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Abstract-A Siliceous Sublimate, Collected from an Active Fumarole of Kuju Volcano, Was Analyzed for Major Constituents

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Abstract-A Siliceous Sublimate, Collected from an Active Fumarole of Kuju Volcano, Was Analyzed for Major Constituents Geochemical Journal. Vol. 2, pp. 1 to 9, 1968. Silicon content of fumarolic gases and the formation of a siliceous sublimate FUMIHIRO HONDA and YOSHIHIKO MIZUTANI Department of Earth Sciences, Faculty of Science, Nagoya University, Chikusa, Nagoya, Japan (Received October 10, 1967; in revised form February 26, 1968) Abstract-A siliceous sublimate, collected from an active fumarole of Kuju Volcano, was analyzed for major constituents. The water soluble fraction of the sublimate contains large quantities of halogen acids and silicon, and the insoluble fraction consists of hydrated silica with a trace amount of native sulfur. In order to as certain the presence of gaseous silicon compounds in fumarolic gases, condensate samples were collected from high temperature fumaroles of Kuja and Nasudake Volcanoes with a silica-free sampling device. The silicon and fluorine contents of fumarolic gases range from 1 to 52 mg Si/kg H20 and 1 to 320 mg F/kg 1120, res pectively. Silicon is transported probably as fluoride in fumarolic gases, and the sublimate is formed by hydrolysis of silicon fluoride when the gas temperature falls to the boiling point of water. INTRODUCTION Fluorosilicic compounds are believed to play an important role in the trans portation of silicon in volcanic gases. LOVERING (1957) studied -the alteration of volcanic ash by the reaction with halogen acid at Valley of Ten Thousand Smokes, Alaska, and suggested that loss or gain of silica on the altered ash possibly re flected the attack of hydrogen fluoride or the hydrolysis of silicon fluoride. NABOKO (1957) also demonstrated the effect of gaseous fluorine compounds on basaltic rocks at Klyuchevskoy Volcano, Kamchatka. YOSHIDA et al. (1966) found a siliceous vol canic sublimate, in an area of high temperature fumaroles at Satsuma-Iwojima Vol cano, Kyusyu, Japan, which contained very high concentrations of halogen acids, and suggested that the sublimate was formed by hydrolysis of silicon fluoride in the volcanic gases. In 1965, the present authors also found a siliceous sublimate in an area of high temperature fumaroles at Kuju Volcano, Kyusyu, Japan, which was similar in occurrence and composition to that reported by YOSHIDA et al. In order to demonstrate the presence of gaseous silicon compounds in fumarolic gases, con densate samples were collected in the Kuju fumarolic area and in the fumarolic area of Nasudake Volcano, Honshu, Japan, in 1966. This study is intended to de termine the chemical composition of the sublimate and the silicon and fluorine contents of the fumarolic gases, and to discuss the behavior of silicon fluoride in fumarolic gases. 2 F. HONDA and Y. MIZUTANI OCCURRENCE OF THE SUBLIMATE In the Kuju fumarolic area, native sulfur is commercially collected by intro ducing high temperature fumarolic gases into artificial gas channels, where native sulfur is deposited as the temperature of the gases falls. A siliceous sublimate was found on the outer wall of a gas channel in the hottest fumarole-group (the highest temperature was nearly 400°C). The sublimate is white and forms a large loose crust; 20 to 30 cm in diameter and 1 to 2 cm thick. Under the sublimate, a weak emission of gases was found, and a temperature of about 80°C was recorded. EXPERIMENTAL Chemical and X-ray diffraction analyses of the sublimate The sublimate was washed with a known volume of distilled water. The in soluble fraction was filtered and dried up to be subjected to X-ray diffraction analysis. An X-ray diffraction pattern was obtained by a Geiger-Flex X-ray dif fractometer, with nickel-filtered copper radiation. The soluble fraction was analyzed as follow: Si : Colorimetric determination with molybdate (Aluminum salt was added to prevent the interference by fluorine (TARUTANI, 1956) ). F : Thorium-alizarin titration. Cl : Colorimetric determination with mercuric thiocyanate. SW : Gravimetric determination as barium sulfate. NHs : Colorimetric determination with Nessler reagent. Br+I : Iodometry. Collection of fumarolic gas samples Fumarolic gases were collected through a teflon tubing into a polyethylene cold trap containing 10 to 20 g of sodium carbonate powder, which prevents for mation of colloidal sulfur from the reaction of hydrogen sulfide with sulfur dioxide, and precipitation of silica in the condensate. Chemical analysis of fumarolic gases The condensate was treated with hydrogen peroxide to oxidize the sulfur com pounds into sulfate, and then subjected to subsequent analyses: Si : Colorimetric determination with molybdate (Aluminum salt was added to prevent the interference by fluorine.). F : Colorimetric determination with Thorin after the separation by perchloric acid distillation. Cl: Colorimetric determination with mercuric thiocyanate and iron alum. RESULTS AND DISCUSSION The chemical nature of the sublimate is similar to that of the sublimate from Satsuma-Iwojima Volcano reported by YOSHIDA et al. (1966) as shown in Table 1. Silicon content of fumarolic gases and the formation of a siliceous sublimate 3 Table 1. Chemical composition of siliceous sublimates Siliceous sublimates Siliceous sublimates from from Kuju Volcano Satsuma-Iwozima Volcano* Sample No. 1 2 4 5 SiO2, insoluble 28.2% 30.7% 2.9% 44.0% S, insoluble tr. tr. 0.28 7.1 F, insoluble 0.12 1.5 Si02, soluble 2.65 1.55 0.46 0.05 H2SiF6** 18.9 11.4 6.3 0.67 HC1 3.65 5.25 8.6 4.3 HI+HBr <10-s <10-s 0.015 0.006 H2S04 <0.05 <0.05 0.01 0.09 NH3 0.011 0.004 H2O 46.5 51.0 81.4 42.2 total 100.0 100.0 100.0 99.9 * Cited from YOSHIDA et al. (1966). ** Calculated allotting the soluble fluorine to this species. s 0 10 20 30 40 50 2 0* Fig. 1. X-ray diffraction pattern of a sublimate collected from Kuju-Volcano, Kyusyu, Japan. S indicates sulfur peaks. These sublimates are characterized by a high halogen acid content. The X-ray diffraction pattern of the insoluble fraction of the sublimate is shown in Fig. 1. The insoluble fraction consists of amorphous silica with a trace amount of rhombic sulfur. The silica must have existed as hydrated silica in the sublimate. In Table 2 are given the silicon and halogen contents of the fumarolic gases from Kuju and Nasudake Volcanoes. Relatively high concentrations of silicon and fluorine are found in the gases from KH-1 series fumaroles of Kuju Volcano, where the siliceous sublimate was found. On the other hand, in fumarolic gases from Nasudake with rather low fluorine contents, low concentration of silicon was found. According to IWASAKI et al. (1966), high temperature fumaroles of Satsuma-Iwojima Volcano, where an abundance of siliceous sublimates were found by YOSHIDA et al., are characterized also by a high fluorine content of fumarolic gases. Fluorine content as high as 2,720 mg F/kg H20 was found in the fumarolic gases of Satsuma-Iwojima 4 F. HONDA and Y. MIZUTANI Table 2. Silicon and halogen contents of fumarolic gases Fumarole Temp. (*C) Si ppm(wt. ) F ppm(wt. ) Cl ppm(wt. ) Kuju Volcano KH-1 d-1 240 52 310 5180 KH-1 d-2 238 51 320 6150 KO-2 148 21 46 1620 KX-5 133 13 100 5660 KO-1 b 128 26 63 2270 KO-3 128 9.8 17 2920 KX-4 123 9.7 160 5060 KX-6 118 13 48 3150 KH-1 b 110 12 110 5670 KX-3 105 18 130 4580 KH-1 e 99 19 170 3780 Nasudake CH-1 308 5.5 15 170 M-4 b 267 9.5 8.5 480 UN-2 190 2.5 1.6 570 0-1 b 188 9.0 25 560 0-1 d 174 5.7 21 550 U-1 148 4.0 1.0 1240 CH-2 135 5.0 1.4 0-2 b 118 2.5 12 120 M-5 96 1.0 3.2 Volcano in 1958 by IWASAKI et al. These evidences suggest that high temperature fumarolic gases containing a large amount of fluorine may transport silicon, and that the silicon may be present mainly as fluoride in the fumarolic gases. Based on these characters of the sublimate and fumarolic gases, it can be assumed that, as pointed out by YOSHIDA et al., the siliceous sublimates were formed by the hydrolysis of silicon fluoride with liquid water: 3 SiF4 gas + n H20(11Q.)= Si02-(n 2)H20 + 2 H2SiF6faq.) (1) The hydrochloric acid in the sublimates was derived probably by condensation of hydrogen chloride in fumarolic gases, and the native sulfur was formed by interaction of sulfur dioxide and hydrogen sulfide, air oxidation of hydrogen sulfide, or sublimation of sulfur vapor. From these considerations, thermodynamic calculations were made to examine the possibility that the silicon in the fumarolic gases is transported as gaseous silicon fluoride. The reactions considered are: CaSiO3 + 6 HF = CaF2 + SiF4 + 3 H2O (2) MgSiO3 + 6 HF = MgF2 + SiF4 + 3 H2O (3) Na2SiO3 + 6 HF = 2 NaF + SiF4 + 3 H2O (4) Si02+4HF=SiF4+2 H2O (5) Silicon content of fumarolic gases and the formation of a siliceous sublimate 5 The equilibrium constants of these reactions, K, were calculated from the thermo dynamical data given by KUBASCHEWSKI and EVANS (1956) : log K2= 0.345 1.651n T+ 1.06 x 10_3 T + 14850 T-'+ 1.06 x 104 T-2 (6) log K3= -6.99-0.6191nT+0.406x10_3T-+ 13950T-1-2.12x104T-2 (7) log K.1= 0.188 1.541n T+ 0.538 x 10_3 T+ 14270 T'-' + 4.92 x 104 Tie (8) log K5 = 1.073 0.635 In T + 0.146 x 10-3 T + 5735 T-1 2.33 x 104 T-2 (9) For reactions (2), (3), and (4), Kmay be expressed as follows by the first approxi mation assuming that the activities of components are unity : y •Xto K X64 HF• P22 (10) and for reaction (5), it may be expressed as 40 30 15 o kl~ I 20 0 10 W 0 teaG SiF4 Si02 10 5 O 0 100 200 300 400 500 600 700 0 100 200 300 400 500 600 700 Temp., ('C) Temp., CC) Fig.
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