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1.
We report chemical compositions (major and trace components including light hydrocarbons), hydrogen, oxygen, helium and nitrogen isotope ratios of volcanic and geothermal fluids of Mutnovsky volcano, Kamchatka. Several aspects of the geochemistry of fluids are discussed: chemical equilibria, mixing of fluids from different sources, evaluation of the parent magmatic gas composition and contributions to magmatic vapors of fluids from different reservoirs of the Kamchatkan subduction zone. Among reactive species, hydrogen and carbon monoxide in volcanic vapors are chemically equilibrated at temperatures >300°C with the SO2-H2S redox-pair. A metastable equilibrium between saturated and unsaturated light hydrocarbons is attained at close to discharge temperatures. Methane is disequilibrated. Three different sources of fluids from three fumarolic fields in the Mutnovsky craters can be distinguished: (1) magmatic gas from a large convecting magma body discharging through Active Funnel, a young crater with the hottest fumaroles (up to 620°C) contributing ~80% to the total volcanic gas output; (2) volcanic fluid from a separate shallow magma body beneath the Bottom Field of the main crater (96–280°C fumaroles); and (3) hydrothermal fluid with a high relative and absolute concentrations of CH4 from the Upper Field in the main crater (96–285°C fumaroles). The composition of the parent magmatic gas is estimated using water isotopes and correlations between He and other components in the Active Funnel gases. The He-Ar-N2 systematics of volcanic and hydrothermal fluids of Mutnovsky are consistent with a large slab-derived sedimentary nitrogen input for the nitrogen inventory, and we calculate that only ~1% of the magmatic N2 has a mantle origin and <<1% is derived from the arc crust.  相似文献   

2.
Phreatic eruptions occurred at the Meakandake volcano in 1988, 1996, 1998, 2006, and 2008. We conducted geochemical surveillance that included measurements of temperature, SO2 emission rates, and volcanic gas composition from 2003 to 2008 at the Nakamachineshiri (NM), Northwest (NW), and Akanuma (AK) fumarolic areas, and the 96–1 vent, where historical eruptions had occurred. The elemental compositions of the gases discharged from the different areas are similar compared with the large variations observed in volcanic gases discharged from subduction zones. All the gases showed high apparent equilibrium temperatures, suggesting that all these gases originated from a common magmatic gas. The gases discharged from each area also exhibited different characteristics, which are probably the results of differences in the conditions of meteoric water mixing, quenching of chemical reactions, and vapor-liquid separation. The highest apparent equilibrium temperatures (about 500°C) were observed in the case of NW fumarolic gases, despite the low outlet temperature of about 100°C at these fumaroles. Since the NW fumaroles were formed as a result of the 2006 phreatic eruption, the high-temperature gas supply to the NW fumarole suggests that the phreatic eruption was caused by the ascent of high-temperature magmatic gases. The temperatures, compositions, and emission rates of the NM and 96–1 gases did not show any appreciable change after the 2006 eruption, indicating that each fumarolic system had a separate magmatic-hydrothermal system. The temperatures, compositions, and emission rates of the NM fumarolic gases were apparently constant, and these fumaroles are inferred to be formed by the evaporation of a hydrothermal system with a constant temperature of about 300°C. The 96–1 gas compositions showed large changes during continuous temperature decrease from 390° to 190°C occurred from 2003 to 2008, but the sulfur gas emission rates were almost constant at about four tons/day. At the 96–1 vent, the SO2/H2S ratio decreased, while the H2/H2O ratio remained almost constant; this was probably caused by the rock-buffer controlled chemical reaction during the temperature decrease.  相似文献   

3.
Remotely sensed measurements of sulphur dioxide (SO2) emitted by Turrialba Volcano (Costa Rica) are reported for the period September 2009–January 2011. These measurements were obtained using images from Advanced Spaceborne Thermal Emission and Reflexion radiometer, Ozone Monitoring Instrument and a ground-based UV camera. These three very different instruments provide flux measurements in good agreement with each other, which demonstrate that they can be integrated for monitoring SO2 fluxes. Fluxes from Turrialba increased fourfold in January 2010, following a phreatic explosion that formed a degassing vent in the W crater of Turrialba. Since then, the SO2 flux has remained high (30–50?kg/s) but seems to be showing a slowly decreasing trend. We interpret this evolution as the start of open vent degassing from a recently intruded magma body. The opening of the degassing vent decreased the confining pressure of the magma body and allowed the gases to bypass the hydrothermal system.  相似文献   

4.
 Two geochemical surveys carried out in March 1991 and September 1992 revealed the existence of a hydrothermal system in the southern portion of Montserrat Island, below Soufrière Hills Volcano. This conclusion is supported by the presence of: (a) the thermal springs of Plymouth which are fed by deep Na–Cl waters (Cl concentration ∼25 000 mg/kg, temperature ca. 250  °C) mixed with shallow steam-heated waters; (b) the four fumarolic fields of Galway's Soufrière, Gages Upper Soufrière, Gages Lower Soufrière, and Tar River Soufrière, where acid to neutral, steam-heated waters are present together with several fumarolic vents, discharging vapors formed through boiling of hydrothermal aqueous solutions. Involvement of magmatic fluids in the recharge of the hydrothermal aquifers is suggested by: (a) the high 3He/4He ratios of fumarolic fluids, i.e., 8.2 RA at Galway's Soufrière and 5.9 RA at Gages Lower Soufrière; (b) the δD and δ18O values of Na–Cl thermal springs and steam condensates, indicating the involvement of arc-type magmatic water in the formation of deep geothermal liquids; and (c) the CH4/CO2 ratios of fumarolic fluids, which are lower than expected for equilibrium with the FeO–FeO1.5 hydrothermal rock buffer, but being shifted towards the SO2–H2S magmatic gas buffer. Received: 26 March 1996 / Accepted: 19 July 1996  相似文献   

5.
 The purpose of this work was to study jointly the volcanic-hydrothermal system of the high-risk volcano La Soufrière, in the southern part of Basse-Terre, and the geothermal area of Bouillante, on its western coast, to derive an all-embracing and coherent conceptual geochemical model that provides the necessary basis for adequate volcanic surveillance and further geothermal exploration. The active andesitic dome of La Soufrière has erupted eight times since 1660, most recently in 1976–1977. All these historic eruptions have been phreatic. High-salinity, Na–Cl geothermal liquids circulate in the Bouillante geothermal reservoir, at temperatures close to 250  °C. These Na–Cl solutions rise toward the surface, undergo boiling and mixing with groundwater and/or seawater, and feed most Na–Cl thermal springs in the central Bouillante area. The Na–Cl thermal springs are surrounded by Na–HCO3 thermal springs and by the Na–Cl thermal spring of Anse à la Barque (a groundwater slightly mixed with seawater), which are all heated through conductive transfer. The two main fumarolic fields of La Soufrière area discharge vapors formed through boiling of hydrothermal aqueous solutions at temperatures of 190–215  °C below the "Ty" fault area and close to 260  °C below the dome summit. The boiling liquid producing the vapors of the Ty fault area has δD and δ18O values relatively similar to those of the Na–Cl liquids of the Bouillante geothermal reservoir, whereas the liquid originating the vapors of the summit fumaroles is strongly enriched in 18O, due to input of magmatic fluids from below. This process is also responsible for the paucity of CH4 in the fumaroles. The thermal features around La Soufrière dome include: (a) Ca–SO4 springs, produced through absorption of hydrothermal vapors in shallow groundwaters; (b) conductively heated, Ca–Na–HCO3 springs; and (c) two Ca–Na–Cl springs produced through mixing of shallow Ca–SO4 waters and deep Na–Cl hydrothermal liquids. The geographical distribution of the different thermal features of La Soufrière area indicates the presence of: (a) a central zone dominated by the ascent of steam, which either discharges at the surface in the fumarolic fields or is absorbed in shallow groundwaters; and (b) an outer zone, where the shallow groundwaters are heated through conduction or addition of Na–Cl liquids coming from hydrothermal aquifer(s). Received: 9 November 1998 / Accepted: 15 July 1999  相似文献   

6.
Lastarria volcano (25°10′ S, 68°31′ W; 5,697 m above sea level), located in the Central Andes Volcanic Zone (northern Chile), is characterized by four distinct fumarolic fields with outlet temperatures ranging between 80°C and 408°C as measured between May 2006–March 2008 and April–June 2009. Fumarolic gasses contain significant concentrations of high temperature gas compounds (i.e., SO2, HCl, HF, H2, and CO), and isotopic ratios (3He/4He, δ13C–CO2, δ18O–H2O, and δD–H2O) diagnostic of magmatic gas sources. Gas equilibria systematics, in both the H2O-H2-CO2-CO-CH4 and alkane–alkene C3 system, suggest that Lastarria fumarolic gasses emanate from a superheated vapor that is later cooled and condensed at relatively shallow depths. This two-stage process inhibits the formation of a continuous aquifer (e.g., horizontal liquid layer) at relatively shallow depth. Recent developments in the magmatic gas system may have enhanced the transfer and release of heat causing shallow aquifer vaporization. The consequent pressure increase and aquifer vaporization likely triggered the inflation events beginning in 2003 at the Lastarria volcano.  相似文献   

7.
This study presents baseline data for future geochemical monitoring of the active Tacaná volcano–hydrothermal system (Mexico–Guatemala). Seven groups of thermal springs, related to a NW/SE-oriented fault scarp cutting the summit area (4,100m a.s.l.), discharge at the northwest foot of the volcano (1,500–2,000m a.s.l.); another one on the southern ends of Tacaná (La Calera). The near-neutral (pH from 5.8 to 6.9) thermal (T from 25.7°C to 63.0°C) HCO3–SO4 waters are thought to have formed by the absorption of a H2S/SO2–CO2-enriched steam into a Cl-rich geothermal aquifer, afterwards mixed by Na/HCO3-enriched meteoric waters originating from the higher elevations of the volcano as stated by the isotopic composition (δD and δ18O) of meteoric and spring waters. Boiling temperature fumaroles (89°C at ~3,600m a.s.l. NW of the summit), formed after the May 1986 phreatic explosion, emit isotopically light vapour (δD and δ18O as low as −128 and −19.9‰, respectively) resulting from steam separation from the summit aquifer. Fumarolic as well as bubbling gases at five springs are CO2-dominated. The δ13CCO2 for all gases show typical magmatic values of −3.6 ± 1.3‰ vs V-PDB. The large range in 3He/4He ratios for bubbling, dissolved and fumarolic gases [from 1.3 to 6.9 atmospheric 3He/4He ratio (R A)] is ascribed to a different degree of near-surface boiling processes inside a heterogeneous aquifer at the contact between the volcanic edifice and the crystalline basement (4He source). Tacaná volcano offers a unique opportunity to give insight into shallow hydrothermal and deep magmatic processes affecting the CO2/3He ratio of gases: bubbling springs with lower gas/water ratios show higher 3He/4He ratios and consequently lower CO2/3He ratios (e.g. Zarco spring). Typical Central American CO2/3He and 3He/4He ratios are found for the fumarolic Agua Caliente and Zarco gases (3.1 ± 1.6 × 1010 and 6.0 ± 0.9 R A, respectively). The L/S (5.9 ± 0.5) and (L + S)/M ratios (9.2 ± 0.7) for the same gases are almost identical to the ones calculated for gases in El Salvador, suggesting an enhanced slab contribution as far as the northern extreme of the Central American Volcanic Arc, Tacaná.  相似文献   

8.
We report the results of four soil H2 surveys carried out in 2000–2003 at Poás volcano, Costa Rica, to investigate the soil H2 distribution and evaluate the diffuse H2 emission as a potential surveillance tool for Poás volcano. Soil gas H2 contents showed a wide range of concentration from 0.2 to 7,059 ppmV during the four surveys. Maps of soil gas H2 based on Sequential Gaussian Simulation showed low H2 concentration values in the soil atmosphere (<0.7 ppmV) for most of the study area, whereas high soil gas H2 values were observed inside the active crater of Poás. A significant increase in soil gas H2 concentration was observed inside the active crater during 2001 and 2002 with respect to year 2000, followed by a decrease in 2003. The observed spatial and temporal variations of soil H2 concentration have been well correlated with seismicity, microgravimetry and fumarolic chemistry changes which occurred during this study. These observations evidence changes in the shallow magmatic-hydrothermal system of Poás, and it might be related to a potential magmatic intrusion during the period 1998–2004. Therefore, monitoring diffuse H2 emission of Poás has become an important geochemical tool for the monitoring of its volcanic activity.  相似文献   

9.
 Approximately 20 km south of Mt. Etna craters, at the contact between volcanic and sedimentary formations, three mud volcanoes discharge CO2-rich gases and Na–Cl brines. The compositions of gas and liquid phases indicate that they are fed by a hydrothermal system for which temperatures of 100–150  °C were estimated by means of both gas and solute geothermometry. The hydrothermal system may be associated with CO2-rich groundwaters over a large area extending from the central part of Etna to the mud volcanoes. Numerous data on the He, CH4, CO2 composition of the gases of the three manifestations, sampled over the past 5 years, indicate clearly that variations are due to separation processes of a CO2-rich gas phase from the liquid. The effects of these processes have to be taken into account in the interpretation of the monitoring data collected for the geochemical surveillance of Etna volcano. Received: 4 September 1995 / Accepted: 14 February 1996  相似文献   

10.
The simultaneous quantitative determination of two-dimensional bromine monoxide (BrO) and sulphur dioxide (SO2) distributions in volcanic gas plumes is described. Measurements at the fumarolic field on the island Vulcano (autumn 2004) and in the plume of Mt. Etna volcano (spring 2005) were carried out with an Imaging DOAS instrument. The SO2 fluxes of several fumaroles were estimated from two-dimensional distributions of SO2. Additionally, the first two-dimensional distributions of BrO within a volcanic plume were successfully retrieved. Slant column densities of up to 2.6 × 1014 molecules per square centimetre were detected in the plume of Mt. Etna. The investigation of the BrO/SO2 ratio, calculated from the two-dimensional distributions of SO2 and BrO, shows an increase from the centre to the edge of the volcanic plume. These results have significance for the involvement of ozone during BrO formation processes in volcanic emissions.  相似文献   

11.
Bulk atmospheric deposition of major cations (Na, K, Ca, Mg) and anions (Cl, F, SO4) were measured at 15 sites around an active volcano, Mount Etna, from 2001 to 2003. Their composition indicates several natural sources, among which deposition of plume-derived volcanogenic gas compounds is prevalent for F, Cl and S. Plume-derived acidic compounds are also responsible for the prevailing acidic composition of the samples collected on the summit of the volcano (pH in the 2.45–5.57 range). Cation species have complex origin, including deposition of plume volcanogenic ash and aerosols and soil-dust wind re-suspension of either volcanic or carbonate sedimentary rocks. Variation of the deposition rates during the March 2001–March 2003 period, coupled with previous measurements from 1997 to 2000 (Appl Geochem 16:985–1000, 2001), were compared with the variation of SO2 flux, volcanic activity and rainfall. The deposition rate was mainly controlled by rainfall. Commonly, about 0.1–0.9% of HF, HCl and SO2 emitted by the summit crater's plume were deposited around the volcano. We estimate that ∼2 Gg of volcanogenic sulphur were deposited over the Etnean area during the 2002–2003 flank eruption, at an average rate of ∼24 Mg day−1 which is two orders of magnitude higher than that typical of quiescent degassing phases.  相似文献   

12.
The densely populated metropolitan area of Quito is located on the slopes of the active Guagua Pichincha volcano at only 10 km from the crater. Recently, the Italian Ministry of Foreign Affairs sponsored a project for the mitigation of volcanic hazard in this area. The geochemical study carried out as part of this project was aimed at constructing a geochemical model of the zone for use in volcanic surveillance.According to this geochemical model, a hydrothermal aquifer (T = 200–240°C), fed both by meteoric waters and by fluids released by a magma body, lies at shallow levels beneath Guagua Pichincha crater. The crater fumaroles are essentially fed by steam boiled off from the hydrothermal aquifer. The high flow rate fumaroles located in the dome area show significant SO2 contents, which suggest a relatively high contribution of magmatic fluids in the zone of the aquifer feeding them. The absence of SO2 in the fumarolic discharges near the southern crater wall indicates instead that the magmatic fluids dissolve entirely into the aquifer here. The hot springs located at the western end of the crater represent the lateral discharge of the hydrothermal aquifer.On the basis of this model, it is likely that an increment in the flux of both the magmatic fluids and the heat from a magma body produces an increase, albeit small, of the pressure-temperature conditions of the hydrothermal system and consequent changes in flow rate and fluid chemistry of the fumarolic vents. In particular, total sulphur and possibly hydrochloric acid may increase in all the vents and sulphur dioxide may appear in other fumarolic discharges. The varying thermodynamic conditions in the hydrothermal aquifer can be evaluated on the basis of the equilibria among carbon species and hydrogen. Only minor delayed changes are expected in the physical-chemical characteristics of the springs located at the western end of the crater.  相似文献   

13.
2 and approximately 85% SO2 of the total sulfur gas. Relative amounts of He, Ar, and N2 show a distinct hot-spot signature ( ). The δ13C–CO2 is approximately −3.6‰ and δ34ST is approximately +3.3‰. The δD/δ18O of fumarole H2O indicates steam separation from local meteoric waters whose estimated minimum mean residence time from 3H analyses is ≤40 years. Fumarolic activity at Alcedo is controlled by a caldera-margin fault containing at least seven hydrothermal explosion craters, and by an intracaldera rhyolite vent. Two explosion craters which formed in 1993–1994 produce approximately 15 m3/s of steam, yet discharge temperatures are ≤97°C. Water content of the total gas is 95–97 mol.%, noncondensible gas is 92–98 mol.% CO2, and sulfur gas is dominated by H2S. Relative amounts of He, Ar, and N2 show extensive mixing between hot spot and air or air-saturated meteoric water components but the average . The δ13C–CO2 is approximately −3.5‰ and δ34ST is approximately −0.8‰. The δD/δ18O of fumarole steam indicates separation from a homogeneous reservoir that is enriched 3–5‰ in 18O compared with local meteoric water. 3H indicates that this reservoir water has a maximum mean residence time of approximately 400 years and empirical gas geothermometry indicates a reservoir temperature of 260–320°C. The intracaldera hydrothermal reservoir in Alcedo is probably capable of producing up to 150 MW; however, environmental concerns as well as lack of infrastructure and power users will limit the development of this resource. Received: 19 April 1999 / Accepted: 23 October 1999  相似文献   

14.
Low-to-high temperature fumaroles discharging from the Active Crater of Lascar volcano (northern Chile) have been collected in November 2002, May 2005 and October 2006 for chemical and isotopic analysis to provide the first geochemical survey on the magmatic-hydrothermal system of this active volcano. Chemical and isotopic gas composition shows direct addition of high-temperature fluids from magmatic degassing, mainly testified by the very high contents of SO2, HCl and HF (up to 87,800, 29,500 and 2,900 μmol/mol) and the high R/Ra values (up to 7.29). Contributions from a hydrothermal source, mainly in gas discharges of the Active Crater rim, has also been detected. Significant variations in fluid chemistry, mainly consisting of a general decrease of magmatic-related compounds, i.e. SO2, have affected the fumarolic system during the period of observation, indicating an increase of the influence of the hydrothermal system surrounding the ascending deep fluids. The chemical composition of Active Crater fumaroles has been used to build up a geochemical model describing the main processes that regulate the fluid circulation system of Lascar volcano to be utilized in volcanic surveillance.  相似文献   

15.
A miniaturized, lightweight and low-cost UV correlation spectrometer, the FLYSPEC, has been developed as an alternative for the COSPEC, which has long been the mainstay for monitoring volcanic sulfur dioxide fluxes. Field experiments have been conducted with the FLYSPEC at diverse volcanic systems, including Masaya (Nicaragua), Poás (Costa Rica), Stromboli, Etna and Vulcano (Italy), Villarica (Chile) and Kilauea (USA). We present here those validation measurements that were made simultaneously with COSPEC at Kilauea between March 2002 and February 2003. These experiments, with source emission rates that ranged from 95 to 1,560 t d−1, showed statistically identical results from both instruments. SO2 path-concentrations ranged from 0 to >1,000 ppm-m with average correlation coefficients greater than r 2=0.946. The small size and low cost create the opportunity for FLYSPEC to be used in novel deployment modes that have the potential to revolutionize the manner in which volcanic and industrial monitoring is performed.  相似文献   

16.
Mombacho is a deeply dissected volcano belonging to the Quaternary volcanic chain of Nicaragua. The southern, historic collapse crater (El Crater) currently hosts a fumarolic field with a maximum temperature of 121°C. Chemical and isotopic data from five gas-sampling field campaigns carried out in 2002, 2003 and 2005 highlight the presence of high-temperature gas components (e.g. SO2, HCl and HF), which indicate a significant contribution of juvenile magmatic fluids to the hydrothermal system feeding the gas discharges. This is strongly supported by the mantle-derived helium and carbon isotopic signatures, although the latter is partly masked by either a sedimentary subduction-related or a shallow carbonate component. The observed chemical and isotopic composition of the Mombacho fluids seems to indicate that this volcanic system, although it has not experienced eruptive events during the last centuries, can be considered active and possibly dangerous, in agreement with the geophysical data recorded in the region. Systematic geochemical monitoring of the fumarolic gas discharges, coupled with a seismic and ground deformation network, is highly recommended in order to monitor a possible new eruptive phase.  相似文献   

17.
A field gas chromatograph, built in 1978, was used in the field to directly analyse volcanic gases before water vapor condensation. Tested in Vulcano (Italy), Kilauea (Hawaii) and Merapi (Indonesia), this field measurement technique provides the actual composition of the volcanic gas mixture. The technique avoids the depletion of sulfur gases and the dissolution of the acid gases in the condensed water during the cooling. Thus the mixture of H2S and SO2 in fumarolic and high temperature gases (up to 819°C) in equilibrium at the emission temperature was examined.  相似文献   

18.
We describe analytical details and uncertainty evaluation of a simple technique for the measurement of the carbon isotopic composition of CO2 in volcanic plumes. Data collected at Solfatara and Vulcano, where plumes are fed by fumaroles which are accessible for direct sampling, were first used to validate the technique. For both volcanoes, the plume-derived carbon isotopic compositions are in good agreement with the fumarolic compositions, thus providing confidence on the method, and allowing its application at volcanoes where the volcanic component is inaccessible to direct sampling. As a notable example, we applied the same method to Mount Etna where we derived a δ13C of volcanic CO2 between −0.9 ± 0.27‰ and −1.41 ± 0.27‰ (Bocca Nuova and Voragine craters). The comparison of our measurements to data reported in previous work highlights a temporal trend of systematic increase of δ13C values of Etna CO2 from ~ −4‰, in the 1970’s and the 1980’s, to ~ −1‰ at the present time (2009). This shift toward more positive δ13C values matches a concurrent change in magma composition and an increase in the eruption frequency and energy. We discuss such variations in terms of two possible processes: magma carbonate assimilation and carbon isotopic fractionation due to magma degassing along the Etna plumbing system. Finally, our results highlight potential of systematic measurements of the carbon isotopic composition of the CO2 emitted by volcanic plumes for a better understanding of volcanic processes and for improved surveillance of volcanic activity.  相似文献   

19.
2 and δ13C in soil gas were measured at three active subduction-related stratovolcanoes (Arenal and Poás, Costa Rica; Galeras, Colombia). In general, Rn, CO2 and δ13C values are higher on the lower flanks of the volcanoes, except near fumaroles in the active craters. The upper flanks of these volcanoes have low Rn concentrations and light δ13C values. These observations suggest that diffuse degassing of magmatic gas on the upper flanks of these volcanoes is negligible and that more magmatic degassing occurs on the lower flanks where major faults and greater fracturing in the older lavas can channel magmatic gases to the surface. These results are in contrast to findings for Mount Etna where a broad halo of magmatic CO2 has been postulated to exist over much of the edifice. Differences in radon levels among the three volcanoes studied here may result from differences in age, the degree of fracturing and faulting, regional structures or the level of hydrothermal activity. Volcanoes, such as those studied here, act as plugs in the continental crust, focusing magmatic degassing towards crater fumaroles, faults and the fractured lower flanks. Received: 16 December 1997 / Accepted: 27 January 2000  相似文献   

20.
The June 1991 eruption of Mount Pinatubo, Philippines breached a significant, pre-eruptive magmatic-hydrothermal system consisting of a hot (>300 °C) core at two-phase conditions and surrounding, cooler (<260 °C) liquid outflows to the N and S. The eruption created a large, closed crater that accumulated hydrothermal upwellings, near-surface aquifer and meteoric inflows. A shallow lake formed by early September 1991, and showed a long-term increase in level of ~1 m/month until an artificial drainage was created in September 2001. Comparison of the temporal trends in lake chemistry to pre- and post-eruptive springs distinguishes processes important in lake evolution. The lake was initially near-neutral pH and dominated by meteoric influx and Cl–SO4 and Cl–HCO3 hydrothermal waters, with peaks in SO4 and Ca concentrations resulting from leaching of anhydrite and aerosol-laden tephra. Magmatic discharge, acidity (pH~2) and rock dissolution peaked in late 1992, during and immediately after eruption of a lava dome on the crater floor. Since cessation of dome growth, trends in lake pH (increase from 3 to 5.5), temperature (decline from 40 to 26 °C), and chemical and isotopic composition indicate that magmatic degassing and rock dissolution have declined significantly relative to the input of meteoric water and immature hydrothermal brine. Higher concentrations of Cl, Na, K, Li and B, and lower concentrations of Mg, Ca, Fe, SO4 and F up to 1999 highlight the importance of a dilute hydrothermal contribution, as do stable-isotope and tritium compositions of the various fluids. However, samples taken since that time indicate further dilution and steeper trends of increasing pH and declining temperature. Present gas and brine compositions from crater fumaroles and hot springs indicate boiling of an immature Cl–SO4 geothermal fluid of near-neutral pH at approximately 200 °C, rather than direct discharge from magma. It appears that remnants of the pre-eruptive hydrothermal system invaded the magma conduit shortly after the end of dome emplacement, blocking the direct degassing path. This, along with the large catchment area (~5 km2) and the high precipitation rate of the area, led to a rapid transition from a small and hot acid lake to a large lake with near-ambient temperature and pH. This behavior contrasts with that of peak-activity lakes that have more sustained volcanic gas influx (e.g., Kawah Ijen, Indonesia; Poas and Rincón de la Vieja, Costa Rica).Editorial responsibility: H. Shinohara  相似文献   

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