CONTRIBUTION TO THE STUDY OF INDUSTRIAL CONTAMINANTS IN SOIL CHARACTERISTICS

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1 CONTRIBUTION TO THE STUDY OF INDUSTRIAL CONTAMINANTS IN SOIL CHARACTERISTICS Aline Marta Vasconcelos Loureiro 1*, Simone Louise D. C. Brasil 2, Lidia Yokoyama 3 1,2,3 Escola de Química Universidade Federal do Rio de Janeiro Abstract. Millions of kilometers of buried pipelines are used in the world to carry crude oil, natural gas, fuels in general, chemical products, etc. If an accident happens in some industries near the pipelines, chemical compounds can be spilled to the soil causing pollution and changing its natural characteristics. This fact modifies physical-chemistry properties of the medium inducing negative impacts. According to the Brazilian Soil Classification, Latossolo is the most common soil in Brazil. Consequently, this typical Brazilian soil would be ideal to investigate the effects of industrial contaminants. This present study aims to analyze the influence of acid, alkali and organic contaminants in the soil concerning its resistivity. These industrial compounds were added to samples of Latossolos in laboratory in order to evaluate the total soil aggressiveness comparing to the soil without contaminants. It s very common to protect the buried pipelines against corrosion, however failures or insufficient protection can possibly occur, this way; the steel would be exposed to the soil with different characteristics. In this case, the alteration of the soil s corrosiveness can accelerate the corrosion process of the steel, and so new spills in the environment can occur. The results obtained by experimental tests would provide useful information about the possible effects of corrosiveness on buried structures using as a model typical Brazilian soil. Keywords: soil characteristics, industrial wastes and buried pipeline 1. Introduction Buried structures corrode in environments such as soil and the corrosion rate depends on the porosity, ph, moisture and depth. Buried pipelines that span long distances pass through varied of soils and, in some places, insidious ions add to the corrosivity of the soil. In practice, it is observed that the corrosiveness of soils determines the service life of the buried metallic structure. Thus, this corrosiveness varies from one location to another due to nature of the soil chemistry, which in addition depends on aeration, dissolved salts and resistivity. Increased resistivity decreases the corrosiveness of the soil, thus indicating that the resistivity is inversely proportional to the rate of corrosion (Oguzie, 24). The goal of this work is to study the influence of some industrial effluents on soil corrosiveness concerning to steel structures when submitted on drastic conditions as absent protection technique on metal (representation of possible failure or protection insufficient) and high humidity on medium (situation of low resistivity). It s important to know the modifications induced on the physical-chemical properties of the soil, caused accidentally by industries close to the pipelines in order to control the process of corrosion. 2. The Soil The soil is considered a heterogeneous system consisting of a mix constituted of inert materials, salts, water and organic compounds. The soil s characteristics are dependent on physical and mineralogical features of essential material, climate, conditions of animal and vegetable life, topography and the soil s development time (Serra, 1982). To whom all correspondence should be addressed. Address: Escola de Química, UFRJ Centro de Tecnologia, Bl. E, Rio de Janeiro Brazil alinemarta@pop.com.br

2 Brazil is a big country, and, it has a variety of climates and kinds of soil making it a complex medium. This large variety of soils makes the study of its corrosiveness difficult. In this work, the soil chosen was Latossolo vermelho-amarelo of Brazilian Soil Classification because this is the most common soil in Brazil (Oliveira, 1992; Lepsh, 22). 3. Soil Corrosiveness The metallic structures are subjected to corrosive processes that are directly related to the physical-chemical properties medium. It s a common practice to coat the pipelines with a highly insulated coating and to apply a cathodic current in order to protect the buried steel pipelines. The efficient cathodic protection demands knowledge about factors that control environment aggressiveness as electrical resistivity, humidity content, redox potential, ph, presence of soluble salts, gases and microorganisms (Baeckmann et al., 1997). Steinrath has proposed a more complete analysis of factors that contribute to the soil corrosiveness by means of determination of parameters that influences the global corrosive process attributing partial indexes. A sum of partial indexes defines the soil aggressiveness. Tables 1 and 2 show the physical-chemical parameters and their respective partial indexes (Trabanelli, et al., 1972). Soils with ph of 5 and lower can contribute to severe corrosion and rapid deterioration of exposed metals. Underground corrosion caused by chlorides ions may be due to the ability of the chloride salts to form hydrochloride acid that contributes to increasing the total acid intensity levels of soil mass. High chloride concentrations lower soil resistivity, facilitating corrosion currents. Sulfates levels are frequently associated with high concentrations of organic matter, which should lead to the corrosion engineer to test for total volatile solids. Measuring the oxidation-reduction (redox) potential is an attempt to identify soil conditions that may support anaerobic bacteria such as sulfate-reducing bacteria. Many scientists and engineers identified more corrosion occurring in low resistivity soils than high-resistivity soils. The attribution of the values for the partial indexes is subjective and the researchers of different countries don t always come to an agreement. It can result different the attribution of the importance to be given to each parameter in evaluating its influence on the global process (Trabanelli et al., 1972). This method is very interesting because it encompasses several important physical-chemical factors in a corrosive process. In this work, the resistivity of the soil was evaluated. Soil resistivity measurement is a very simple test and it has been used as an indicator of the ability of the soil to promote corrosion on a metal structure. The corrosion occurs more intensively in low resistivity soils because the current flows easily. Ramanoff states the simplest criterion for estimating the corrosivity of a given soil is its resistivity, which depends largely on the nature and amount of dissolved salts in the soil and is also affected by temperature and moisture content, compactness of the soil, and presence of inert materials, such as stones and gravel. Robinson (1993) describes the level of soil corrosiveness in relation to the resistivity, as shown in table 3. When the pipeline traverses soil that varies in resistivity, corrosion cells develop between the high and low resistivity areas. Sections of pipe located in low resistivity areas became anodic to sections of pipe located in high resistivity areas. The magnitude of variation in resistivity is of greater significance than the absolute value of resistivity (Robinson, 1993).

3 Table 1. Parameters of the Soil and their Partial Indexes Parameters of the Soil Partial Index > to to <2. -4 E redoxi (mv/nhe) > to a -2 < -4 ph >5 <5 1 Humidity (%) <2 >2-1 Cl - (mg/kg) <1 1 to >1. -4 SO 2-4 (mg/kg) <2 2 to 3-1 >3-2 S 2- (mg/kg) Absent <,5-2 >,5-4 Table 2. Classification of Soil According to Aggressivity Total Index Classification of Soil Aggressivity Total Index Not aggressive Slightly aggressive -1 to -8 Medium aggressive -8 to -1 Very aggressive < -1 Table 3. Soil Corrosiveness vs Resistivity Soil Corrosiveness Soil Resistivity (Ω.cm) Severely corrosive to 5 Very corrosive 5 to 1. Corrosive 1. to 3. Moderately corrosive 3. to 1. Slightly corrosive 1. to 25. Relatively less corrosive Above Industrial Effluents There are several industrial sectors that can contaminate the soil. Chemical industries produce acids, alkalis, metals, solvents, etc. Petrochemical industries produce various contaminants: hydrocarbons, phenols, acids, alkalis, asbestos. There are other industrial sectors that produce contaminants in their activities, for example, energy, production and transformation of metals and minerals extraction sectors (CETESB, 24).

4 The presence of chemical industries close to buried pipelines is a preoccupation factor because if an accident happens, the spilling chemical compounds can cause pollution and change the natural characteristics of the soil. This alters the physical-chemical properties of the medium inducing negative impacts. The transportation of chemical products through a pipeline is relatively safe as long as the structure is adequately maintained. About 37% of the accidents involving chemical products occurred on rail transport, 29% on road transport, 6% on marine transport, 18% on pipeline transport, 4% on loading and unloading chemicals. Ammonia is the chemical product most frequently involved in accidents (Khan and Abbasi, 1999). This study aims to analyze the behavior of soils concerning its corrosiveness when chemical compounds are spilled in an accident. For this propose, three industrial compounds were chosen to represent the principal industrial effluents: an acid (sulfuric acid), an alkali (ammonia) and an organic compound (1,2-dichloroethane). The sulfur acid has a large production and it is used for the manufacturing of fertilizers, aluminum sulfate, ammonium sulfate, detergents, cellulose, treatment of minerals and metals, pharmaceutical industry, petrochemicals, etc. (Amonex do Brasil, 24). Nitric acid, fertilizers and explosives are some examples of products obtained from ammonia. The production capacity per year in the world overcomes 12 million tons (BBS de Química e Ciências Afins, 24). Besides, the ammonia is a chemical compound often involved in accidents during pipeline transport, as cited above. The 1,2-dichlorethane is an organic compound used as a solvent of blacking, past and on composition of the cleanness products. Highly volatile (evaporate at room temperature), promote negative impacts persisting in underground waters and soils (Estadão, 24). 5. Experimental Procedure The soil sample used in all experiments was Latossolo vermelho-amarelo coming from Juiz de Fora (Minas Gerais, Brazil). The soil was crushed to reduce soil-particle size and dried at 1ºC for 24 hours. The resistivity was measured by a 4-pin soil resistance meter (Nilsson Electrical Laboratory Inc. products, model 4). The study of soil resistivity was carried out in the following stages: 5.1 Evaluation of the Soil Resistivity Variation After Addition of Humidity Content (%) Sufficient amount of previously dried soil was put on Soil Box in order to measure its resistivity. After this first measurement, the soil was mixed with 5% (weight) distilled water and put again on Soil Box in order to register the new resistivity value. This procedure was repeated adding more 5% (weight) distilled water to each measurement until the resistivity value became constant. In this way, it s possible to know the soil resistivity behavior on dry and rainy simulated periods. 5.2 Evaluation of the Soil Resistivity Variation After Addition of Industrial Effluents Content (%) The evaluation of soil resistivity variation involves the gradual addition of different quantities of sulfuric acid, ammonia and 1,2-dichloroethane to a samples of soil containing humidity corresponding to the lowest resistivity measurement determined on previous test. The results reveal the amount of each industrial effluent that represents the lower environment resistivity.

5 5.3 Evaluation of the Soil Resistivity Variation Along Contact Time The soil must be considered as a heterogeneous system having capillary-pores and often, also colloidal characteristics. The heterogeneous characteristics at both microscopic and macroscopic level, the limited mobility of the gaseous and liquid phases and the possible interaction between the water and soil particles come to define the soil as a complex electrolyte (Trabanelli, 1972). The moisture and contaminants can interact with the soil constituents in a continuous and complex way resulting in soil resistivity changes. The proposal of this test was to verify the resistivity variations during some days keeping the initial conditions. 6. Results and Discussion 6.1 Evaluation of the Soil Resistivity Variation After Addition of Water The results obtained by experimental results can be observed on table 4 and figure 1. The dry soil and humidity content until 2% (w/w) had high resistivity measurements (greater than 1 6 ohm.cm). The lower resistivity was found in the sample of soil with about 6% of water, representing strong rain periods. Therefore the following essays with addition of contaminants were carried out using soil containing 6% of moisture (w/w). According to the resistivity soil classification proposed by Robinson, the Latossolo with 6% moisture is able to promote the significant corrosion on metals. 6.2 Evaluation of the Soil Resistivity Variation After Addition of Sulfuric Acid Table 5 and Figure 2 show the results obtained from gradual addition of sulfuric acid to soil with critical humidity condition (6% moisture). This experiment simulates a situation in which the soil receives defined quantities of this contaminant in a eventual accident. The addition of only 1 ml H 2 SO 4 concentrated to 1 g soil (1,8%(w/w) H 2 SO 4 ) caused a significant decrease of soil resistivity. The minimum value of resistivity measurement was found when 3 ml H 2 SO 4 concentrated was added to 1 g soil (5,4% (w/w) H 2 SO 4 concentrated) resulting in a severely corrosive medium. For this reason, this concentration value of H 2 SO 4 contaminant was used in other experiments. Table 4. Soil resistivity variation after addition of humidity content (%) Humidity Content (%) >1M 5 >1M 1 >1M 15 >1M 2 >1M

6 Humidity Content (% ) Fig. 1. Soil resistivity variation after addition of humidity content (%) Table 5. Soil resistivity variation after addition of sulfuric acid content (%) H 2 SO 4 Content (%) 35 1,8 31 3,6 18 5,4 13 7,3 13 9, H 2 SO 4 Content (%) 1 Fig 2. Soil resistivity variation after addition of sulfuric acid content (%) 6.3 Evaluation of the Soil Resistivity Variation After Addition of Ammonia The same procedure was done to study the resistivity variation of soils with 6% humidity when ammonia is spilled on soil. The results are showed in table 6 and figure 3. The minimum resistivity value occurs when ammonia content is 1,4%(w/w) corresponding from a severe to a very corrosive medium, according to Robinson. Table 6. Soil resistivity variation after addition of ammonia content (%) NH 3 Content (%) 35,2 9,5 59,7 545, ,1 5 1,4 49 1,6 49

7 ,2,4,6,8 1 1,2 1,4 1,6 1,8 NH 3 Content (%) Fig 3. Soil resistivity variation after addition of ammonia content (%) 6.3 Evaluation of the Soil Resistivity Variation After Addition of 1,2-dichloroethane Whereas the addition of acid or alkali content to humid soil caused reduction of the resistivity, the presence of 1,2-dichloroethane (also named DCE) increased the resistivity measurements. The resistivity value of environment rises until DCE content reaches 3,8%(w/w). It isn t expected that DCE shows the same behavior than the previous effluents analyzed. The organic contaminant doesn t have an essential ionic characteristic; so the increasing of resistivity can be attributed to the DCE sorption phenomena by soil. Due to the high polarity of water, the DCE shows more affinity by soil. Then, the resistivity value is mainly influenced by the moisture content that is free in the environment. Using as reference table 3, this humid soil before and after addition of DCE promotes a weak corrosion on steel. Table 7. Soil resistivity variation after addition of 1,2-dichloroethane content (%) DCE Content (%) 35 1,3 37 2,5 38 3,8 4 5, 4 6, DCE Content (%) Fig 4. Soil resistivity variation after addition of DCE content (%) 6.4 Analysis of Soil Resistivity After Addition of Different Humidity Contents Along Contact Time Samples of Latossolo were kept at constant moisture of 1, 2, 3, 4, 5 and 6% (w/w) without contaminants by the use of a plastic film to avoid water evaporation. Resistivity measurements (ohm.cm) were

8 done for each humidity content until 13 days as shown at table 8 and figure 4 the behavior of soil containing 4% humidity or more and their similar resistivity values. Table 8. Soil resistivity values (ohm.cm) along contact time H2O (%) >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M >1M % H2O 4% H2O 5% H2O 6% H2O Fig 5. Variation of humidity soil resistivity along contact time 6.5 Analysis of Soil Resistivity at 4 and 6% Humidity Contained 5,4% H 2 SO 4 Along Contact Time Soil samples containing 4 and 6% (w/w) humidity received 5,4% (w/w) sulfuric acid and the resistivity were read along 13 days. The reasons for using 4 and 6% humidity content are: from 4% humidity the similar behavior showed at figure 5 along 13 days, and 6% due to the resistivity doesn t vary with increase humidity content (item 5.1). The results of this test are in table 9 and figure 6. Table 9. Humidity soil resistivity values (ohm.cm) containing 5,4% H 2 SO 4 along contact time H2O (%) , 28,5 14, 63, 92, 92, 115, 125, 16,5 25, 1, 39, 64, 69, 7, 68, % H2O 6% H2O Fig 6. Variation of humidity soil resistivity containing 5,4% H 2 SO 4 along contact time

9 6.5 Analysis of Soil Resistivity at 4 and 6% Humidity Contained 1,4% NH 3 Along Contact Time The similar procedure was done with 1,4% (w/w) ammonia. According to item 5.3, the minimum resistivity was obtained with this value of concentration. The table 1 and figure 7 show that soil containing 4% humidity showed higher resistivity values, as also observed with sulfuric acid. Table 1. Humidity soil resistivity values (ohm.cm) containing 1,4% NH 3 along contact time H2O (%) Contact Time (days) % H2O 6% H2O Fig 6. Variation of humidity soil resistivity containing 1,4% NH 3 along contact time 6.6 Analysis of Soil Resistivity at 4 and 6% Humidity Contained 3,8% DCE Along Contact Time As previously mentioned (item 5.4), 3,8% DCE content was chosen due to the fact that the resistivity didn t vary over this contaminant concentration. Soil with 6% humidity in contact with this organic contaminant exhibited higher resistivity measurements (see table 11 and figure 7). Table 11. Humidity soil resistivity values (ohm.cm) containing 3,8% DCE along contact time H2O (%) Contact Time (days) % H2O 6% H2O Fig 7. Variation of humidity soil resistivity containing 3,8% DCE along contact time

10 7. Conclusions The 6% humidity content simulates a drastic corrosiveness condition for Latossolos in strong rain periods. The addition of sulfuric acid and ammonia resulted in decrease of soil resistivity (aggressiveness increased). On the other hand, the addition of DCE increased soil resistivity (less aggressive environment). Analyzing the results obtained by these experiments, it was observed that the aggressiveness of the three contaminants added on humid soil decreases in this order: H 2 SO 4 > NH 3 > 1,2-dichloroethane. According to Soil Classification by Robinson, the soil aggressiveness is, respectively: severely, very to severely and less corrosive. Despite maintaining the initial conditions, the resistivity values varied during 13 days probably because of the contaminants interaction with the moisture present and the complex soil composition. In relation to addition of effluents to soils containing 4 and 6% humidity, sulfuric acid or ammonia in 4% humidity soil resulted be more resistive than in 6% humidity soil, while the addition of DCE in 4% humidity soil caused it to become less resistive than 6% humidity soil. It can be proposed for next experiments to adopt 4% humidity content as drastic condition for corrosiveness soil studying by three reasons. First, it was observed a similar behavior for 4 and 6% humidity content along 13 days with respect to resistivity measurements. Besides, the essay of addition ammonia to 6% humidity soil resulted in very fluid consistency; this physical state for soil doesn t reflect real situation, even occurring strong rains periods. Finally, it s very common to find in literature works about studying of resistivity soil using 3% humidity content as limit humidity ; so, the 4% humidity value become near of moisture content that researches usually study with soils. 8. References A monex do Brasil. Ácido Sulfúrico. Site consulted on December 24 Baeckmann, W. V., Schwenk, W., Prinz, W. (1997). Handbook of Cathodic Corrosion Protection, 3ª ed., Gulf Pub. BBS de Química e Ciências Afins. consulted on December 24. CETESB. Apostila 61 - Métodos de Screeming. consulted January 24. Estadão. Ciência e Meio Ambiente. consulted on December 24. Khan, F. I., Abbasi, S. A. (1999). Major Accidents in Process Industries and an Analysis of Causes and Consequences. Journal of Loss Prevention in the Process Industries 12, 361. Lepsh, I. F. (22). Formação e Conservação dos Solos. Oficina de Textos, São Paulo, Brasil. Oguzie, E. E, Agochkwu, I. B., Onuchukwu A. I. Monitoring the Corrosion Susceptibility of Mild Steel in Varied Soil Textures by Corrosion Product Count Technique. Materials Chemistry and Physics 84, 1. Oliveira, J. B, Jacomine P. K. T, Camargo, M. N. (1992). Classes Gerais de Solos do Brasil. FUNEP, Jaboticabal, Brasil. Robinson, W. C. (1993). Testing Soil for Corrosiveness. Materials Performance, Intermountain Corrosion Service Inc. Pacific Highway, Tacoma, WA. Serra, E. T. (1982). Corrosão pelo Solo: agentes, avaliação e soluções. Eletricidade Moderna. São Paulo, Brasil. Trabanelli, G., Zucchi, F., Arpaia, M. (1972). Methods of Determination of Soil Corrosiveness With Respect to Metallic Structures. Chinica Pura ed Applicata, 3, Acknowledgments The first author is thankful to financial support given by ANP (Agência Nacional do Petróleo) and institutional support by Escola de Química UFRJ.

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