ( c aver = 21.2), Parameter Bradaczekite Urusovite –6 –1 αβ = 6.8 × 10 °C . Chemical formula NaCu4(AsO4)3 Cu(AsAlO5) Comparison of the thermal expansion of bradacze- Symmetry, space Monoclinic, C2/c Monoclinic, P21/c kite along atomic rows make it possible to distinguish group axis c as the direction of the greatest expansion (aver- α × –6° –1 a (Å) 12.053(2) 7.314(2) age value c = 21.5 10 C ), whereas the expansion along axes a and b is 1.5 and 2.5 times less, respec- b (Å) 12.432(2) 10.223(3) tively. c (Å) 7.2529(13) 5.576(2) The major values of the thermal expansion tensor of β (deg) 117.793 99.79 the mineral reveal a much greater anisotropy of deforma- 3 α × α V (Å ) 961.5(3) 410.9(2) tions: 11 = 16 + 0.02 T (average value 11 average = 23), α = 8, α = –1 + 0.02 × T (α = 6) (10–6 °C–1), Calculated density, 4.77 3.93 μ22 α 33 ° 33 average D , g/cm3 (c ^ 33) = 73 . x α Mohs hardness – 5 The volume expansion of the structure V = 23 + × α × –6 ° –1 0.038 T ( V average = 36 10 C ) is estimated as that Color Dark blue Light green expected for arsenate compounds. Origin Volcanic exhala- Volcanic exhala- The cause of the anisotropic thermal expansion of tion tion bradaczekite can be established from comparison of the α values with the crystal structure of the mineral. Bra- daczekite belongs to the alluaudite, Na[MnFe2(PO4)3], EXPERIMENTAL structural type. In the structure, there are three indepen- The X-ray diffraction patterns of polycrystals were dent Cu2+ atoms. The Cu(1) atom is square-coordinated obtained in air using a DRON-3 diffractometer with a mean bond length of Cu2+–O = 1.91 Å. Cu(2) equipped with a KRV-1100 high-temperature device, and Cu(3) atoms (Fig. 2) exhibit distorted tetrahedral using Cukα radiation, Ni β-filter, and tape recording of coordination due to the Jahn–Teller effect. Two sym- reflections. The temperature range is 20–700°C; tem- metrically independent As atoms are tetrahedrally coor- perature step is 40°C. dinated with average As–O bond lengths of 1.69 Å and The dimensions of monoclinic unit cell were deter- 1.70 Å for As(1) and As(2), respectively. The structure mined by the least squares procedure using the Unit is based on a sheet of octahedrons [Cu(2)O6] and Cell program and approximated by equations not [Cu(3)O6] combined with tetrahedrons [As(2)O4] (Fig. higher than of the second order. The thermal expansion 2a). Edge-sharing octahedrons make up zigzag chains, coefficients were calculated with the DTC program; which form a sheet via [As(2)O4] Tetrahedrons. The sheets are linked to a framework via [As(1)O4] tetrahe- patterns were drawn according to the DTP program + (Belousov and Filatov, 2007). drons and [Cu(1)O4] squares. Na cations occupy cages in the framework (Krivovichev et al., 2001). In Fig. 2b, the pattern of coefficients of the thermal RESULTS AND DISCUSSION expansion of bradaczekite is comparable with the crys- No phase transitions were detected for either min- tal structure of this mineral. Four short equatorial bonds 〈 2+ 〉 eral in the temperature range of 20 to 700°C. The Cu –Oeq = 1.98 (solid lines) and two long apical 〈 2+ 〉 selected range covers typical temperatures of formation bonds Cu –Oap = 2.49 Å (dashed lines) are distin- and transformation of exhalative minerals at volcanoes. guished for each Cu(2) and Cu(3) octahedrons. It is Heating simulation is appropriate to the results of seen that the longest (and weakest) Cu–O bonds 30-year-regime observations, when local temperature (dashed lines in Fig. 2b) are close in orientation to axis α oscillations of cooling at the cones of the GTFE 11 of the maximal thermal expansion of the structure. reached 400°C (Vergasova et al., 2007). The results of Thus, the anisotropy of thermal deformations of the study of thermal expansion of the minerals are given bradaczekite structure is caused by nonequivalent below. lengths of chemical bonds in octahedrons Cu(2)O6 and Bradaczekite. The temperature-dependent varia- Cu(3)O6 distorted due to the Jahn-Teller effect. tions of monoclinic unit-cell dimensions (Fig. 1a) were Urusovite. In urusovite, the monoclinic unit-cell fitted by polynomials not higher than the second order: dimensions linearly vary with temperature to a first a = 12.049 + 0.104 × 10–3 × T + 0.139 × 10–6 × T2, b = approximation (Fig.
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