Bulletin of Volcanology

Volatiles and Energy released by the Puracé volcano, Colombia

--Manuscript Draft--

Manuscript Number:

Full Title: Volatiles and Energy released by the Puracé volcano, Colombia

Article Type: Research Article

Corresponding Author: Salvatore Inguaggiato, M.D.

Istituto nazionale di geofisica e vulcanologia
Palermo, ITALY

Corresponding Author Secondary

Information:

Order of Authors: Luisa Fernanda Meza Maldonado

Salvatore Inguaggiato, M.D.

Marco Tulio Jaramillo

Gustavo Garzón Valencia

Agnes Mazot

Funding Information:

Abstract: Total CO2 output of Puracè volcano (Colombia) was carried out on the basis of fluids
discharged by fumarole, soil gases and dissolved carbon species in the aquifer. The
soil CO2 output emission was computed utilizing a geochemical field survey of 512
point of measurements of CO2 soil fluxes from the whole Purace volcano area. While,
the CO2 flux from Puracè "plume" was estimated with a indirect method, considering
the SO2 plume flux and CO2/SO2 ratio of main high temperature fumarole. The overall
output of CO2 was estimated around 1500 t/day. The main contribution of CO2 comes
from the "plume" (summit degassing) and from the San Juan soil emission (peripheral
degassing) with respectively 673 and 812 t/day. The contribution of summit and
peripheral areas are comparable 698 vs 851 t/day, indicating an intermediate
degassing style between closed and open conduct volcanic systems. The H2O vapor
estimation (by the chemical composition of fumarole and the SO2 plume flux) allowed
to calculate the related thermal energy released from the Puracè volcano system (163
MW).

Suggested Reviewers: Deborah Bergfeld

dbergfel@usgs.gov

Jennifer L. Lewicki
jllewicki@lbl.gov

Yuri Taran
yuri.taran@gmail.com; taran@geofisica.unam.mx

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Volatiles and Energy released by the Puracé volcano, Colombia

Luisa Fernanda Meza Maldonadoa, c, Salvatore Inguaggiatob,*, Marco Tulio Jaramilloc,
Gustavo Garzón Valenciad, Agnes Mazote
a. Servicio Geológico Colombiano, Observatorio Vulcanológico y Sismológico de Popayán,
Colombia
b. Istituto Nazionale di Geofisica e Vulcanologia, Palermo, Italy
c. Universidad de Caldas, Manizales ,Colombia
d. Servicio Geológico Colombiano, Observatorio Vulcanológico y Sismológico de Pasto, Colombia
e. GNS Science Wairakei Research Centre, Taupo, New Zealand

* Corresponding author

To Bullettin Volcanology

Total CO2 output of Puracè volcano (Colombia) was carried out on the basis of fluids discharged by
fumarole, soil gases and dissolved carbon species in the aquifer. The soil CO2 output emission was
computed utilizing a geochemical field survey of 512 point of measurements of CO 2 soil fluxes
from the whole Purace volcano area. While, the CO2 flux from Puracè "plume" was estimated with
a indirect method, considering the SO2 plume flux and CO2/SO2 ratio of main high temperature
fumarole. The overall output of CO2 was estimated around 1500 t/day. The main contribution of
CO2 comes from the "plume" (summit degassing) and from the San Juan soil emission (peripheral
degassing) with respectively 673 and 812 t/day. The contribution of summit and peripheral areas are
comparable 698 vs 851 t/day, indicating an intermediate degassing style between closed and open
conduct volcanic systems. The H2O vapor estimation (by the chemical composition of fumarole and
the SO2 plume flux) allowed to calculate the related thermal energy released from the Puracè
volcano system (163 MW).

Suggested reviewers:
Deborah Bergfeld
U.S. Geological Survey MS #434
345 Middlefield Rd.
Menlo Park, CA 94025
Tel: (650) 329-4657
e-mail: dbergfel@usgs.gov

Jennifer L. Lewicki
Address: Earth Sciences Division
Lawrence Berkeley National Laboratory
1 Cyclotron Rd., MS 90-1116
Berkeley, CA 94720
Work Phone: 510-495-2818
e-mail: jllewicki@lbl.gov

Yuri Taran
Instituto de Geofísica, UNAM,
México DF, Mexico
email: taran@geofisica.unam.mx,
email: yuri.taran@gmail.com,

Dmitri Rouwet
INGV_Bologna
Italy
e-mail: dmitri.rouwet@ingv.it
Best Regards
Salvatore Inguaggiato
Manuscript Click here to download Manuscript Purace CO2 Meaz.docx

Click here to view linked References

1 Volatiles and Energy released by the Puracé volcano, Colombia

2 Luisa Fernanda Meza Maldonadoa, c, Salvatore Inguaggiatob,*, Marco Tulio Jaramilloc,

3 Gustavo Garzón Valenciad, Agnes Mazote
4
5 a. Servicio Geológico Colombiano, Observatorio Vulcanológico y Sismológico de Popayán, Colombia
6 b. Istituto Nazionale di Geofisica e Vulcanologia, Palermo, Italy
7 c. Universidad de Caldas, Manizales ,Colombia
8 d. Servicio Geológico Colombiano, Observatorio Vulcanológico y Sismológico de Pasto, Colombia
9 e. GNS Science Wairakei Research Centre, Taupo, New Zealand
10
11 * Corresponding author
12
13 Keywords: CO2 output; Helium isotope; Puracè volcano; Soil CO2 degassing; SO2 plume output
14
15 Abstract

16 Total CO2 output of Puracè volcano (Colombia) was carried out on the basis of fluids discharged by

17 fumarole, soil gases and dissolved carbon species in the aquifer. The soil CO2 output emission was

18 computed utilizing a geochemical field survey of 512 point of measurements of CO 2 soil fluxes

19 from the whole Purace volcano area. While, the CO2 flux from Puracè "plume" was estimated with

20 a indirect method, considering the SO2 plume flux and CO2/SO2 ratio of main high temperature

21 fumarole. The overall output of CO2 was estimated around 1500 t/day. The main contribution of

22 CO2 comes from the "plume" (summit degassing) and from the San Juan soil emission (peripheral

23 degassing) with respectively 673 and 812 t/day. The contribution of summit and peripheral areas are

24 comparable 698 vs 851 t/day, indicating an intermediate degassing style between closed and open

25 conduct volcanic systems. The H2O vapor estimation (by the chemical composition of fumarole and

26 the SO2 plume flux) allowed to calculate the related thermal energy released from the Puracè

27 volcano system (163 MW).

28

29 1. Introduction

30 The active volcanoes discharge significant amount of gases into the atmosphere throughout their

31 visible manifestations like plume and fumaroles. Moreover, several investigation carried out in the
32 last decades showed the importance of volcanic gases emitted from soils and aquifers (Inguaggiato

33 et al. 2012, 2013; Cardellini et al., 2003; Chiodini et al., 1996; Pecoraino et al., 2005; Mazot et al.,

34 2011). The soil degassing in the volcanic areas are characterized mainly by CO 2 emissions,

35 considering that this gas represents the dominant dry volcanic gas. In general, the study of the

36 fluxes of carbon dioxide emitted from the active volcanoes has environmental and surveillance

37 applications.

38 The measurement of carbon dioxide fluxes from the soils is a tool to quantify changes in surface

39 geothermal activity (Chiodini et al., 2005; Inguaggiato et al., 2012, 2017; Fridriksson, 2009). The

40 carbon dioxide is effectively used as a degasification tracer for magma due to its low solubility in

41 silicate castings (Gutiérrez, 2009). This gas travels to the surface through advective-diffusive

42 processes and manifests itself on the surface of the volcano. (Hernández et al., 2001). The amount

43 of carbon dioxide emitted by the different hydrothermal alterations (fumaroles, hot soils, geysers,

44 mud puddles) can be studied in such a way as to provide interesting information. According to

45 Fridriksson (2006), the measurement of the concentration of carbon dioxide in the released vapor,

46 allows to quantify directly the vapor flow and the heat flow, from the carbon dioxide flows

47 measured in the hydrothermal system. According to Padrón et al. (2003), Magaña et al. (2004) and

48 López et al. (2004), the carbon dioxide emitted in hydrothermal systems serves to identify areas

49 where anomalies occur, which usually coincide with areas where there is a great vertical

50 permeability, characterized by a greater flow from the reservoir to the surface, where CO2-rich

51 water moves easily. Therefore, it is clear that the study of this gas has an important role in the

52 individuation of weak structural zones and in the study of the evolution of hydrothermal flows at

53 different depths (Gutiérrez, 2009).

54 Recently, studies have been focused on the study of diffuse carbon dioxide emissions across the

55 whole surface of the volcano, considering that these emissions arrive at the surface in different

56 carbon species form and connected to different surface manifestations (plume, fumaroles, waters
57 and soil degassing). This kind of investigation allowed a better estimation of the total output of CO2

58 discharged from the studied volcanic system. (Inguaggiato et al., 2012;Aiuppa et al., 2005; Chiodini

59 et al., 2011).

60 Areas with high CO2 discharges can indicate large and deep pressures in the pores of the system,

61 which allow the identification of high potential seismic regions. In addition, high CO2 emission

62 fluxes can be related to zones of failure or fracture that facilitate the emission of gas from magmatic

63 reservoirs. (Toutain and Baubron, 1999).

64 Among the active volcanoes in Colombia, there are some where the amount of carbon dioxide

65 ejected is significant, as in the case of the Puracé Volcano (4650 m a.s.l.), located in the central

66 mountain, between the departments of Cauca and Huila, 26 km of the city of Popayán (Figure 1).

67 The Puracé volcano is characterized by (1) Solfataric activity with a wide fumarolic field mainly

68 located in the summit crater area with fumarole temperature up to 184°C; (2) Strong soil degassing

69 in the summit and on the flanks of the volcano; (3) several acid thermal springs, with pH down to

70 1.5 and temperature up to 80°C.

71 The aim of this work was carried out the first systematic investigation to estimate the total output of

72 volatiles and energy emitted from the Puracè volcano throughout the fluids discharged by

73 fumaroles, hot springs and soils. Moreover, the realization of a soil CO2-degassing map, which is

74 useful to identify anomalous degassing areas and suitable sites for installation of new geochemical

75 monitoring systems to evaluate the level of volcanic activity.

76 To reach this aim, a geochemical survey to measure the soil CO2 fluxes was performed in

77 September 2016 covering the whole surface of Puracè Volcano. Particular attention was paid to the

78 summit of the active crater and to the flank areas close to San Juan, Pozo Azul y Piñuelas thermal

79 springs. In order to obtain a complete picture of carbon output, fumarolic gases and thermal well

80 waters were also sampled and analyzed.

 81

82 2. Geological Setting

83 The Puracé Volcano, one of the most active volcanoes in Colombia, is located in the extreme north-

84 west of the Coconucos volcanic chain, located in the Central Cordillera of Colombia (Fig. 1), on the

85 border of the Departments of Cauca and Huila, at the coordinates (2 ° 19 '01 "and -76 ° 23' 53" m,

86 4630 masl). It is located 27 km south-east of the city of Popayán (Cauca). The most important

87 populations near the volcano are: The indigenous reserves of Puracé and Coconuco, located 9.5 and

88 11.5 km, respectively, to the north-west and Paletará to 16 km to the southwest; these populations

89 are part of the municipality of Puracé.

90 Its building is in the form of a truncated cone with slopes of 30 ° inclination, has an inner and an

91 outer crater, concentric of 500 and 900 m in diameter respectively. The fumarolic activity is

92 concentrated in the interior of the crater, mainly in a great crack that crosses the bottom of the same;

93 The Puracé volcanic region (RVP) is aligned following the Coconucos fault line, and is affected by

94 three regional fault systems with north-east main directions. Southwest, northwest-southeast and

95 north-northeast, (Monsalve et al., 1999)

96 Its activity has been reported since 1801 and since 1827 at least 15 well documented historical

97 eruptions have been described. In the last 150 years it has presented/displayed at least 5 important

98 eruptive periods, that have been characterized by being of explosive type, with periods of rest

99 between 10 and 30 years approximately, its last eruptive activity was reported in 1977 which was

100 manifested with Low ash emissions

101
102 3. Volcanological activity

103 The volcanic chain of the Coconucos (CVLC) (Monsalve & Pulgarín, 1999), of which the Puracé

104 Volcano forms part, is an alignment of several volcanoes in NW-SE direction, whose tendency is

105 almost perpendicular to that of the Colombian mountain ranges The regional tectonic structures

106 (NE-SW), which constitutes a specific case of exception with respect to the parallelism approach
107 that exists between the rows of volcanoes in the mountain ranges and the compressive limit. Hall &

108 Wood (1985), recognize in the regional tectonic context, a predominant NW-SE direction that

109 delimits the distribution of volcanism in Colombia and Ecuador; According to these authors, the

110 Puracé Volcano marks the northern limit of the southern volcanism of Colombia.

111 The Puracé Volcano is built at the junction of the Fallas Moras and Coconucos, along which is

112 aligned the volcanic chain of Los Coconucos. Its evolutionary history is linked to previous volcanic

113 buildings (Pre Puracé and Chagartón) that have been interpreted as resurgent volcanism of the

114 Caldera de Paletará. The present Puracé volcano (VPA) represents the most recent period of activity

115 of the Puracé Volcano; Is constructed inside the remnant of the Pre-Puracé Volcano and is

116 characterized by being a stratum volcano that has generated lava flows and pyroclastic products of

117 deposits of Piroclastic Density Currents (CDP), as well as of fall, associated with eruptions of the

118 groundwater type, Phreatomagmatic and, mainly, Strombolian - Vulcanian. The geological record

119 of this activity is represented by hydrothermal deposits and by deposits of both dilute CDP

120 (pyroclastic waves) and concentrated CDP (slag flows, block flows), ash fall, lapilli and bombs and

121 blocks emitted as ballistic projectiles. For VPA there is a historical report of its activity since the

122 sixteenth century, and has been better documented since the nineteenth century, describing eruptive

123 events that have caused both loss of life and materials, due to its explosive nature.

124 From the regional point of view, the area is geologically very complex due to the variety of outlying

125 littoral units and the presence of a dense network of geological faults, most of them considered to be

126 active, which have played an important role in the geological evolution of this part of The

127 Cordillera Central (Orrego & Acevedo, 1999).

128

129 4. Materials and methods:

130 A geochemical survey to sampling the main fluids discharged from the Puracè volcano was carried

131 out by 2016, sampling (i) 10 thermal springs to analyze their chemical and isotopic composition, (ii)

132 the higher temperature fumarole located in the summit fumarolic area (P1), and (iii) soil CO2
133 degassing measurements, with 512 point of measurements over the whole volcanic area of Puracè

134 performed utilizing the accumulation chamber method (Chiodini et al. 1998) by West systems

135 equipment. Moreover, (iv) the SO2 flux of the Puracè "plume" was measured by the UV-scanning

136 DOAS system installed on the north-side flank of Puracè volcano in the framework of NOVAC

137 project (Fig.2).

138 The gases emitted at P1 fumarole were sampled by inserting a pipe 50 cm into the fumarole and

139 connecting this pipe via a Dewar tube to a Giggenbach bottle filled with 4 M NaOH solution

140 (Giggenbach, 1975). The CO2 content of the solution was analyzed by potentiometric titration, and

141 for Stot, HCl, and HF according to the method described by Sortino et al. (1991).

142 The thermal springs waters was sampled in several polyethylene bottles to allow its major

143 components and its stable isotopes compositions (18O and D) to be analyzed. The samples for

144 cations were filtered and acidified with suprapure HNO3. Alkalinity was determined in situ by

145 titration with 0.1 N HCl, whereas major elements were analyzed in the laboratory using a double

146 ion chromatograph (Dionex-Thermo ICS 1100) at an accuracy of ±2%. A column (Dionex CS-12A)

147 with a conductivity suppressor (CSRS 300) was used for the cations (Li, Na, K, Mg, and Ca), while

148 a column (Dionex AS14A-SC) with conductivity suppressor (ASRS 300), were used for the anions

149 (F, Cl, Br, and SO4). The water dissolved CO2 was determined utilizing the sampling and analytical

150 methodology proposed by Capasso and Inguaggiato, 1998.

151 The sampled gases (from the P1 fumarole, and those dissolved in the waters) were analyzed using a

152 gas chromatograph (Perkin Elmer Clarus 500) equipped with a double detector (thermal

153 conductivity detector [TCD] and a flame ionization detector [FID] with a methanizer) using Ar as

154 the carrier gas and a 3-m packed column (Restek Shincarbon ST). He, H2, O2, N2, and CO2 were

155 measured using a TCD detector, while CH4 and CO were determined using an FID detector coupled

156 to a methanizer.
157 The abundance and isotopic composition of He as well the 4He/20Ne ratios were determined by

158 separately admitting He and Ne into a split flight tube mass spectrometer (Helix SFT). The

159 measured elemental and isotopic abundances of He were calibrated using the atmospheric standard.

160 The analytical error of the He isotope analysis was less than 0.3%. The 3He/4He ratios were

161 corrected for the atmospheric contamination on the basis of their 4He/20Ne ratios (Sano and Wakita,

162 1985), and are reported as R/Ra values (where Ra is equal to 1.3910–6). C isotopic values are

163 expressed in  vs PDB, with an accuracy of 0.2‰. The O and H isotopic compositions of the water

164 samples were determined using an Analytical Precision AP 2003 device and Thermo Finnigan Xp

165 Plus IRMS interface to TC/EA, respectively. The outlet temperature, electrical conductivity, and pH

166 of the waters at were measured every spring site using a conductimeter (ORION 250A+), a

167 thermometer, and a pH meter (ORION 250A+), respectively.

168

169 5. Geochemistry of fumarole, plume and thermal springs:

170 5.1 Fumarole: The crater area is characterized by a fumarolic field with temperatures ranging from

171 100° to 184°C located in the northern side of the summit area. The chemical composition of the

172 higher temperature fumarole (P1, 184°C) showed H2O and CO2 content respectively around 94 and

173 5% vol (Tab. 1). Moreover, the fumaroles gas show high SO2 dominant composition for the sulphur

174 species with SO2/H2S ratio around 15, and a CO2/SO2 ratio around 5 (Tab. 1). The helium isotope

175 composition of P1 fumarole give a clear magmatic origin for this gas with R/Racorr value around 6.1

176 (Tab. 2) similar to San Juan bubbling gases (R/Racorr=6.6; Sturchio et al. 1993) and Cerro Machin

177 volcano fumarole (R/Racorr=5.9; Inguaggiato et al., 2016a) located on the Colombian Ande chain

178 close to Puracè volcano. Plotting the helium isotope value vs the log C/3He (fig. 3a) together with

179 the value of the MORB, Arc Volcanism and Sedimentary fields, the Puracè fumarole and San Juan

180 bubbling gases showed log C/3He in the range of magmatic values ranging between 9 to 10. Similar
181 magmatic origin indication arrive from the 13CCO2 values of 7.5 and 8.8  vs PDB respectively for

182 P1 and San Juan (fig. 3b).

183 5.2 Plume: The plume SO2 flux was measured by the continuous UV-scanning DOAS system

184 installed, in the framework of the NOVAC European Project, in the flank of Puracé volcano in the

185 Vinagre zone (Fig. 2). The SO2 fluxes recorded showed values ranging from 20 to 1800 t/day. The

186 normal probability plot of plume SO2 flux was utilized to assess the anomaly threshold of a

187 different degassing families. The entire dataset of 3741 measurements points of SO 2 flux show a

188 bimodal distribution (Fig. 4a), with two lognormal population, named A and B, representing

189 respectively 20 and 79 % of data (Fig. 4b). The family A is characterized by an average value of 30

190 t/day, while the family B have an average value of 162 tons/day. Moreover, 1% of data are

191 characterized by higher SO2 flux with an average value around 1580 tons/day (Fig. 4b).

192 On the basis of the individuated degassing families A,B, and C characterized respectively by 20, 79

193 and 1% of degassing percentage, a weighted average of SO2 flux value of 208 t/day was estimated.

194 5.3 Thermal springs: The sampled thermal springs (23.4 to 86.4 °C) showed very acidic pH values

195 from down to 1.5 with salinity ranging from 1.8 to 11.6 mS/cm. The chemical composition of

196 major elements (Tab. 3) show three group of waters: (i) Cl-SO4 alkaline, (ii) Cl-SO4 Earth-alkaline,

197 (iii) Carbon Earth-alkaline (Fig 5a,b). The higher content of SO4 coupled with the strong acidity of

198 many springs suggest a process of direct input of magmatic gases with the aquifer (steam heated

199 waters).

200 6. CO2 Output

201 To evaluate the total output of CO2 emitted from the Puracè volcano a systematic investigation of

202 the different shallow fluids emission of this volcano was studied to analyze the CO 2 in all the

203 showed main different carbon species. In particular, we measured the CO2 discharged by (a)

204 fumaroles, (b) soil degassing, (c) water dissolved carbon species (CO2 and HCO3). Different
205 methodology procedures of sampling, analysis and measurements was utilized to determine the CO2

206 amount and their fluxes. Descriptions of methodologies are given in the following sections.

207 6.1 Crater area CO2 fumarole degassing

208 The estimation of the CO2 flux emitted from the solfataric area was made by the indirect method

209 proposed and utilized by Inguaggiato et al., 2011, 2012, 2013, that is based on the plume SO2 flux

210 and fumarolic CO2/SO2 ratio.

211 Coupling the information of weighted average value of SO2 flux (208 t/day, Tab. 1) estimated by

212 UV scanning DOAS measurements, and the CO2/SO2 weight ratio (3.2) calculated from the

213 chemical composition of the main high temperature fumarole, the estimation of the "Plume" CO2

214 flux was carried out by the following relation:

215 CO2 Farea SO2 Plume * (CO2/SO2)fumarole (1)

216 where CO2 Farea is the flux of CO2 evaluated for the crater plume, SO2 Plume is the SO2 flux of the

217 plume, and (CO2/SO2) fumarole is the weight ratio of (CO2/SO2) in the fumarole. The CO2 flux

218 released from the fumarolic area resulted in about 673 t/day.

219 6.2 Soil CO2 degassing

220 Soil diffuse CO2 flux output, measured utilizing the accumulation chamber method (Chiodini et al.

221 1988) (West system equipment), have been carried out on the basis of 512 CO2 flux measurements

222 performed in different areas over the Puracé volcano edifice (Fig. 6). In figure 2 the location of the

223 main measurement degassing areas have been reported (4 areas). The density of measurements

224 points for a single area is reported in table 4.

225 The probability plot of the considered 512 data (Fig 7) shows three populations named A, B, and C.

226 On the basis of the Sinclair (1974) technique, mean log flux CO2 values of 4.59, 1.71 and -0.34,

227 and relative proportion of 3.5, 56.6 and 40 %, were computed for populations A, B and C
228 respectively. The mean flux CO2 and the 95 % confidence interval of the mean (David, 1977) are

229 for population A 398,771 g/m2/d (156,231-2,124,175 g/m2/d), for population B 226 g/m2/d (358-

230 162 g/m2/d) and for population C 0.8 g/m2/d (1.2-0.5 g/m2/d).

231 6.2.1 Summit crater area

232 The measured CO2 fluxes in randomly distributed points on the Crater surface were interpolated

233 by a distribution over a grid of 8x8 m2 covering an area of 90,300 m2 using so-called exponential

234 variogram model. Then, 100 simulations of the CO2 fluxes with the obtained distribution were

235 performed (Fig 8). For each simulation, the CO2 flux estimated at each cell is multiplied by 64 m2

236 and added to the other CO2 fluxes estimated at the other cells of the grid to have a total CO2 output

237 for the simulation. The mean of the 100 total simulated CO2 outputs, 25 t/d, represents the

238 estimation of the total CO2 output from the Crater area with a standard deviation of 3.9 t/d.

239 6.2.2 Slope crater area

240 The measured CO2 fluxes in randomly distributed points on the track surface were interpolated by a

241 distribution over a grid of 36x36 m2 covering an area of 915,000 m2 using so-called exponential

242 variogram model. Then, 100 simulations of the CO2 fluxes with the obtained distribution were

243 performed (Fig 9). For each simulation, the CO2 flux estimated at each cell is multiplied by 1444 m2

244 and added to the other CO2 fluxes estimated at the other cells of the grid to have a total CO2 output

245 for the simulation. The mean of the 100 total simulated CO2 outputs, 9.1 t/d, represents the

246 estimation of the total CO2 output from the Subida area with a standard deviation of 0.48 t/d.

247 6.2.3 Piñuelas area

248 The measured CO2 fluxes in randomly distributed points on the track surface were interpolated by

249 a distribution over a grid of 1x1 m2 covering an area of 38,000 m2 using so-called exponential

250 variogram model. Then, 100 simulations of the CO2 fluxes with the obtained distribution were

251 performed (Fig 10). For each simulation, the CO2 flux estimated at each cell is multiplied by 1 m2
252 and added to the other CO2 fluxes estimated at the other cells of the grid to have a total CO2 output

253 for the simulation. The mean of the 100 total simulated CO2 outputs, 0.03 t/d, represents the

254 estimation of the total CO2 output from the Pinuelas area with a standard deviation of 0.00097 t/d.

255 6.2.4 San Juan area

256 The measured CO2 fluxes in randomly distributed points on the track surface were interpolated by

257 a distribution over a grid of 6x6 m2 covering an area of 17,600 m2 using so-called exponential

258 variogram model. Then, 100 simulations of the CO2 fluxes with the obtained distribution were

259 performed (Fig 11). For each simulation, the CO2 flux estimated at each cell is multiplied by 36 m 2

260 and added to the other CO2 fluxes estimated at the other cells of the grid to have a total CO2 output

261 for the simulation. The mean of the 100 total simulated CO2 outputs, 813 t/d, represents the

262 estimation of the total CO2 output from the San Juan area with a standard deviation of 227 t/d.

263 6.3 Water dissolved gases discharged from thermal and cold springs

264 The estimation of the total dissolved carbon discharged by the aquifers linked the Puracè was

265 carried out considering the total amount of CO2 and bicarbonate dissolved in the cold and thermal

266 springs outflow on the flanks of the volcano and their relative water discharge by the following

267 equation (Inguaggiato et. al.,2012):

268 CO2 aquifer i water * (CO2 + HCO3)ispring (2)

269 where CO2 aquifer represent the total amount of carbon of aquifer expressed in CO2, water

270 represent the total discharge of the single spring, and (CO2 + HCO3)ispring represent the total

271 dissolve carbon of the single spring, i represent the sum of the single spring contribution.

272 The 10 thermal springs collected on the Puracè flanks area are characterized by dissolved total

273 carbon ranging from 28 to 1100 mg/l and a flow discharge ranging from 0.5 to 403 l/s (Tab. 3). On

274 the basis of this data input and the equation (1) a total value of 13.7 t/day of discharged CO2 was

275 estimated.
276 7. Discussion and conclusions

277 A total CO2 output of around 1550 t/day was estimated for the Purace Volcano, taking in account

278 the discharged fluids from the crater fumaroles, soil degassing over the whole volcano edifice, and

279 dissolved gases in the aquifer. The summit area contribute, for less of 50% of the whole CO2

280 degassing with around 700 t/day (673 t/day from the plume and 25 t/day from the soil crater

281 degassing). The soil gas emission from peripheral areas contribute for about 837 t/day more of 50%

282 of the whole CO2 degassing and more of one order of magnitude respect to the CO2 discharged

283 from the aquifer. These higher values of peripheral soil CO2 discharging (San Juan) respect to the

284 aquifer, reflect the high flux of deep degassing fluids that acidify the aquifers moving the pH down

285 to 1.5 (Tab. 3) and making it saturated respect to the CO2 dissolved. Therefore, any further

286 dissolution of this gas is greatly lowered or negligible allowing to the deep CO 2 to flow through the

287 aquifer without significant interaction (Giammanco et al., 1998, Inguaggiato et al., 2005;

288 Inguaggiato et al., 2016b). The isotopic composition of San Juan volatile degassing confirm it and

289 indicate the clear magmatic origin of CO2 and He characterized respectively by -8.5 13C vs PDB

290 and 6.1 R/Ra (Sturchio et al., 1993) very close to the isotopic composition of the main fumarole of

291 Puracè crater area (Figg. 3,4).

292 On the basis of all the different contributions to deep CO2 degassing from the Puracè volcano, we

293 improved the degassing system model of Puracè and compared the total CO2 output estimated

294 with other volcanic system of the worlds (Fig. 12). The estimated value of Puracè (1,550 t/day) is in

295 the same order of magnitude as other quiescent volcanoes, like Pantelleria (1,071 t/day), Ischia

296 (1,313 t/day). While, it is very interesting to observe that the degassing proportion of peripheral

297 and summit degassing is close to 1 (Fig. 13), reflecting degassing processes style between closed

298 volcano systems with solphataric activity (like Ischia and Pantelleria), and open volcano systems

299 (like Stromboli, Popocatepetl, and Etna).

300 On the basis of the measured SO2 flux and the total chemical composition of the main crater

301 fumarole of Puracè, the flux of the other chemical parameters have been estimated utilizing the

302 same approach of equation (2) and reported in table 5. In particular, the flux of water vapor was

303 estimated around 5400 t/day, HCl and H2S fluxes around 15 and 7.7 t/day respectively. The fluxes

304 of the incondensable gases CO, CH4 and He have been estimated around 10-4 t/day.

305 Taking in account the estimated amount of vapor out-gassing from the fumarolic area, the energy

306 released from the Puracè volcano was computed. Considering the water flux of 5430 t/day and the

307 only latent heat of evaporation of water (2500 Kj/kg), a value of energy of 1.36*1010 Kj/day (157

308 MW) was estimated. If we consider also the CO2 soil degassing in the summit area outside of the

309 fumarolic field (25 t/day), on the basis of the same H2O/CO2 ratio of fumaroles, a water flux of 201

310 t/day could be estimated with an associate energy of 5.04*108 Kj/day (5.9 MW).

311 Acknowledgement

312 The field campaigns carried out during this study were funded by the SGC (Servicio Geologico

313 Colombiano). Chemical analysis were performed by SGC laboratories, while the isotopes analysis

314 were possible thanks to Geochemical Laboratories of INGV Palermo.

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403 Figure and table captions:

404 Figure 1: Puracè volcano map and the volcanic chain of Coconucos.

405 Figure 2: Location of sampled thermal springs, blue circles; Crater fumarole (P1) yellow square;
406 UV Scanning DOAS (Vinagre) pink triangle.

407 Figure 3: a) Log C/3He vs R/Ra. The signature fields value of MORB, Arc volcanism and
408 Continental crust have been added for reference; b) Log C/3He vs 13CCO2. The signature fields
409 value of MORB, Sedimentary and Limestone have been added for reference. San Juan sample data
410 is from Sturchio et al. 1993.

411 Figure 4: a) histogram of SO2 plume flux data; b) Cumulated probability of SO2 plume flux data.
412 Three families have been individuate: Family A, B and C respectively 30, 162, and 1580 t/day and
413 with a percentage of occurrence of 20, 79 and 1%. The estimated SO2 weighted average flux is 208
414 t/day.
415 Figure 5: a) Langelier diagram plotting the thermal water samples data. The data samples fall in
416 three fields: (i) Cl-SO4 alkaline, (ii) Cl-SO4 Earth-alkaline, (iii) Carbon Earth-alkaline; b) The
417 triangular diagram Total Carbon, Cl and SO4 showing high SO4/Cl proportion of thermal wells with
418 lower amount of dissolved total carbon. Only one sample Versalles fall close to the Carbon vertex.

419 Figure 6: Purace volcano map with the 4 areas of degassing CO2 measurements. Pozzo Azul, San
420 Juan, Piñuelas, and Summit (crater and slope crater) areas.

421 Figure 7: The histogram (a) and the probability plot (b) of the considered 512 soil measurements
422 data showing three populations named A, B, and C.

423 Figure 8: Soil CO2 degassing map of the crater area.

424 Figure 9: Soil CO2 degassing map of the slope crater area.

425 Figure 10: Soil CO2 degassing map of the Piñuelas area.

426 Figure 11: Soil CO2 degassing map of the San Juan area.

427 Figure 12: 1,550 t/day of total CO2 output of the Puracè volcano compared with the total CO2
428 output estimated with other volcanic system of the worlds.

429 Figure 13: Peripheral vs Summit degassing of CO2 of Puracè volcano (closed system with
430 solphataric activity). The data have been compared with other closed and open volcanic systems.

431 Table 1: Chemical composition of high temperature fumarole (P1) of Purace' crater area. The data
432 are expressed both in vol% and wt%.

433 Table 2: Isotope composition of high temperature fumarole (P1) of Purace' crater area.

434 Table 3: Chemical composition of sampled thermal well located on the flanks of Puracè volcano.
435 The CO2 flux discharged by the aquifer have been estimated on the basis of the total dissolved
436 carbon (HCO3 and CO2) and by the measured water flow for any single spring.

437 Table 4: Summary of the soil CO2 flux measurements with the estimation of the Total CO2 output
438 for single area.

439 Table 5: Computed volatile fluxes of Puracè "plume" on the basis of SO2 flux and chemical
440 composition of fumarole expressed in wt% (Tab.3).
Figure 1
Figure 1: Puracè volcano map.

Figure 1: Puracè volcano map and the volcanic chain of Coconucos.

Figure 2

Figure 2: Location of sampled thermal springs, blue circles; Crater fumarole (P1) yellow square; UV Scanning DOAS (Vinagre) pink triangle.
Figure 3

10.0 14.0

9.0 MORB
Arc Volcanism a) S Purace' L
b)
8.0

7.0
12.0 Cerro Machin
San Juan
6.0

LogC/3He
Puracè
R/Ra

Cerro Machin
5.0

4.0
10.0
3.0 San Juan Puracè

2.0 M
1.0 Continental crust

0.0 8.0
6 7 8 9 10 11 12 13 14 -40 -30 -20 -10 0 10

LogC/3He d13CCO2

Figure 3a
Figure 4

Puracè
a) b)
350 3.5
2.21= 162 ton/day C
300
3.0

250 3.2= 1580 ton/day

2.5

Log SO2 Flux

1.45= 30 ton/day
200 B
Count

2.0

150
1.5
100

1.0
50
A
0.5
0 0.1 1 10 30 50 70 90 99 99.9
1.0 1.5 2.0 2.5 3.0
Cumulated Probability
Log SO2 Flux

Figure 4: a) histogram of SO2 plume flux data; b) Cumulated probability of SO2 plume flux data. Three families
have been individuate: Family A, B and C respectively 30, 162, and 1580 t/day and with a percentage of occurrence
of 20, 79 and 1%. The estimated SO2 weighted average flux is 208 t/day.
Figure 5

Figure 5: a) Langelier diagram plotting the thermal water samples data. The data samples fall in three fields: (i) Cl-SO4 alkaline, (ii) Cl-
SO4 Earth-alkaline, (iii) Carbon Earth-alkaline. The triangular diagram Total Carbon, Cl and SO4 showing high SO4/Cl proportion of
thermal wells with lower amount of dissolved total carbon. Only one sample Versalles fall close to the Carbon vertex.
Figure 6

Figure 6: Purace volcano map with the 4 areas of degassing CO2 measurements. Pozzo Azul, San Juan, Pinuelas, and Summit
(crater and slope crater) areas.
Figure 7

The probability plot of the considered

512 data (Figure 1) shows three
populations named A, B, and C. On the
basis of the Sinclair (1974) technique,
mean log flux CO2 values of 4.59, 1.71
and -0.34, and relative proportion of 3.5,
56.6 and 40 %, were computed for
populations A, B and C respectively. The
mean flux CO2 and the 95 % confidence
interval of the mean (David, 1977) are
for population A 398,771 g/m2/d
(156,231-2,124,175 g/m2/d), for
population B 226 g/m2/d (358-162
g/m2/d) and for population C 0.8
g/m2/d (1.2-0.5 g/m2/d).

Figure 7: The histogram (a) and the probability plot (b) of the considered 512 soil measurements data showing three populations
named A, B, and C.
Figure 8

Figure 8: Soil CO2 degassing map of the crater area.

Figure 9

Figure 9: Soil CO2 degassing map of the slope crater area.

Figure 10

Figure 10: Soil CO2 degassing map of the Pinuelas area.

Figure 11

Figure 11: Soil CO2 degassing map of the San Juan area.
Figure 12

100000

Total degassing of CO2 from the Purace Volcano 1549 t/day

10000
CO2 flux t d-1

1000

100

10

Figure 12: 1,550 t/day of total CO2 output of the Puracè volcano compared with the total CO2 output estimated with other
volcanic system of the worlds.
Figure 13

1.E+05

CO2 Peripheral degassing t/day

1.E+04 Etna

Popocatepetl
Puracè
Ischia
Ischia
1.E+03
Pantelleria
Pantelleria

1.E+02

Vulcano
Vulcano
Stromboli
Stromboli
1.E+01

CO2 Summit degassing t/day

1.E+00
1.E+00 1.E+01 1.E+02 1.E+03 1.E+04 1.E+05

Figure 13: Peripheral vs Summit degassing of CO2 of Puracè volcano (closed system with solphataric
activity). The data have been compared with other closed and open volcanic systems.
Table 1

vol% wt%
T°C 182.4 182.4
H2O 93.9 85.33577
CO2 4.76 10.57432
HCl 0.13 0.239568
H2S 0.07 0.120163
SO2 1.01 3.263581
He 6.70E-05 1.35E-05
H2 5.80E-04 5.86E-07
CO 1.23E-06 1.74E-06
CH4 4.20E-06 3.39E-06
N2 3.30E-01 4.7E-01

Table 1: Chemical composition of high temperature fumarole (P1) of Purace' crater area.
The data are expressed both in vol% and wt%.
Table 2

40
Ar/36Ar d 15N N2/36Ar N2/Ar d 15Ncorr He/Ne R/Ra R/Racorr dD d 18O d 13CCO2 log C/3He
294.6 -0.3 26366.7 89.5 -0.5 14.5 6.0 6.1 -54.5 -0.6 -7.5 12.8

Table 2: Isotope composition of high temperature fumarole (P1) of Purace' crater area.
Table 3

SAMPLE Data pH T Cond. Li Na K Mg Ca Cl SO4 HCO3 CO2 dis SiO2 F Water F CO2
°C mS/cm mg/l mg/l mg/l mg/l mg/l mg/l mg/l mg/l mg/l mg/l l/s t/day

LA MINA 15/05/2014 1.52 45.1 9.5 0.2 295 67.0 260.0 335 1246 3526 117 144 2 0.02
A. Hirviendo 15/05/2014 6.57 73.1 11.6 6.4 2280 212.0 36.0 152 1600 2223 1055 45 151 1 0.09
AGUA TIBIA 15/05/2014 6.27 54.1 8.2 3.8 2080 63.3 9.8 96 1319 1051 988 85 138 9 0.82
POZO AZUL 2 13/05/2014 1.67 86.4 4.7 <0.1 21 2.2 20.2 16 64 458 21 317 15 0.03
SAN JUAN 9 14/05/2014 4.63 34.6 1.8 <0.1 64 8.7 66.0 350 74 1007 49 169 136 403 7.57
HORNOS 3 13/05/2014 3.52 80.0 3.9 1.8 715 93.5 6.4 40 517 619 34 321 0.5 0.00
HORNOS 7 13/05/2014 3.50 78.1 4.0 1.9 615 100.0 7.5 44 534 639 31 34 334 0.5 0.00
GUARQUELLO 15/05/2014 2.17 23.4 2.9 0.2 42 20.0 36.0 44 239 519 28 123 2 0.01
VERSALLES 14/05/2014 6.19 34.7 2.1 0.8 335 23.4 42.0 90 199 176 781 53 152 71 5.11
PULULO 15/05/2014 2.01 26.9 2.2 0.2 120 22.1 108.0 112 341 829 37 129 12 0.04

Total F CO2 13.68

Table 3: Chemical composition of sampled thermal well located on the flanks of Puracè volcano. The CO2 flux
discharged by the aquifer have been estimated on the basis of the total dissolved carbon (HCO3 and CO2) and by
the measured water flow for any single spring.
Table 4

Total
Number Mean CO2
Area Standard CO2 Standard
Study Area of 2 flux
(m ) 2 Deviation output Deviation
samples (g/m /d)
(t/d)

Summit 253 90300 279 43.3 25.22 3.91

Subida 167 195000 46 2.5 9.06 0.48

Pinuelas 59 38000 0.8 0.03 0.03 0.00097

Pozo Azul 8 160 96125 33965 15.4 5.4

San Juan 27 17600 46136 12898 812 227

Table 4: Summary of the soil CO2 flux measurements with the estimation of the Total CO2 output for single area.
Table 5

t day-1
H2O 5,434
CO2 673
HCl 15
H2S 7.7
SO2 208
He 8.6E-04
H2 3.7E-05
CO 1.1E-04
CH4 2.2E-04
N2 3.0E+01

Table 5: Computed volatile fluxes of Puracè "plume" on the basis of SO2 flux and
chemical composituion of fumarole expressed in wt% (Tab.3).