Radon determination in ground water
Transcription
Radon determination in ground water
Revista Mexicana de Física 38, Suplemento 1 (1992) 242-248 Radon determination in ground water N. SEGOVIA AND S. BULBULIAN Instituto Nacional de Investigaciones Nucleares Apartado postal 18-1027, 11801 México, D.F., México Recibido el 15 de agosto de 1991; aceplado el 29 de abril de 1992 ABSTRACT. In this paper a review of environmental radioactivity studies in groundwater from a11uvial and volcanic aquifers in Mexico is presented. Thc water samples were taken from wells and springs in San Luis Potosi, Mexico, and Michoacan states in Mexico. 222Rn was extracted from lhe samples wilh pure loluene and radiaclivily measured wilh lhe Iiquid scinlillalion lechnique. Results indicate a low radon content confirming that water samples from alluvial and basaltic rocks have in general low radon levels. RESUMEN. En este trabajo se presenta una revisión de los estudios sobre la radiactividad natural realizados en algunas muestras de agua de pozos y manantiales ubicados en los Estados de San Luis Potosí, México y Michoacán, México. Todas las muestras estudiadas provienen de acuíferos ya sea aluviales o de origen volcánico. El radón (222Rn) de las muestras se extrajo con tolueno puro y se midió por la técnica de centelleo líquido. Se encontró que estas muestras tenían un contenido muy bajo de radón lo cual confirma que las muestras provenientes de acuíferos aluviales o volcánicos basálticos contienen muy baja concentración de radón. PAes: 89.60.+x INTRODUCTION The groundwater 222Rn source is the decay of 226Ra within the solid matrix of an aquifer and exhaled from 226Ra dissolved in the water. 226Ra, with a half Jife of 1 600 years, supplies a continuous source of 222Rn to the fluid in the pores of the matrix. I3eing chemically inert, radon incorporates into ground water systems via molecular diffusion. Ground water flow is then the dominant mechanism by which radon is transported; the Iimiting factor in the transport length being its half-Iife. In areas where surface waters infi¡trate to aquifer, radon may be used as a tracer for qualitative investigatious. The natural radiactivity of ground water varies markedly from site to site. In general, granite areas and those where pegmatites are abundant, seem to favor e¡evated levels of 222Rn and other natural radionuclides in ground water. On the other hand, 222Rn concentration could be mueh lower in aquifers imbedded in alluvial deposits and basaltic rocks [1,2,31 when the uranium content is low. l!owever, given a site, the actual situation may tUfO out to be quite different. As a mattef of fact, in the case of 222Rn al least, the concentration depends not only on that of its progenitor but also on the degree of fracturation of the rocks and on the percolation time of the water. The rnaxilllum 222Rn content is achieved when the velocity of the percolating water is low enough so that it can pick-up as much 222Rn as possible, but not too slow so that 222!ln does not have euough time to decay in large amounts [41. RADONDETERMINATION IN GROUNDWATER 243 FIGURE 1. Sampling Locations in San Luis Potosi State. Studies on natural radioactivity in ground water were started in Mexico in San Luis Potosi state followed by samplings from deep wells and springs in the states of Mexico and Michoacán [5,6,71. In this paper sorne of the radon concentration levels found, as analysed by the radon extraction in toluene method, are reviewed. SITES DESCRIPTION 1. San Luis Potosi State The water samples were collected from 4 wells in the Villa de Reyes valley and 3 wells in the San Luis Potosi valley, both located in the State of San Luis Potosi, Mexico, approximatelly 400 krn NE of Mexico City (Figure 1). The Villa de Reyes valley is forrned by cernented sandstones, alluvial deposits and volcanic tu!fs. A non confined aguHer is found forrned by clastics and rhyolites. Ground water movernent is non-horizontal; downward movement occurs is the center of the valley where rainfall and water from excess irrigation recharges the aguifer system. On the other hand, the San Luis Potosi valley has a shallow alluvial aguifer and a deep one separated by a clay and clayey sand body located in the middle of the valley [51. 2. Mcxico and Michoacan Sta/es The sampling incllldes 46 wells drilled up to 200 m frorn the City of Toluca, and 6 springs located at the sw part of the sta te. 244 N. SEGOVIAANDS. BULBULlAN ... . . .•."-,. .. -~= ,o ••. FIGURE 2. Sampling Localions in lhe Cily of Toluca. The aquifers of the studied zone in the state of Mexico are found mainly in basaltic racks, particularly around the City of Toluca where igneous racks are found produced by ancient eruptions from Nevado de Toluca volcano [5]. Water samples fram 2 spriugs belonging to lhe geothermal field of Los Azufres in the state of Michoacan have al so been studied. The geothermal field of Los Azufres belollgs to the Solfataras regio n located at the Sierra de San Andres in the Central Part of the Mexican Neovolcanic bel!. The rocks found in the are a are ba,alts. rhyo!ites, dacites and andesites. llydrothermal springs are found in this under exploilation geothermal field [7J. The sampling lacations are indicalecl in Figures 2 and :l. EXPERIMENTAL The samples were analyzed for solubilized and nOHa-supporled also studied for 234U/238U activity ratio. 222Rn. Sorne oflhem were Sampling 222Rn in natural water easily escapes from waler samples, lherefore, the sarnpling has to be done \Vilh gleal careo The \Valer musl rUII steadily in lhe one liler \Vashed and decontarninated container achieved after sampling and wit!Jout any air buhblcs, in arder lo avoid degassing. and pcrff'ct sealing has to be RADONDETERMINATION IN GROUNDWATER ; (;-e.' ,,-... '''. , 245 ,- '-/ , , ,, (4 .••.••.•.• I '" ! ~--t , ,, { FIGURE 3. Springs Sampled in Mexico and MidlOacan States. Finally lhe sample musl he transporled to the laboratory conlenl w¡lhin 24 h from the lime of sampling. Radon determination lo be analysed for 222Rn in the water saml'les Measuremenl of radon and shorl Iived radon daughlers aclivily in water samples was perfomed with a Packard No. 4530 scintillation deteclion system. The toluene extraction melhod reporled by Noguchi and \Vakila [8] was slightly modified in order to measure very low 222Rn conlenl in the water samples. These authors reported the radon extraction from water with a toluene base Iiquid scintillator, obtaining an exlraction efficiency of 80%. \Vilh lhe modificalion used in lhe presenl work, an extraction efficiency of 97% was obtained when using pure loluene lo extracl radon from lhe waler samples. Aliquot.s of 100 mI sample and 10 mi of pure toluene were lransferred lo a separatory funnel and vigorously shaken fol' 2 minules for radon separation. \Vhen lhe mixture reseltled in two phases, the organic phase was lransferred into a counting vial lo which 10 mi of INSTAGEL scintillation solution was added. Samples were counted immediately after radon separation and again about fOUf hours after the first measurerncnt, radioac.tive eqllilibrium with his daughters. Corrections for decay of radon amI decay and growth of the daughter samples \\'ere necessary. upon rcaching products in the 246 N. SEGOVIAANDS. BULBULlAN TABLE 1. Results obtained in San Luis Potosi State [5). U 234U/238U Temperaturc Radon (Bq/l) (I'g/i) SLP 901 507 918 2.18 1.31 1.42 0.56 0.47 0.49 1.72 0.96 1.02 36.5 36.2 36 VR 397 416 398 354 5.26 8.7 3.2 1.21 0.34 0.72 0.32 0.48 1.03 1.09 1.68 1.07 31 28.6 27.8 41.6 Well ('C) Calibration of the collnter w•.., performed with a 226Ra-standard solution from NBS. Systematic countings of selected samples wcre made during several days in order to ascertain that the decay of the extracted nllelide in tolllene corresponded to the 222Rn half-life. Radon supported radium determination 226Ra support of 222Rn was determined in sorne samples from the same water ali'luots from where original 222Rn present in the samples was extracted. Those ali'l"ots were sealed and left for one month in order to reach equilibrium between 226Ra present in water amI 222Rn. Once the time elapsed, 222Rn extraction was performed from the samples in the same way as specified in the previous paragraph. Measurement 01234 Uf38 U activity ratio Uranium was concentrated from twenty-liter water samples by co-precipitation in b•..,ic media. The precipitate was dissolved in 0.1 N HCl solution. Uranium was then purified by the extraction-chromatographic method using di-2-ethylhexylphosphoric acid. Thin foils of U compollnd were prepared for use in o-spectrometry. Alpha-counting was performed IItilizing a sllrface barrier detector collpled to a 1024 channel analyzer. The time of measurement of the activity of the sources ranged from several hOllrs to two days, depending on the intensity of the a-sources. RESULTS ANO OISCUSSION Results of 222Rn, U and 234U j238 U activity ratio as obtained from water samples of seven wells in San Luis Potosi and Villa de Reyes valleys are shown in Table 1. The water temperatllres at sampling time are also indicated in this tableo From these results we can scc that radan solubility in water dccreascs with incrcasillF; temperature. No corrclation wa.sfound bclween radon and uranium conccntration Icvels HADON DETERMINATION IN GROUND WATER 247 " " ,o , . FIGURE 4. Radon Concentration in Water Samples Crom the City oC Toluca [6). in water. This lack of correlation has often been reported in aquifers since radon migration iuto the pore fluid is higher than uranium. The values of the activity ratios obtained, very c10se to equilibrium, together with the low uranium content seem to confirm a rapid water transit from the recharge zone to the sampling site. Radon content for the samples from Villa de Reyes is higher than that of San Luis Potosi by an average factor of 2.8, suggesting a radon enrichment from a flow of more ancient subsurface water into the aquifer of Villa de Reyes. The distribution of 222Rn concentration as found in 46 wells from the City of Toluca is shown in Figure 4. It can be observed that 58% of the sampled wells have less than 2..1 Bq/I; the highest value obtained being 11.3 Bq/l. Those wells with the higher 222Rn concentration were found in regions where local rock composition is mainly andesites and rhyolites. 222Rn supported by 226Ra dissolved in the water samples was below the detecting threshold of the measuring equipment (0.009 Bq/I as reported by Olguin el al. [6]), showing that radon input into the fluids of the aquifer is much higher than that of 226Ra . .Radon content in the water from eight springs in the states of Mexico and Michoacan is shown in Table 2. The spring water samples were taken in the same month (November) as those of the wells of the City of Toluca. CONCLUDING In this papcr, REMARKS uranium and radon rncasurements in sorne ground water samplcs werc reviewed. As it is Iikely, since the embedding rocks of the studied aquifers are of basaltic or sedimentary essence, low levels of radioactive nuclei have beeu found. In addition, the samples were retreived at the eud of the rainy season when the aquifers were undergoing 248 N. SEGOVIA ANO S. BULBULlAN TABLE JI. Radan concentrations in spring water samples from ~lexico and Michoacan states [7]. Radon (Bq/I) Spring Mexico State Las Tazas Tonatico Ix tapan de la Sal Nevado de Toluca Ixtapan del Oro I Ixtapan del Oro Il Michoacan State San Alejo Los Azufres Temperature 0.491 1.518 2.362 0.375 1.037 0.117 17 33 32 16 31 25 1.335 0.25 41 82 (OC) their latest recharging phase. Accordingly, the dilution effect was at its maximum, which also accounts for the presented findings. It" is worth mentioning that the use of pure toluene for radon extraction allowed us to obtain a higher radon extraction yield. ACKNOWLEDGEMENTS The authors are grateful to the technicians of the Chemistry and Nuclear Tracks Departments, ININ; to R. Noriega for linguistic revision. \Ve acknowledge financial support from CONACYT, Mexico. REFERENCES 1. 2. 3. J. Michel and M.J. Jordana, "Nationwide Dislribution oC 228Ra, 226Ra, 222Rn and U in Groundwater", in Radan in Ground Water. B. Graves, ed. Lcwis Publishers Ine., Chelsca, Mi. 227-240 (1988). Z. Szabo and 0.5. Zapecza, ~'Rclation Belween Natural Radionuclidc Activities and Chemical Constituents in Groundwaler in the Newark basin, New Jersey", in lladon in Ground Water. B. Graves, ed., Lewis Publishers Inc., Chelsea, Mi. 283-308 (1988). W.C. Burnell, J.B. Cowart and P.A. Chin, "Polonium in the Surficial Aquifer of West Central Florida" in Radon in Ground Water. B. Graves, ed., Lewis Publishers Inc., Chelsea, Mi. 251-269 (1988). M. Monnin. Private Communication (1992). M.T. Olguin, N. Segovia, J. Carrillo. E. Ordoñez, J.L. !turbe and S. Ilulhulian, "22'Rn Content and 23'U/23.U Activity Ratio in Groundwaters", J. Radioanal. Nud. ChelO. Art. 141 (1990) 17-23. M.T. Olguin, N. Segovia, E. Tamez, M. Alcántara and S. Ilulhulian, Radon Concentrotion Levels in Ground i-Vaterlrom the City 01 Toluca, Ateneo. Sci. Tolo Environ. (in press, 1992). N. Servín, N. Segovia, ~1. A. Armienta, A. Aguayo, N. Ceniceros and F. Juárcz, "Estudio Geoquímico y Emanométrico de Aguas de Manantiales". Informe Técnico IA.9G-25, ININ, México (1990). M. Noguchi and 11. Wakita, "A Method for Continuous Measurernent of Radon in Groundwater for Earthquake Prediction". J. Geophys. Res. 82 (1977) 1353-1357. 1 4. 5. 6. 7. 8.