WASTEWATER REUSE IN VALSEQUILLO AGRICULTURAL AREA, MEXICO: ENVIRONMENTAL IMPACT ON GROUNDWATER

E. DOMNGUEZ-MARIANI, A. CARRILLO-CHVEZ , A. ORTEGA and M. T. OROZCO-ESQUIVEL

Centro de Geociencias-UNAM, Campus Juriquilla, Juriquilla, Quertaro, 76230, Mxico ( authors for correspondence, e-mail: eloisa@geociencias.unam.mx and ambiente@geociencias.unam.mx)

(Received 27 June 2002; accepted 30 December 2003)

Abstract. Wastewater and groundwater has been used for irrigation in the Valsequillo District, east central Mexico, for nearly 50 years. The environmental impact of wastewater on groundwater in the unconned shallow aquifer is evaluated by means of hydrogeological, microbiological, hydrogeochemical and isotopic evidences. The shallow aquifer consists of upper Tertiary volcano-sedimentary rocks with a calcite-rich matrix. Groundwater from wells near the wastewater canal had similar total coliforms concentrations as the wastewater (100 MPN 100 mL1 ). The hydraulic head in near-canal wells had a recovery of 10 m until 1983, indicating shallow recharge from wastewater. A bicarbonate vs. calcium plot shows a well-dened mixing process between wastewater and unaffected groundwater. Stable isotopic data ( D and 18 O) show characteristic signatures for wastewater and non-impacted groundwater, and dene a mixing line between those end-members and groundwater affected by wastewater inltration. Tritium data indicate that non-impacted groundwater is pre-atomic hydrogen bomb (>50 yr), whereas the wastewater has a younger signature. Tritium data from wells inside the district clearly indicate a mixing process between waste and groundwater. These results demonstrate the interaction and hydrochemical processes between wastewater and shallow groundwater at the site. Keywords: groundwater, irrigation, Mexico, mixing processes, reuse water, Tecamachalco, Valsequillo, wastewater

1. Introduction The growing demand of water for agricultural irrigation has produced a marked increase in the reuse of treated and/or untreated industrial wastewater worldwide. The effects of industrial and municipal wastewater on agricultural soils have been widely documented, mostly in relationship with heavy metal concentrations (Fazelli et al., 1991; Boon and Soltanpour, 1992; Rao et al., 1993) and toxicological studies. However, the environmental impact of irrigation wastewater has not been widely investigated. In this paper we present new hydrogeological and hydrogeochemical data, as well as a general description of a conceptual model for the interaction between reused wastewater from the city of Puebla, central Mexico, with the shallow aquifer of Tecamachalco.
Water, Air, and Soil Pollution 155: 251267, 2004. 2004 Kluwer Academic Publishers. Printed in the Netherlands.

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The city of Puebla (1.3 million of inhabitants in 2000, 26% of the state population) is located in a valley on the volcanic highlands of east central Mexico. The estimated industrial growth of 60% for the last 20 yr (INEGI, 2000) in this city is mainly related to its vicinity to Mexico City valley, where growing environmental problems have forced industrial decentralization. In Mexico, industrial and municipal wastewater has been widely used for several years for agriculture. The best known case is the Mezquital basin, north of Mexico City, where 45 m3 s1 of wastewater from Mexico Citys metropolitan area are used for agricultural irrigation (ERNR, AIC and ANI, 1995; Chilton et al., 1996). Similar practices take place at a smaller scale in the nearby cities of Puebla, Cuernavaca, Toluca and Pachuca. The environmental impact of the wastewater reuse at these places has been recently recognized as a major problem that needs a multidisciplinary approach for its evaluation. The purpose of the present work is to evaluate the hydrogeologic and hydrogeochemical interaction between wastewater used in the Valsequillo Irrigation District and groundwater from the shallow aquifer. We also propose a general hydrogeologic-hydrogeochemical conceptual model of this interaction. This work is part of a major research project, designed to analyze the interaction between wastewater from the irrigation canal and groundwater from the shallow aquifer.

2. Site Description and Geologic-Environmental Background The Valsequillo Irrigation District (2000 m a.s.l.) is located on the high plains of central-east Mexico, 30 km southeast from the city of Puebla (Figure 1), in a broad valley (260 km2 ) bordered by two large volcanoes: the Malinche volcano to the northwest, and the Citlaltpetl volcano to the northeast. The stratigraphy of the area (Figure 2) is dominated by Cretaceous reefal limestones, interstratied limestones, shales, sandstones, and ne grained-limestone units (Units A and B in Figure 2). These units constitute a deep aquifer, with few groundwater wells reaching it. This aquifer is conned by a massive, heavily packed, well-consolidated conglomerate of Tertiary age (Unit C, thickness 200 m). Lava ows and volcanic breccias (Unit D), and non-consolidated carbonate-rich volcanoclastic rocks from Late Tertiary and Quaternary (Unit E), constitute the upper 100200 m of the stratigraphic column. The most productive groundwater wells are located in those uppermost volcano-sedimentary units that constitute the shallow aquifer. This aquifer has secondary permeability due to the development of dissolution canals, fractures, and matrix porosity. The Valsequillo Irrigation District, located within the basin of the lower Atoyac River, started the irrigation operations in 1946. Until 1975, the water was supplied mainly by the Valsequillo reservoir, and subsequently was complemented by groundwater from drilled wells (Figure 3). The Valsequillo reservoir supplies 163 m3 yr1 , and additional 55 m3 yr1 are withdrawn from wells for the irriga-

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Figure 1. Generalized map of the Atoyac River in central Puebla State, Mexico (inset), the Valsequillo dam and the Valsequillo Irrigation District. The study is centered on Unit 1 of the irrigation district, east of Tecamachalco (boxed area). The irrigation dam of Valsequillo was built south of the city of Puebla, where the Alseseca River ends in the Atoyac River. Numbers 1 to 7 indicate surface water sampling sites (data from PDRA, 1995).

tion of a total of 33 820 ha. The relative amount of water from the reservoir and from groundwater used in irrigation varies every year, depending on the amount of water accumulated in the reservoir. Since 1960, untreated industrial and municipal sewage water from the city of Puebla has been discharged in minor scale into the Atoyac River, and is nally conducted to the Valsequillo reservoir (Contla, 1976). By 1976, as the dam was at its lowest level, due in part to poor water-use and conservation planning, the induction of a drilling program was necessary (Contla, 1976; SARH, 1973, 1974a, b, 1976, 1979 and 1982a). Since 1976, the size of the surface irrigated has varied every year according to the storage water in the dam and the groundwater extraction. By 1978, the piezometric level has ascended due to the amount of surface water used for irrigation, which was an additional component of shallow recharge. Variations on stable isotope compositions were also noticed (SARH, 1979, 1982b).

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Figure 2. Geologic map of the study area, including values of hydraulic head (m), direction of groundwater ow, and local stratigraphic column (see text for discussion). Localization of sampling sites of irrigation groundwater and surface water is shown in the map. Hydraulic head data from CNA (1995, 1996).

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Figure 3. (A) Evolution of piezometric levels in sites of piezometric observation (SPO) with time. Location of SPO is showed in Figure 1. (B) Evolution of groundwater withdrawal and number of wells. Data from SARH (1974, 1989) and CNA (1996).

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In the early 1980s, formal hydrogeology and hydrogeochemistry studies began being conducted in this area. In 1994, the extension of the irrigation area reached its maximum, in coinciding with the drilling of wells and the extraction volume. In 1984, it was estimated that 30% of the total volume of water in the Valsequillo dam came from industrial and municipal sewage water (Orta-Ledezma, 1985). The water is conducted from the dam to the irrigation district by a surface canal, which is cement-lined in only 42% of its 15 km length. Studies show that considerable loss of water through the unlined canal walls results in inltration to the groundwater system (CNA, 1996). However, no instrumentation has been available at the site to measure the inltration volume of wastewater from the canal.

3. Methods From December 1995 to January 1996, 48 samples of water were collected in the area: 44 from groundwater wells and 4 from canal water. Groundwater samples were taken from productive irrigation wells located inside and outside the district. Water samples were collected for chemical (major and trace elements), isotopic ( D, 18 O and tritium), and microbiological analyses. Temperature, electric conductivity, pH, and alkalinity (acid-base titration to pH = 3.5) were directly measured in the eld. Samples were ltered through 0.45-micron Millipore lters, collected in double acid washed, high-density polypropylene opaque bottles, and conserved at 4 C until they were analyzed. Major dissolved ions and microbiological analyses were done in the Laboratorio de Edafologa Ambiental, Instituto de Geologa, UNAM-Mxico. Isotopic analyses (oxygen and hydrogen stable isotopes) were done at the Laboratorio Universitario de Geoqumica Isotpica (LUGIS), Instituto de Geologa-Instituto de Geofsica, UNAM-Mxico, with the technique of Epstein and Mayeda (1953) for 18 O and the technique of Coleman et al. (1982) for D. Tritium samples were analyzed at the Environmental Isotope Laboratory (EIL), University of Waterloo (Canada), following the method proposed by Taylor (1977).

4. Results and Discussion 4.1. E VOLUTION OF THE PIEZOMETRIC SURFACE Six sites were selected for piezometric observations (SPO1-6, see Figure 2 for location) on the basis of well density, hydraulic head, and location with respect to the wastewater canal. Figure 3A shows a plot of time (years) vs. hydraulic head (m asl) for the six sites of piezometric observations (SPO). Site SPO1 (Figures 2 and 3A) presents the highest increase in hydraulic head with time, most likely because it is located near

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the wastewater canal and have a major inuence from irrigation and inltration. Site SPO6, located on the southest end of the irrigation district, shows no variation in hydraulic head, probably due to lesser inuence from inltration of wastewater. Figure 3A indicates a variation of hydraulic head with time due to local recharge from inltration, and a decline in hydraulic head due to increasing extraction done since 1974. The major recovery occurred during the 19741983 period. After 1983, the increase in groundwater pumping has caused a general decline in hydraulic head. The data of Figure 3A can be summarize as follow: (1) As groundwater extraction started (on early 1970s), the effect of inltration was negligible. (2) During the early 1970s, when mainly dam water and wastewater was used for irrigation, the inltration reached its maximum, causing a rise in hydraulic head. (3) After 1983, irrigation was mainly done with groundwater, causing the declining trend in hydraulic head in all the sites of piezometric observation. From 1983 to 1988, the mean decline in hydraulic head was of 10 m, and between 1988 and 1996 had achieved more than 15 m (Figure 3B shows the increasing number on groundwater wells, and the increase in groundwater withdrawal volume vs. time). An increase in the slope of both curves indicates the increase in groundwater withdrawal after 1985. 4.2. WATER QUALITY VARIATIONS The contaminant load discharged from the Valsequillo reservoir into the canal is, in terms of biologic oxygen demand (BOD5), 1125 mg L1 (Rodrguez-Velasco, 1996). This value is considered a high concentration (averages values of BOD5 are: 110 mg L1 = low; 220 mg L1 = medium; 400 mg L1 = high; Tchbanoglous, 1991). Therefore, due to this high values and the high concentration of dissolved heavy metals and other ions (i.e., Cd, Pb, Cr, Co, As, Fe, Mn, and NO 3) (PDRA, 1995), the canal wastewater is actually not suitable for agricultural use (Orta-Ledezma, 1985; NOM, 1997). The Atoyac River, the main water supply of the Valsequillo dam, collects refuse water from the Puebla municipal discharge. Figure 4A,B and C show the concentration of total and fecal coliforms, specic conductance, and NO3 -N and NH4 -N measured along the Atoyac River. The sampling points are located: before entering to the city of Puebla (sites 1, 2 and 3), between the city and the dam (sites 4 and 5), after the dam (site 6), and in the open unlined canal (site 7). Figure 4A shows a sudden decrease in coliforms bacteria immediately after the Valsequillo dam. The amount of total coliforms is relatively high in the Atoyac River (Figure 4A, sites 1, 2 and 3), and remains high at sites 4 and 5. The values in these sites vary from 1 108 to 1 1010 MPN 100 mL1 . When water ows out of the dam and

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Figure 4. Sections from High Atoyac River to Valsequillo dam in points showed in Figure 1 (see text for discussion). (A) Total and fecal coliforms; (B) Specic conductance; (C) NO3 -N and NH3 -N. Data from PDRA (1995).

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enters the canal, the coliforms decrease to approximately 1 103 MPN 100 mL1 ; we consider that this is the total coliforms value of the canal water inltrating in the groundwater system. The effect of decreasing values after the dam is also observed in the behavior of the specic conductance (amount of total dissolved solids in water, Figure 4B), and NO3 -N and NH4 -N in solution (Figure 4C). This behavior indicates that the Valsequillo dam is acting as a giant open-batch bioreactor, oxidizing the wastewater, and decreasing the amount of coliforms introduced by the municipal discharges. Dilution, precipitation, adsorption, and other similar processes, which take place in the Valsequillo dam, control the hydrogeochemistry of the system and improve the quality of the water. Total coliforms and fecal bacteria were also analyzed in groundwater samples. Figure 5 shows a contour map of the concentration of total coliforms (in MPN 100 mL1 ) in groundwater of the Valsequillo Irrigation District. The highest values of total coliforms in groundwater (1000 MPN 100 mL1 ) are observed on the northwest portion of the irrigation district, and are similar to the average value in the last section of the canal (after water has been in the Valsequillo dam). These high values of total coliforms coincide with the location of site SPO1, which also shows the strongest effect in vertical local recharge and rise of hydraulic head. The coincidence of strong rise in hydraulic head and high total coliforms concentration indicate a high inltration velocity that would favor the preservation of microorganisms in the aquifer. This observation contradicts the conclusion of Orta-Ledezma (1985), who considered that the aquifer would not be affected by irrigation water because of its relative depth and the clayey and silty nature of the aquifer material.

4.3. C ARBONATE AND CALCIUM BEHAVIOR In the northern section of the study area (north of the canal), only groundwater has been used for irrigation and, apparently, no inuence from canal wastewater is observed. Although, the possibility of some local inltration in near-canal areas remains, because no specic studies have been performed in that areas. In this work, we assume that wastewater has no inuence on the groundwater from the northern sector. The unaffected groundwater in the northern section is classied as a bicarbon1 ate type of water, with HCO 3 concentrations ranging between 7 to 11 meq L (Figure 6), and Ca2+ that varies from 9 to 16 meq L1 . On the other hand, the canal water (wastewater), is carbonate-poor water, with concentrations of HCO 3 and Ca2+ ranging between 44.2 meq L1 , and 2.63 meq L1 , respectively. These two types of water can be assumed as end-members of a water mixing system. 2+ in groundwater samples affected Figure 6 shows that values of HCO 3 and Ca by wastewater inltration are located between the values of surface water (canal wastewater) and unaffected groundwater dening a mixing trend.

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Figure 5. Contour map of iso-concentration lines for total coliforms (MPN 100 mL1 ) in groundwater of Valsequillo Irrigation District (see text for discussion). Data from CNA (1995).

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1 Figure 6. Plot of Ca2+ vs. HCO 3 (meq L ) for groundwater and surface water of Valsequillo Irrigation District. The end-members (wastewater and unaffected groundwater) dene a mixing process. Data from CNA (1995).

4.4. S TABLE ISOTOPES The results of isotope analyses in canal wastewater and groundwater are showed in a plot of D ( ) vs. 18 O ( ) (Figure 7A). Groundwater samples from the northern section, with no inuence of wastewater (wells P3, P2Z and P47.3, see Figure 2 for location) plot on the Global Meteoric Water Line (GMWL), and represent the rst end-member in a binary water-mixing process. On the other hand, the isotopic composition of canal wastewater plot away from the GMWL, with higher 18 O and D, this composition is considered as the second end-member of the binary mixing process. The mixing line delineated between these end-members has the expression D = 4.913 18 O 23.054; groundwater samples with inuence from wastewater plot along a mixing line, indicating that they are the result of mixing processes. Figure 7B shows a plot of 3 H (tritium) vs. 18 O( ) only for samples plotting in the mixing line. Groundwater from the northern section, with no canal water inuence, has 3 H values of <0.8 tritium units (TU), which indicates that water is older than 50 yr (pre-hydrogen bomb testing; Clark and Fritz, 1997). For this study we consider those low values as the tritium baseline for the aquifer. On the other

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Figure 7. Isotopic analysis of ground and surface water from Valsequillo Irrigation District. (A) 18 O ( ) vs. D ( ) for all points sampled; (B) Plot of 18 O ( ) vs. 3 H (UT) including samples that plot along the mixing line of Figure 7A. Data from CNA (1995).

hand, groundwater with inuence of canal water (mixing processes, wells P911, P4B, P28 and P111B) show an increase in values of 3 H. Surface water collected in the Valsequillo dam, and eventually conducted through irrigation canals to the district, is dominated by meteoric water from the Atoyac Basin with an important contribution of municipal wastewater from the city of Puebla. Thus, the tritium values in the canal water would indicate relatively young water due to recent precipitation and inltration. This process is indicated by the values showed in Figure 7B, where the groundwater affected by canal water has values ranging between 3 and 7 TU. If the tritium values of affected groundwater are the result of a mixing process, then the canal water should have tritium values lower than 10 TU. Such values would correspond to water ages ranging between the mid 1970s and the mid 1980s. This age agrees with the beginning of the hydraulic head rise (mid-late 1970s), due to wastewater inltration into groundwater (Figure 3A). Therefore, tritium data clearly show the impact of canal water on groundwater from the Valsequillo Irrigation District.

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Figure 8. Schematic cross section of Valsequillo Irrigation District, showing the general hydrostratigraphic units and the sources of wastewater and groundwater used for irrigation. Inset shows the location of the section in Valsequillo Irrigation District.

4.5. C ONCEPTUAL MODEL FOR THE INTERACTION BETWEEN WASTEWASTE

AND GROUNDWATER

Figure 8 shows a schematic representation of the interaction processes between the wastewater from the irrigation canal and the groundwater from the Valsequillo Irrigation District. This scheme indicates the different hydrostratigraphic units of the sub-surface. The uppermost unit (E) represents the main aquifer in the zone, which is composed by a Pleistocene-Quaternary volcano-sedimentary unit of about 100 200 m in thickness. The hydrogeochemical processes taking place in this unit are mixing of wastewater and groundwater, advection, molecular diffusion, dilution, etc. The next unit stratigraphically below is an aquitard in fractured lava ows and volcanic breccias (unit D) of Miocene-Pleistocene age. This unit outcrops in the study area as isolated domes and is covered by unit (E). The extension of unit D in the sub-surface is unknown, but it is probably connected at depth to other igneous bodies forming sub-surface structures of lower hydraulic conductivity. Such struc-

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tures would be acting as an irregular and discontinuous barrier for groundwater lateral ow. The next unit (lettered C) is an aquitard in a heavily packed, well cemented, strongly consolidated conglomerate sequence of possible OligoceneMiocene age. This unit connes the Shallow Aquifer. Most of the drilled wells penetrated just a couple of meters into this unit before stopping. Finally, (lower unit, AB) is a fractured aquifer composed by a sequence of reefal and interstratied limestones, shales and sandstones and a ne grained-limestones from the Upper Aptian to Maastrichian (Upper Cretaceous). Only in the southest extreme of the area few wells are drilled in this unit, which is considered as the Deep Aquifer, separated from the Shallow Aquifer (unit E) by an aquitard (unit C). As mentioned above, we considered that most of the hydro-geochemical processes are taking place on the water table of the shallow aquifer. In the non-saturated zone, the canal wastewater moves down and interacts with the calcareous matrix of the aquifer. When the wastewater reaches the water table, a mixing process begins, diluting the wastewater, which is evidenced by the bicarbonate and calcium concentrations, and the 2 D, 18 O and tritium data. The occurrence of advection and diffusion processes is indicated by the distribution of total coliforms in groundwater. The irregular distribution of the volcanic bodies in the sub-surface (volcanic aquitard) could explain the low tritium and total coliforms concentrations in wells located in this unit, because this unit acts as an irregular lateral barrier.

5. Conclusions Studies of reuse of non-treated wastewater on agriculture have been mostly done regarding the effect upon the environment, including soils, plants and human health. However, studies about its inuence in the chemistry of groundwater are scarce. Therefore, our approach is important for evaluation studies at sites where nontreated wastewater is used for irrigation and the collateral effects are still unknown. The Valsequillo water reservoir has been receiving surface water from the Atoyac and Alseseca rivers, municipal-industrial refuse water from the urban zone of the city of Puebla and from some rural areas from north of Puebla for more than 50 yr. Despite the fact that the Valsequillo dam performs as a big bioreactor, the surface water preserves a high load of contaminants through irrigation canals to the Valsequillo District. The studied area has two aquifers: (1) a Shallow aquifer in a Tertiary-Quaternary deposit, where most of the productive wells are located; and (2) a Deep aquifer in Mesozoic limestones, used in a minor scale in the zone. The Shallow aquifer consists of a volcano-sedimentary deposit with calcareous matrix. Because of its high solubility and additional fracturing, this aquifer has double porosity, which implies fast inltration of wastewater toward the saturated zone. Outside of the irrigation district, only groundwater is used. Therefore, this zone is considered not affected by wastewater. The chemical composition of ground-

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water permits the identication of hydrogeochemical and isotopic baseline data, which is the original composition in the aquifer before the irrigation with wastewater began. Four types of interactions have been identied between groundwater and wastewater: (a) hydrogeological, (b) microbiological, (c) hydrochemical, and (d) isotopic. During the 70s, high volumes of surface water were used for irrigation on high hydraulic conductivity materials, favoring the recovery of water table levels. Therefore, the irrigation is an important component of the groundwater recharge. The response to this articial recharge varied at different points of the irrigational district, e.g., hydraulic head measured between 1975 and 1980 shows an increment of more than 10 m close to the irrigation canal (SPO1, SOP2, SOP3), and of less than 4 m in the southern part of the aquifer (SOP4). The agricultural district is irrigated with 70% wastewater and 30% groundwater from the Shallow Aquifer. In years of low disponibility of surface water, the district uses a higher volume of groundwater. This has caused extensive use of groundwater, leading to a decrease of the piezometric levels. The rates of descent of the groundwater levels depend on different responses of the aquifer to exploitation. These responses correlate with the characteristics of the geologic media and recharge components (inltration from the irrigation canal, from agricultural surface and lateral underground ow). Total coliforms have been detected in groundwater in concentrations that makes it unt for supply of potable water. This fact is directly associated with the mixing with wastewater. The short periods of survival of the microorganisms, like the coliform group, indicate relatively fast inltration through macropores and/or fractures. Plots of calcium (Ca2+ ) and bicarbonate (HCO 3 ) concentrations show two welldened end members. Surface water has lower concentrations for both ions, while the baseline (unpolluted groundwater) data has higher concentrations. Evidence of inltration and mixing of wastewater with groundwater is clear in these plots. Stable isotopic data ( D and 18 O) shows that non-impacted groundwater plots on the Global Meteoric Water Line (GMWL), while wastewater data plot away from the GMWL line. Intermediate values are interpreted as an evidence of mixing between the two end members. Tritium values below 0.8 TU are associated with non-impacted groundwater with pre-atomic hydrogen bomb age, whereas the canal water has a younger signature (higher TU values). Stable isotopes and tritium data dened two types of recharge water: (1) meteoric pre-atomic water with <50 yr (north zone), and (2) recent evaporated surface water.

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Acknowledgements This work was funded in part by Ph.D. scholarship 93725 from CONACyT-Mxico and Grants 030607 and 103308 from PAEP-UNAM. The authors wish to thank the Comisin Nacional del Agua-Mxico (CNA) for allowing the use of their data. Finally, the authors also wish to express special thanks to Pedro Morales y a Edith Cienfuegos for isotopic analyses, and to the anonymous reviewers of the nal manuscript.

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