Ann. It Super. Sanita Vol 25,. 3 (1989), pp. 17-524 SOLID WASTE MANAGEMENT AND BIOELEMENTS IN SOIL E. ZAVATTIERO, O. CASTAGNOLI and L, MUSMECI Laboratorio di Igiene Ambientale, Istituto Superiore di Sanita, Rome, Italy Summary.- Two studiesare reportedinthe field of solid waste management. The firstconcerns heavy metal migra- tion below a landfill site. The results show that total and Ieachable heavy metal concentrations are more variable in refuse than in soil samples, as refuse is not homoge- neous but can be influenced by local conditions and the seasons. Inthe soil below refuse, the concentration of total ‘metals is low and similar to control soil samples, whereas leachable metals behaved differently in the two drillings, their mobility depending on soil characteristics. The bulk of heavy metals, however, remains immobile. The second study regards the uilization of compost as afilter bed for pig slurry to reduce its pollution load hence enriching the compostof the nutrientsit lacks. A pilotplant was installed utilizing pressed straw bale containersfilled with compost through which pig slurry was filtered. The filtering tests demonstrated a reduction of the pollution load of slurry and at the same time evidenced the possibility of utilizing the entire filtering system as a fertilizer to improve com- post, with heavy metal concentration tolerance limits lower than the ones proposed at anational level to prevent environmental pollution. Riassunto (Bicelementi nel suolo nella gestione dei ri- fiuti solidi). - Sono riportati i risultati di due indagini ef- {fettuate nel campo della gestione dei rifiai. La prima ha ‘presoinconsiderazione la migrazione di metallipesantiin tuna discarica per rifiut solidi urbani e nel terreno sotto- stante. I risultati delle analisi hanno messo in evidenza una variabilita maggiore nei rifiut rispettoal suolo dovu- taalla disomogeneita dei materiali smaliti che €influen- zatada situazioni localie dalle stagioni. Il compertamento della parte rilasciabile dei metalli é diversa nelle due perforazioni essendo la loro mobilita tegata alle caratte ristiche del suolo. Tuttavia la maggior parte dei metalli risulta immobilizzata, La seconda ricerca é stata miata allo studio della utilizzazione del compost quale letto {filtrante per iliquani diallevamenti suinicoli, cont inten- 10 di ridurre il carico inquinante di questi e contempora- neamente arricchire il compost degli elementi nuritivi. Dopo varie fasi di sperimentazione in laboratorio é stato ccostruito un impianto pilota che wilizzava balle di paglia pressata come vasca di contenimento riempita di compost ‘come filtro. I risultati delle prove difiltraggio del liquame ‘hanno mostrato una riduzione del carico inquin questo € messo in evidenza la possibilitd di wil Tintero sistema filtrante quale concime con un contenuto di metalli pesanti al di sotto dei limiti previsti dali’ attuale normativa nazionale. Introduction ‘The use of land as a waste management alternative involves technological and potential health problems that ‘ced further research. Investigation of landfill sites indica- tes that most sites have problems associated to leachate migration that pollutes the environment, Disposal or recy ‘cling of increasingly large amounts of agricultural wastes also poses a problem. Lack of comparable control and technology has made disposal of agricultural wastes more of a pollution hazard than municipal wastes. ‘The climination or improvement ofthese problems lies in the understanding of the quantitative aspects regarding the transfer of pollutants through soils and in a better knowledge of the soil environment in which each waste application is located, Soil characteristics Soil is a heterogeneous and complex three-phase sy- stem containing, solid, liquid and gaseous components. The sizeot the solid particles between which pore space is, Formed is occupied by the liquid and gaseous phases in & proportion,sig According to statistical studies on soil composition the ‘mean values are as follows: 50% oxygen, 25% silicon, 15% sesquioxide-forming elements and 10% water. The solid fraction of soil is composed mainly of inorganic materials such as silicates, oxides and phosphates: the organic soil content is low and it results from biological degradation of wastes. both animal and vegetal. Its low quantity is compensated by being very reactive. ‘The soil properties, both physico-mechanical and che- ‘ical are related to solid particle size. In particular, the mobility and accumulation of pollutants ischiefly control- led by their reaction with the solid phase; it depends on solid particle size, on the amount, size and shape of pore space and on the amount and type of soil mineral. ‘The solid particles taken intoaccountare less than 2mm in diameter and are mixtures of sand, silt and clay in relative proportions. The latter has a particle size smaller than 0.002 mm, Solids with particles larger than 2mm in diameter constitute the soil skeleton, such as gravel, stone and conglomerates. Their large pores provideacontinuous channel, so they do not chemically influence the pollution phenomena of soil ‘Sand and clay, differ from each other both in dimension and chemical composition. Sand is composed of quartz and silicates, whereas clay consists of a group of silicate minerals known as clay minerals, These clay minerals comprise cations coordinated tetrahedrally and octahe- drally, forming either sheets or chains. “Moreover, trace elements occur in soil at alow concen- tration and steady state. Sometimes these elements are found in particular locations in unusually high concentra- tions, Neverthless, they do not cause pollution since they are naturally immobilized. In fact, an example is the presence of Fe in Elba soil and Hg near mount Amiata. ‘The liquid phase enveloping the solid phase contains dissolved substances both organic and inorganic, which influence their mobility. Water is a fundamental compo- nent because it is the principal carrier of possible pollu- tants. Air, the third component of the soil system, tends to attain equilibrium with the soil solution. Airis present in the first soil layers where the biological living matter, microrganisms and plant roots breathe. In the deeper layers, instead, pore spaces are gradually filled with water, thus developing anacrobic conditions. This type of envi- ronment supports the diffusion of facultative anaerobic microrganisms that can also live without oxygen and later favours the growth of obligate anaerobic bacteria. So pollution When duc to human activities a pollutant penetrates the soil system in large quantities, not only it can alter the composition and functioning of soil, butalsoandabove all, itcan produce groundwater pollution asa consequence of the migration of substances not connected withthe natural environment by transporting them into water solution causing change of its physical, chemical and microbiolo- gical properties. Soi migration ‘Transport and accumulation of various pollutants in soil is controlled by physical, chemical and biological mechanisms. The physical mechanisms are: diffusion caused by the thermal motion of ions and molecules, dispersion due to velocity variation in pore space; dilution ‘with passage of fluids from unsaturated zones to saturated cones below a clay layer; physical sorption which involves the attachment of the sorbent and sorbate through the Van der Waal forces, and filtration through solid particles. ‘The chemical mechanisms are: precipitation and solu- tion characterized by the establishment of a chemical equilibrium between the liquid and solid phases, adsorp- tion (the adhesion of ions or molecules in extremely thin layers to the surface of soil solids with which they are in contact); desorption (the opposite phenomenum); com plexation (the chemical reaction between metal ions with anions and with organic chelant to form organic and organometallic complexes); and ion exchange (the inter- change between a cation in solution and another cation adsorbed on a surface of any surface-active material), Microbiological mechanisms are the most difficult to quantify. They have enormous influence on the migration of toxic pollutants, with consequences on redox processes, mineralisation, immobilisation and complexation reac- tions. Objectives Considering that land disposal and treatment must be taken as separate altematives, the purpose ofthis study was two-fold: 1) to document the behaviour of pollutants in a landfill and their migration in the soil below refuse; 2) 10 study the possibility of maximum utilisation of agricultural wastesand, atthe same time, to provide public health protection. Analytical methods The determination of total heavy metal content was performed on air-dried, sieved and pulverized samples by ‘atomic absorption spectrometry (AAS), predigesting the samples with nitric acid under pressure and heat. The Ieachabble heavy metal concentration was determi- ned on fresh samples placed in a vessel with deionized water in a 1:16 ratio and continuously stirred for 24 h adding 0.5 N acetic acid to reach the pH of 5 + 0.2. The liquid phase obtained after centrifugation (and filtered if necessary) was analyzed by means of AAS with graphite furnace. Migration from landfill sites ‘The first part of this study regards the disposal of ‘municipal solid wastes and the consequences it hason soil, pollution. The oldest and most diffused method of house-hold refuse disposal consists in dumping into pits or trenches digged expressly for that purpose or in excavated sgravel or sand pits, clay quarries and other lands otherwise unsuitable for cultivation or construction. After the refuse is dumped and compacted, tis covered with soil, minimi- zing the problem of odors, fires and vectors which are critical environmental factors in sanitary landfill plants. If the design and construction of landfill and operation plants are not adequately done, the refuse disposal can cause damage to soil because fill leachates can migrate tounder- lying groundwater, eventually causing contamination. Leachates are pollutants caused by inflow of rainfall and produced by organic solid waste decomposition that can contain dissolved and suspended organic and inorganic material. ‘The present legislation (DPR 915/82 and its regulation) prohibits landfills which are not sanitary and prescribes technical guidelines according to waste characteristics, 10 be employed for landfill site design, construction and ‘operating procedures. Itis necessary, however, to consider old open dumps that donotcomply with sanitary regulations and that were not regulated by law at the time they were filled. Even small quantities of abusive disposal may cause pollution ‘due to toxic substance contents, To verify the way in which refuse can contribute to harmful dispersion in soil, a survey of several municipal landfills includedin various teritorial contexts was carried ‘out incollaboration with the Veneto region (Fig. 1) [1-3]. In these landfills drillings were performed using a hollow steam rotating auger and samples of refuse and soil be- neath the landfill were drawn in the zone of influence of leachates produced by refuse. Analyses of significant ‘parameters to monitor pollution such as chemical oxygen demand (COD), conductivity, organic carbon, phosphate and nitrogen were performed together with a survey of Riu VENEZIA GIULIA TRENTINO ALTO ADIGE oe . ga ere ~ gar Fig. 1. = Location of Veneto landfill diling. Landfills: 1) Ponzano ‘Veneto; 2) Aivole 3) Campodarsego; 4) Cerea; 5) Este; 6) Sandrigo: 7) Rosa 519 heavy metal concentrations. To evaluate the amount lea- ched, refuse and soil samples were analyzed by a standard elution testto determine the release and the evaluation of what is supposed to take place on a long-term basis. ‘The results presented in this paper were taken from the municipal solid waste landfill of Ponzano Veneto in the Treviso area. This landfill is tocated in an abandoned gravel pit where the refuse is disposed of in a way that cannot be considered “controlled” because the soil is permeable and easily leachable by liquids that alsocontain inorganic pollutants. Fig. 2 reports a cross-section of this, landfill, the drilling sites and the different depths. Results and conclusions on migration from landfill sites Tables 1-5 report the analyses carried out in refuse and soil samples obtained from two drillingsand also from soil samples collected in three sites further away from the landfill area at 1 m depth From the results the following conclusions can be drawn: 1) metal concentration in refuse layers does not present regular trend as the materials disposed of are not homo- ‘gencous,¢.g. even houschold refuse is determined by local influences such as socioeconomic conditions, recreational areas (picnic and camping sites) and commercial and institutional areas. Moreover, yard-wastes, a part of muni- cipal refuse, can vary with the seasons. The municipal ‘waste disposal system of piling up and compressing refuse ‘without homogenizing it, can greatly affect these results; 2) the higher concentrations of total metals are found in refuse layers; 3) the high level of total Cr in drilling site no. 1 is probably due to industrial waste disposal in that zone evidenced also by the presence of ammonium and sulfur fumes during drilling operations; 4) the higher values of otal Fe, Cuand Zn indrilling site no, 2 prove the disposal of household refuse in that zone ‘because of the metals normally present in many materials discarded; 5) total metal concentrations in soil samples beneath the landfill are inferior to those of refuse samples, but similar to those of control soil samples at three sites beyond the zone of influence of the refuse; (Groundwater —e] 2. Crt sexton ofthe Pavano Veneto landfill520 ‘Table 1. - Ponzano Veneto landfill: analytical results of refuse samples collected at drill no. 1 (xis) Depth) Fe Ma co a cr x ot $446.08 17425 29128 109379 43050 6150 1s J og 098 1368 10 7317 a10 a2 wa oor 738 os 68 oa 5536 L 1633.26 29850 14925 168 1835, 32 4s Waal ot 192 3500 192 010 288 188 wn 603 838 139 ars 193 151 ‘ 883721 sas 18140 i093 2326 ss WAl : 519 less L7 2585 268 488 wn dios saat 098 ia iss 938 — 12896390 43608 ais00 rizr 26890 4845 us : $29 Teao 10 1074 303 132 —t sin oe ans on 627 fey 1533 ‘ sss131 25150 5030 2628 29030 16150 nsf] ot 11833, 3089 282 fer 78) Soa wk 139 2008 Sor 9203 233 2175 t sai29s 301.83 1924 wes 28750 a1 Average © 2638 1623 159 963 336 1093 wn 031 2132 ret 2400 it 152 ‘ wast 9580 sor 4340011988 on Standard deviation 3155 69 090 so 270 1436 wen at 1480 196 3839 as 619 wastes clay Le sin Hla sans ws gravel or) released ‘Table 2. - Ponzano Veneto landjill: analytical results of soil samples collected at drill no. I (ug!s) Depth (m) re Mn zn or a ws eta 2408 wows (12019 1202 133 YMA 15433 1673 ‘60 601 521 684 a2 an 288 8 Ba seo ‘ sms) 3976 2007 9.01 21 1453 us QM & Tis iaaas i300 193 0 ea an 108 as 389 BB tke an © 92 eal 39.39 au Msi £1.00 3s Qe Sas Take a3 28 Sas a8 sn 035 a0 ai Sie 33 3s . mst 267 240 ae wi 2500 s Qe M980 tor 3 00 an eu on 38 Het as i0t Ot 1. was 37 om R06 1187 1s Gla Fe 333 ss 8 ‘ato 2s sa obs Sie 1053 22 ots ehh ‘ soy. 20148 3668 sas 90 1531 13s We : He 8 8 rr 301 a8 ldla on sR 18 as i sop 23.64 2002 2 igo 2141 om : ie BS 23 48 3 A wk ast Be Ba it Bh ae ‘ 63.36 4604 50s let alas 1985 suabiaceriiey 35 6 if $3 id 35 if ise 38 ae it oh ey Lin Ch sass gre2 ‘Table 3. - Ponzano Veneto landfill: analytical results of refuse samples collected at drill no. 2 (ugig) Depth (m) Fe Ma cu Zn cr ‘ 17660.00 710.70 3782 108.80 182 25.90 + 44.60 365.25 040 394 040 0.60 sth 478 31.39 Lo 56 338 232 ' 13310.09 539.80 11789) 10790 2863 2010 ' 65.03, 2orss 020 580 040 240 rn 5.00 49.62 047 538 140 1198 t 19970.00 77880 2730.02 398.70 52.28 4870 r 22595 29°94 020 3.80 020 3.00 wk 13 3123 001 oss 038 616 ‘ 4010000, 41210 23259 34720 532s 20 r esos 92.03 080 620, 200 720 win ‘oat 2233 038 15 376 1030 ' 19130.00 671.00 n36 137.70 3879 7450 50 ' 192.01 274.00 1a 3.80 ‘080 200 wrk 1.00 40.47 19s 276 224 268 t 22034.00 623.68, 628.18 22006 3635 4768 Average : 418.45 257.81 0.60 Sul 076 3.04 wn 2.46 40.21 on 327 223 670 1 10420.09 46.87 L768 Mos 1733 2459 Standard deviation 31434 10053 052 120 073 249 an 233 Thiet 080 201 139 38 tetotal released 6) the presence of higher metal concentrations in some layers of drilling no. 1 is due to retention of small layers of lay and silt; 7) the percentage of leachable metals is very low with respect to the total amount. The soil below the landfill site shows similar values to those of control soil, with the exception of Ni present in the soil of drilling no. 1 and of Cr in the soil of drilling no. 2; 8) if weconsider leachable metals as a whole (i... both drillings) different behaviours can be observed. In drilling no. 1, the concentration of leachable Fe, Mn and Zn decreases in soil layers, whereas the concentration of Cu, Ct and Ni increases in soil as compared to refuse. In drilling no.2, the concentration of Zn, Cr and Ni decreases in the soil below the landfill and the concentration of Fe, Mn and Cu increases with respect to refuse. As far as the concentration of Mn, Zn, Cr and Cu is concerned, the higher release occurs two-three meters below the refuse, where a series of sand and gravel layers in clay and silty matrix are present. Leachable Cr and Fe tend to decrease in proportion to depth. However, in the last soil layer, an increase was observed. Compost and agricultural wastes ‘The second study regards both the treatment of land through which nutrients return to their natural cycle and the disposal of wastes in such a way that any adverse impact can be examined and controlled, The resource values of wastes must be safe for public health and envi- ronmental reasons. ‘Composting isa decomposition and mineralization pro- cess, under controlled conditions, for converting munici- pal solid wastes into a product that can be used in agricul- ture without causing damage to public health. The chief agricultural utilisation of compost is as a soil conditioner for its organic matter content, but its use is limited because itlacks nutritional elements such asN and P, necessary for plant growth. In the field of pig husbandry many industrialized coun- ties converted from traditional methods of farming with production of farmyard manure to modern methods with the concentration of large numbers of animals in intensive earings, This type of industrial breeding has created {enormous problems of disposal or utilisation of vast quan- tities of animal waste that exceed the quantities that can be utilized by soil. Excessive applications throughout the year may cause pollution of surface water for the following reasons: organic matter, salt and chemical run-off, pollu- tion of groundwater because of nitrate, nitrite, salt and chemical leaching, reduction of crop yield due to nutrients build-up, and damage to soil properties (pH, structure, salinity, tc.) because the excreta is applied in semiliquid form. The prospect of reducing the pollution level of liquids and at the sime time of enriching compost with the elements it lacks, has stimulated research of systems that tuse compost as a filter bed. In this manner, a harmless disposal of the two types of refuse can be carried out without causing522 Table 4. - Ponzano Veneto landfill: analytical resulis of soil samples collected at drill no. 2 (ug/g) Depth (m) Fe Mn co In or N \ 790m 23530 3595 7820 3336 39.090 3s Ya 380 300 a 130 335 130 ZZ rh O21 23.97 1.76 153 659 3.08 i 26000 26890 605 ona 2559 5450 «0 YA .* 23 a 1 213 33 8 wk on Bn 23 380 508 ae ' 900 20520 3206 4168 258 1800 «s YU By a 308 ot 23 2 an an $9 ae 1682 338 nit ‘ $00 22280 1798 256 2586 2150 10 W : ass m3 oer iss 2a aa Wild ork 024 31.40, 484 458 10.09 1214 : r19999 —ats90 2602 897 2692 19.00 13 Wa Be a0 $i 53 3 Aa en a8 se 30 30 isi 0s : momo 21930 a3 5080 5198 1770 s YA: i3%8 138 oss 18 Sas oe - fork 0.19 36.09 1.80, 252 Ta 1s 7 i 294009 16930 sos was ass 550 ss Wh e38 ois 168 27 330 398 Uda 0.29 43.14 335 293 592 B15 i 55000 2o3g0 1999 suo nx 1630 °° Wl « cd 3103 a8 80 360 S80 wis ass ees 0 ion ie His ‘ som = 162 80 3819 2040 °s WHA 2300 tan $0 es se 330 ‘as oe 18. MB 3H Be i esse 1658 3140 seas 2330 2800 aes : ie aH ie sie 38 et ods 2 i ass 38 Bae ‘ ree 401 1870 nurs 937 1440 Sunda deviation + 218 i a8 308 oz im win oo coe Be 530 158 30 ] wases oy LA" Warn re meeased Table 5. - Ponzano Veneto landfill: analytical results of soil samples collected in three locations out of landfill site (ugls) Sample Fe Mn co tm c Ni t T3061 249.88 4988 ast 10973 236 | Ya 625 03 268 357 337 aa wn 008 no Sa sos 335 8 ‘ 8841 23913 oss 2364 ozs 3936 > Was 316 99.55 199 28 199 Sa wn ann 3997 338 ane 26 Bi ‘ 683633 32835 13228 as 1471 2495 3 : 738 10888 20 336 “00 505 We an ae Ber ite Me ne) ‘ 800417 m2 7398 4197 ngsg 2933 Average : 800 3661 22 338 285 S18 win on 3836 Sat 30 249 wis (7) emtes chy Yn tual fe teleased‘The research developed in two subsequent stages. In the first stage, slurry was filtered (with or without recy- cling or under ventilation) through the compost held in plexiglass lysimeters (4, 5]. The second stage consisted in the introduction of straw into the filters leading to a substantial improvement of the filtering capacity and to a reduction of pollution load (6-8].In the third stage, a pilot plant was installed ina farm with intensive methods of pig rearing [9, 10}. A lank was built with the sides and bottom made of pressed wheat straw bales and spread with a 30cm layer of compost. The tank was filled at a rate of 2.5 /s and successively with 2147 lof liquid pig manure, viaa supply pipe coming from a nearby lagoon (Fig. 3). Complete analyses of liquid manure, compostand effluent were done regularly, ‘After 10 days, when the leaching of the liquid manure ‘was completed, the filtering system was sectioned and various layers were identified. Dry fraction of manure, straw and compost samples of various layers were taken and analyzed, Finally, the filtering system was destroyed and the material was carefully mixed, ‘The analyses were done considering two different aspects: environmental and agronomical. The analyses of the original and filtered liquid manure evidenced adecrea- se in biological oxygen demand (BOD), COD, suspended solids ($$), N and P and an increase in the BOD/COD ratio, anindicator of biodegradability. From the agronomi- 523 Fig. 3. - ilo plant scheme. cal pointof view, the material obtained from the mixing of the filtering system presented a higher content of N and P than the compost. In addition, the presence of heavy metals in the experi- mental system was studied to verify whether their concen- trations constitute a health or environmentai hazard. Re- sults are reported in Table 6. ‘The total and theoretical quantities ofthe experimental system were estimated and the results reported in Table 7 Table 6.- Heavy metals concentrations carried out in the single layers Layer Material ‘Concentration (ug/g) Zn co cr Pb co Ni Mn ca 1 SL 1265.7 565.1 38 288 156 322 1468 282 2 SL 15923 6813 545 297 na ort 185 3 SL 1539.8 5958 337 403 68 188 155 4 SL+co 6646 2797 452 3704 137 397 191 S$ SL+Co+st 625.1 2782 1025 2797 168 692, 4174 ns 6 SL+sT 22675 1339 216 1508 93 381 224 45 7 st 23.4 1456 3 7 199 898 656 484 SL; sludge; CO: compost; ST: straw Table 7. - Total amount of heavy metals in the whole filtering system Layer Material - ‘Amount (9) zn cu cr Pb co Ni Mn ca 1 sl. 14 33 03 02 on 02 44 02 2 st. 301 29 09 06 02 13 218 03 3 St 981 319) 21 26 08 12 552 1 4 SL+00 197 83 13 ta 04 12 B3 06 5 SL+CO+st 76 34 3 34 02 08 st 02 6 st+st 1948 ns. 19 29 08 33 34 08 7 st na 69 on 9 ua 43 32 23 Total 368.8 178 79 7 32 3 54 sa Concentration (ug/g) 2781 Mis ot 254 23 93 946, 38 Limits (8/9) EEC 2500 1000 750 150 won sone 20 600 200 00 100 1000 io Italy (Decree no, 915/82) 2500 SL sludge; CO: compost: ST: saw524 ‘The maximum heavy metal concentration values proposed by the EEC and those prescribed by the Decree of the President of the Republic (DPR) no. 915/82.are also repor- ted in this table, The results showed concentrations below the values proposed. Conclusions on migration from compost and agricultural wastes ‘The experimental system is an effective pretreatment as organic fertilizer better than compost at the end of the filtering cycle. The heavy metal content is not dangerous for the agricultural environment, as it was below the proposed limit values. This system can also be developed for pratical use. These studiesrepresentiwo practical examplesofsound and effective procedures to protect soil from undue conta- rmination from the elements. They also reflect the overall waste management trends to be further encouraged and applied. plant for the separation of the solid fraction of pig slurry with low energy consumption. Moreover, the utilized ‘wastes (straw, compost and solid fraction of pig slurry) are completely recycled because the whole plant can be used Review submitted on invitation by the Editorial Board of the Annali REFERENCES 1. -ZAVATTIERO, E,, BONTEMPELL, R,, CALLEGARI, E, MUSMECI, L.& CASTAGNOLI, O. 1984, Indagini su una disca contollata in reazione alle possibiithd'inguinamento delle acque sotternes In: Ati dele giornate di studio "SEP pollaion” . Padova, 8-12 aprile, 1984. E.A. Fire di Padova, pp.143-153, 2 BONTEMPELLI, R. & ZAVATTIERO, E. 1986. Verfca della migrazione di inguinani da dscariche nel Veneto tramite caotaggi. In: Au delle giornateinernationali di stdio “SEP pollution". Padova, 610 aprile, 1986. E.A. Fier di Padova, pp. 739-754, 3. CASTAGNOLI, 0.,ZAVATTIERO, E, & MUSMECI, L. 1988. Municipal solid waste landfill and risk for groundwater system, In: Second {international conference on environment protection. 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