International Journal of Engineering Trends and Technology- Volume4Issue3- 2013
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Programa de Pós- Graduação em Engenharia Química, Escola de Engenharia, Universidade Federal Fluminense (UFF),
Rua Passo da Pátria 156, 2° andar, Niterói, Rio de Janeiro, Brasil, CEP 24220-240
Abstract
With increasing pressure from society and environmental agencies of industries and other sectors that use natural resources, especially water, it is necessary to develop new technologies to minimize water abstraction and effluent discharge in water bodies. An alternative to reduce these environmental impacts is the capture of rainwater, especially in regions of high rainfall. However, in regions with intense industrial activity, the presence of air pollutants can impair the quality of water collected. Oil refineries have great polluter potential, generating several pollutants such as NH
3
, SO x
, NO x
.
In this context, this work aims studying the feasibility of capturing rain water in an oil refinery, both for industrial use and for non-potable use. Rainwater collectors were developed and subsequently some contaminants were analyzed in the water collected. Analytical techniques such as ion chromatography, atomic absorption and potentiometry were selected for the determination of pH, conductivity, ammonia, sulfate, nitrate, chloride and metals such as aluminum, calcium, magnesium and sodium.
Keywords— Water, rainwater, pollutants, oil refinery.
I.
I NTRODUCTION
The concern of authorities and society is bigger everyday on environmental issues, especially when it comes to the rational use of water resources, causing a great pressure from environmental agencies on the branches of the economy that best utilize these resources, the industry and agriculture.
In Brazil, the Law 9433/97 [1] establishes a series of conditions on the use of water, in order to ensure the current and future generations the necessary availability of water in adequate quality standards. One of the instruments of this law is to establish a value to be charged for water used and stipulate a maximum value that can be used by an institution through the use of grants.
The environmental agencies have encouraged the reuse of water, either through rewards or reduction of grant, so that industries start to optimize their processes to reduce water consumption.
One way to optimize such processes is making use of the reuse of industrial waters, taking advantage of an effluent for "less noble" use, also reducing the load of effluents discharged into water bodies.
An alternative way is to reuse water by capturing rain water, but the presence of air pollutants may limit the use of water abstracted. Authors like [1] compare the rainwater to distilled water in purity, and recommend its use for nonpotable purposes, as authors such as [2] and [3] draw attention to the pollution of rainwater in metropolitan and industrialized regions, which makes this source of water unsuitable for direct use. Several papers have been published on methods of rainwater harvesting, including [4] dealing specifically in the capturing in residential and agriculture.
In 2002, [5] rated water availability in Brazil as very high, but the situation in the Southeast is more critical, being ranked low due to its high population density, further reinforcing the need for new technologies to capture water resources , especially rainwater, since the rainfall is high in the region.
One of the branches of an industry that best uses water resources are oil refineries, making the abstraction of water for various purposes, from drinking water production to use in various processes. The water consumption in refineries is approximately 0.7 to 1.2 m
3
water/m
3
of oil, being a refinery like REDUC (Oil Refinery, Caxias, Brazil), that processes approximately 38,000 m
3
of oil per day, can consume over 45 million liters of water/day. An alternative way of reducing water consumption in a refinery would be to capture rainwater, but the presence of air pollutants such as
NH
3
, H
2
S [6], phenols, SO x
, NO x
and other metals, common in a refinery, could derail this alternative.
The only treatment unit of acid water of a refinery processes approximately 153 kg/h of H
2
S and 152 kg/h of
NH
3
, with the monthly rainfall being able to reach 390 mm.
The ammonia gas for example, is very soluble in water and your solubility can be favored by an increase in the pH of the water and rain variations.
According to [7], ammonia has a residence time in the atmosphere ranging from one to two weeks and may be removed there from by dry or wet deposition processes and photochemical processes. Acids generated by oxidation of
SO
NH
2
and NO
4
+ x
are also neutralized by ammonia (NH
3
salts in particulate form.
) forming
This study has as one of its goals evaluate the viability of capturing storm water in an oil refinery as well as investigate the presence of contaminants that make their use unfeasible as process water and propose technologies already existent to treat this water and make it suitable for the nonpotable use or process water.
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International Journal of Engineering Trends and Technology- Volume4Issue3- 2013
II.
M ETHODOLOGY
The Refinery under study is located in the state of
Rio de Janeiro and has an area of 13 square kilometers and produces more than 50 kinds of products among them gasoline, jet fuel, diesel, LPG (Liquefied Petroleum Gas), paraffin and it is responsible for producing over 80% of the country’s lubricants.
The metropolitan region of Rio de Janeiro is divided into four air basins called sub-regions and the Refinery is situated in the sub-region 3, which covers an area of approximately 700 km
2
that covers the counties of Nova
Iguaçu, Belford Roxo and Mesquita; the districts of Nilópolis and Olinda, in Nilópolis County; the districts of São João de
Meriti, Coelho da Rocha and São Mateus, in São João de
Meriti County; the districts of Duque de Caxias, Xerém,
Campos Elíseos and Imbariê, in Duque de Caxias Ciy; the districts Guia de Pacobaíba, Inhomirim and Suruí, in Magé
County and the administrative regions of Portuária, Centro,
Rio Comprido, Botafogo, São Cristóvão, Tijuca, Vila Isabel,
Ramos, Penha, Méier, Engenho Novo, Irajá, Madureira,
Bangu, Ilha do Governador, Anchieta and Santa Tereza, in
Rio de Janeiro County. It is a region of great industrial activity and surrounded by the city’s major traffic routes.
The collection of rainwater was conducted between
May and September 2012, a period of dry with low amount of rainfall which favors the buildup of pollutants in the atmosphere. We used an artisan collector of wet and dry deposition, passive, low-cost, composed of a glass funnel of
20 cm diameter coupled to an amber glass bottle. Campos et al
[8], showed the predominance of higher concentrations in samples of total deposition facing the deposition collectors to only humid to most studied ions.
To avoid loss of volatile substances in the sample rubber seals were placed in the bottle cap and latex tubes at the ends of funnels and in the tube of collected water for analysis of ammonia was added 1 mL of concentrated sulfuric acid to encourage the formation of ammonium ions and therefore avoid volatilization of ammonia gas.
The collectors were placed on the laboratory‘s roof of the refinery, located 4 meters above ground level during rainfall. The laboratory is located in a central area of the refinery and is surrounded by several generating units of pollutants, among them an FCC (Fluid Catalytic Cracking) unit, three units of acid water treatment, a hydrotreating unit and a delayed coker unit.
The Na
+
, Ca
2 +
, Mg
2 +
and Al
3 +
ions were determined using an atomic absorption spectrophotometer Varian 240 FS with their respective hollow cathode lamps. An aliquot of 100 mL of water collected was treated with concentrated HNO
3 and placed on a heating plate for volume reduction and then fattened in a 50 mL volumetric flask.
For the analysis of sodium ion was used a dilution with 10% volume balloon ionization cesium suppressor. In the
2+ analyzes of Ca and Mg
2+
suppressor ionization and cesium releasing agent lanthanum were used respectively in a 10 mL volumetric flask resulting in a dilution of 1.11 times. Each ion was analyzed with its respective hollow cathode lamp
For the determination of ions NH
4
+
, SO
4
2+
, Cl
 and
NO
3

an ion chromatograph Metrohm 850 with conductivity detector was used. For the NH
4
+
a column C4 cationic
Metrosep 150 and an eluent of 1.7 mmol/L HNO
3
and 0.7 mmol/L dipicolinic acid was used, an initial flow of eluent of
0.9 mL/min and the column conditioned 30° C. For ions SO
4
2+
,
Cl

and NO

3
an anion column was used Metrosep The Supp
5150, a pre-column of 50 mm length, eluent of 3.2 mmol/L
Na
2
CO
3
and 1.0 mmol/L NaHCO
3
. The conductivity measurements made on a form Metrohm conductivity from
856 to 25º C and pH with a pH meter Metrohm 827 pH Lab using a combined glass electrode.
III.
R ESULTS
The results analyzes performed on the waters collected are shown in Table 1 .
To mitigate discrepancies regarding dilutions caused by differences in the volumes of water collected during precipitation, the average volumetric concentration calculation
(VCC) was used, since in very low rainfall the concentration of the analyzed species tend to be higher towards those whose volume of precipitation is larger [9]. VCC can be calculated according to the equation:
Where,
C i
= concentration of the analyte in the sample; v i = volume collected during precipitation.
The VCC's calculated and the mean and standard deviation are shown in Table 2.
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International Journal of Engineering Trends and Technology- Volume4Issue3- 2013
TABLE 1
R ESULTS OF ANALYZES OF SAMPLES OF RAINWATER COLLECTED
Analysis
Na
+
Ca
2+
Mg
2+
Al
3+
NH
4
+
Cl

SO
4
2 
NO
3

pH Conductivity
Sample Collection Date
C1
µmol/L
23/05 - 03/06 113,5 142,5 45,3 163,1 35,6 108,9 122,8 27,7 7,37
(µS/cm)
72,84
C2 06/06 - 08/06 77,4 245 5 1,5 46,1 38,6 22,5 15,6 6,46 16,43
C3
C4
09/06 - 11/06
28/ago
101,7 52 8,3
76,5 41,25 10,8
2,6
2,2
63,9
87,2
50,2
50,2
37,3 17,6 6,61
54 24 5,76
79,38
52,59
TABLE 2
A VERAGE VOLUMETRIC CONCENTRATION , ARITHMETIC MEAN , MINIMUM , MAXIMUM AND
STANDARD DEVIATION OF RAINWATER COLLECTED IN THE REFINERY
Parameters/Ions Na
+
Ca
2+
Mg
2+
Al
3+
NH
4
+
Cl

SO
4
2 
NO
3

pH Conductivity
µmol/L (µS/cm)
Average
VCC
92,28 120,19 17,35 42,35 58,20 61,98 59,15 21,23 6,55
91,70 104,40 12,72 22,11 61,89 54,83 48,48 19,91 6,22
76,50 41,25 5,00 1,50 35,60 38,60 22,50 15,60 5,76 Minimum
Maximum 113,50 245,00 45,30 163,10 87,20 108,90 122,80 27,70 7,37
Standard Deviation 18,34 94,79 18,78 80,50 22,59 31,76 44,34 5,61 0,66
55,31
57,94
16,43
72,84
28,32
In order to calculate the pH’s VCC, the concentration of H
+
ions obtained by the measurement of pH was used. The high values of standard deviation can be attributed to variation in local atmospheric conditions that are subject to different rates of pollutant emissions from the refinery, direction and speed of winds. The validation of the data was made using the criterion of ionic balance as presented by Lara [10]: concentrations of these ions as well as excess amount using the equation presented by Riley& Chester [12]:
According to [11], BI-valued samples exceeding 15% should be rejected, because in these cases problems are evidenced sampling and/or analysis.
The graph of Figure 1 shows the relationship between cations and anions in samples collected. According to calculations and the obtained correlation data set seen in the graph (r = 0.98), none of the samples was rejected in this study.
Some ions present in samples such as Na
+
, Ca
2+
,
Mg
2+
, SO
4
2-
and Cl

can have "sea spray" as its origin, particularly in coastal regions as the area studied. It is possible to calculate the contribution of the "spray" in the
Figure 1 – Ionic balance in samples of the refinery’s rainwater.
[X]
Seawater
= {[X]/[Na
+
]} seawater
x [Na
+
]
analyzed where the ions Ca
2+
, Mg
2+
, Cl

and SO
4
2+
are represented by X and the ratio {[X] / [Na]} is assigned to seawater.
The concentration in excess can be obtained by subtracting the marine concentration, [X] seawater
of the total
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International Journal of Engineering Trends and Technology- Volume4Issue3- 2013 concentration according to the equation presented by Souza et al [13]:
[X] excess
= [X] total
– [X] seawater
Table 3 shows the contribution of ionic concentrations in marine and the respective reasons
{[X]/[Na
+
]} given by Riley e Chester [12].
Ions
Ca
2+
Mg
2+
Cl

SO
4
2 
TABLE 3
C ONTRIBUTIONS OF IONIC CONCENTRATIONS
[X]/[Na
+
]
*
Relations
[X]/[Na
+
] [X] excess
[X] seawater
0,02
0,11
1,17
0,06
1,14
0,14
0,6
0,64
102,6
2,63
-52,5
42,98
1,83
10,09
107,3
5,5
* RILEY e CHESTER (1971)
The high values found for the ratio [SO
4
2-
]/[Na
+
] were expected because of the SO x
emissions by industrial plants, refinery emissions and vehicle on the highways surrounding the same that incorporate the raindrops.
The high ratio of [Ca
2+
]/[Na
+
] draw attention but it is probably due to the large civil construction activity within the refinery, especially near the collection sites.
The anomalous result of the ratio [Cl
-
]/[Na
+
[Cl] excess
], as well as a negative value of
leads to believing that not all Na
+
found is of marine origin and may also be attributed to anthropogenic sources continental.
The other ions except for Mg
2+
, also appear with much higher concentrations in excess bigger than the marine contribution, causing the latter apparently is negligible.
Rain with a pH below 5.0 caused by the presence of traces of strong acids in the atmosphere as H
2
SO
4
, HNO
3
and also by H
2
CO
3
is called acid rain [14]. However it was observed in the samples that none of them had values in the pH range of acid rain, despite the excess of SO
4
2 
and the presence of nitrate in chemical composition of these waters. A likely explanation for this phenomenon may be the presence of ammonium in high concentrations, promoting the neutralization of acids formed.
According to [15], because ammonia is very soluble in water, it increases the pH of rain and also converts salts of acidic species into nitrate salts (NH
4
NO
3
) and sulphate
((NH
4
)
2
SO
4
) forming aerosols which comprise the smallest fraction of the material particulate.
Also according to [15] the main sources of ammonia in the atmosphere is the burning of fossil fuels, which occurs intensively at the refinery, biomass burning, sea surface, pet waste and human excrement emissions from soil. Guimarães
& Mello [16] found an average flow of ammonia nitrogen in the range of 26.2 micromole/L in surface waters of Guanabara
Bay (Rio de Janeiro), along with that, the presence of a landfill near the refinery, vehicular emissions on highways around it and own emissions of ammonia generated in the refinery can be attributed to high concentrations of this ion found in samples collected.
The fluidized catalytic cracking units (FCC) are responsible for emissions of aluminum in the atmosphere due to loss of catalyst during the process. Although the sample C1 has submitted a peak concentration of aluminum, the other samples showed no significant amounts of this ion which does not bring great impact in the event of the use of rainwater for other purposes as will be shown later.
The results obtained in the present study compared with previous studies on ionic composition of rainwater in order to assess the impacts of pollution generated at the refinery in relation to other places without much industrial activity and also subject to local anthropogenic sources of ions analyzed. Table 4 presents a comparison between six studies performed in Brazil and also in Spain.
Analyzing the data above shows the influence of where the collections are made of rainwater. For samples of the Refinery, collections are made very close to sources of pollution that are quickly incorporated into raindrops during precipitation, in this case the influence of residence time in the atmosphere becomes negligible since the pollutants are continuously generated. High values for NH
4
+
, SO
4
2-
and NO
3
were expected because it is a unit where they burn tons of fossil fuels every day.
Among the related work which showed a concentration closer to the value found in this study for ammonium and nitrate was [17], where the author gives as the source of these ions and the intense metabolic emissions vehicle traffic in the study area. Peña et al. [18] attributes the high sulfate concentrations in anthropogenic contributions to his work, but does not specify an activity. Campos et al [19],
Souza et al [8] and Peña et al. [18] had high concentrations of chloride ions in their samples for their work because they were performed in air as well as the coastal area where the refinery is located, but calculations shown previously showed a low influence of the "spray" on marine samples.
Honorius et al. [19] was the only one to analyze the aluminum ion, and attaches it to the continental crustal origin of this cation, differing sources of aluminum cited in this work.
Among the pH, the water collected in the refiner also had the highest value due to high concentration of ammonia, which neutralizes acidic species responsible for lowering the pH.
Peña et al. [18] also assigns the excess of calcium and magnesium ions in their dust samples of soil, since these ions had an excess over the marine "spray".
Henceforth are evaluated parameters related to the quality of the water collected in the face of legislation and technical parameters in order to classify the water as to its possible use in the refinery. Table 5 shows the parameters related to CONAMA [20] resolution 357 and the 1469
Ordinance of the Ministry of Health are compared with values obtained in the analysis of rainwater.
Taking into account only the ions analyzed and executing the values of aluminum, the rainwater collected in the refinery could even be used as drinking water, after its
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International Journal of Engineering Trends and Technology- Volume4Issue3- 2013 disinfection and fluoridation, since all parameters are specified by both regulators.
TABLE 4
C OMPARISONS OF RESULTS BETWEEN STUDIES ON IONIC COMPOSITION OF RAINWATER
Parameters Na
+
Ca
2+
Mg
2+
Al
Ions, µmol/L
3+
NH
4
+
SO
4
2 
Refinery
Honório et al.(2010) *
Peña et al (2002)
Leal et al (2004)
Souza et al (2006)
91,1 104,9 12,72 22,11 61,89 59,15
15,4 17,1 2,1 951 - 9,5
114,0 22,0
Campos et al (1997)** 154,0 15,6
15,0
142,2
5,33
4,6
13,0
23,4
2,51
20,2
-
-
-
-
25,0
0,98
37,6
9,9
30,0
25,0
12,4
17,4
* Results of open area in Manaus (Brazil); ** Results total deposition
Cl

203
8,54
178,2
NO
3

54,83 21,23 6,55
10,1 12,3 4,1
110 17,0 4,95
1,12
21,2
12 pH
5,51
5,19
5,22
Conductivity
(µS/cm
57,94
-
-
30,7
13,0
29,9
TABLE 5
C OMPARISONS OF RESULTS OBTAINED WITH PARAMETERS SPECIFIED BY CONAMA RESOLUTIONS 357 AND DECREE 1469 OF M INISTRY OF H EALTH I SSUES
Refinery
Class 1
Class 2
Al
3+
1,14
0,1 *
0,1 *
NH
4
+
1,05
Ions, mg/L
Cl

2,2
SO
4
2 
5,68
NO
3

1,32 pH
6,55
Class 3
Class 4
Drinking Water***
0,2 *
0,2 *
0,2
13,3 **
13,3 **
1,5
250
250
250
250
250
250
10
10
10
6,0 - 9,0
6,0 - 9,0
6,0 - 9,5
* Values for dissolved aluminum (CONAMA 357, 2005); ** Values in mg/L specified for pH <7.5 (CONAMA 357, 2005)
*** Ministry of Health, Decree 1469 (2001)
3,7 **
3,7 **
250
250
250
250
10
10
6,0 - 9,0
6,0 - 9,0
The CONAMA 357 [20] specifies only the concentration of dissolved aluminum as aluminum, and the values found in the samples are reported as total aluminum.
Generally the total aluminum is greater than or equal to dissolved aluminum, but this was not possible to quantify the second form, and therefore it is not possible to state conditions of potability of the rainwater. Freitas et al. [21] reports that there is a debate in the medical circle on the relationship between aluminum and Alzheimer's disease and also reports the neurotoxic effect of this metal in the long term, may cause severe encephalopathy in patients suffering from renal dialysis, which may lead to neurological disorders.
We must take into account the presence of other chemical species that may be present in rainwater and were not analyzed in this study, such as carboxylates, aldehydes, formates, and others that may compromise the quality of water.
Aiming the use of rainwater as process water becomes necessary to compare the samples with technical data.
Table 6 shows the comparison of the values obtained from data provided by [22]. Total hardness is the sum of the concentrations of calcium and magnesium salts, such as sulfates, nitrates, carbonates and chlorides. For purposes of calculating the hardness takes into account the carbonate salts according to the equation:
Hardness (CaCO
3
) = [C
Ca2+
x (50/20)] + [C where the numbers 50, 20 and 12 respectively represent the gram equivalents of CaCO
3
, Ca
2+
e Mg
2+
.
Mg2+
x(50/12)]
Salts of calcium and magnesium have a tendency to form incrustations on surfaces where there is heat exchange, resulting, for example, the blocking of boiler tubes and heat exchangers in cooling water systems, corrosion by differential aeration and efficiency loss of the heat exchange surfaces [23].
The pH and the chloride content are also treated to prevent corrosive processes. The presence of ammonia also becomes an inconvenient and requires treatment to avoid corrosive processes.
TABLE 6
C OMPARISONS OF RESULTS FOR RAINWATER REFINERY WITH TECHNICAL
DATA PROVIDE BY S PANIARD (2005)
Parameter
(mg/L)
Chlorides
Hardness pH
Ammoniacal nitrogen
Aluminium
Calcium
Magnesium
Cooling
Water
500**
650
6,9 a 9,0
1,0
0,1
50
0,5
Pressure
Boiler
(<10bar)
***
350
7 a 10
0,1
5
***
***
Pressure boiler
(>10bar)
***
1,0
8,2 a 10
0,1
0,1
0,4
0,25
Sulfate 200 *** ***
** In some types of systems this concentration must be less.
*** Accepted as received if other limits are met.
Rainwater
Refinery
2,2
11,75
6,55
1,05
1,14
4,2
0,3
5,68
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International Journal of Engineering Trends and Technology- Volume4Issue3- 2013
Ammonia, in the presence of dissolved oxygen in water is corrosive to copper and its alloys and in very high concentrations is corrosive to copper even in the absence of dissolved oxygen [23]. The removal of sulfate is needed to prevent the formation of calcium and magnesium salts.
[5] UNEP, United Nations Environment Programmer, Global Environment
Outlook 3: past, present and future perspectives. Earthscan, UK, 2002.
[6] F. B. Mainier, G. C. Sandres, R. J. Mainier, Integrated Management
System for in-House Control of Accidental Hydrogen Sulfide Leaks in
Oil Refineries, International Journal of Science and Advanced
Technology, volume 2, issue 9, September, p. 76-84, 2012.
IV.
C ONCLUSIONS
Despite the close proximity of sources of air emissions from the refinery to the collectors of rainwater and the influence of other sources of pollutants such as motor vehicles on highways surrounding the industrial park, landfills and also the Guanabara Bay, the results showed that rainwater can be a viable alternative to reduce water consumption and spending with your collection, treatment and effluent disposal as the refinery. It is necessary, however, a pretreatment of the water collected to adapt it to various purposes required by the refinery.
The present study showed that for the parameters analyzed rainwater compares to the quality standards required by agency inspectors as CONAMA, since disinfection treatments and removal of ions Al 3+ performed on it. Removal of the Al 3+ ion would also be required for use in generating of high and medium pressure steam.
SIMÕES FILHO [23] suggests treatment with ion exchange column for removal of this ion and Freitas [21] recommends the use of membrane filtration with reverse osmosis to remove dissolved ions.
For its use as industrial water would be needed other treatments in order to make it conform to the specifications required for each purpose. The simplest treatments would pH adjustment and subsequent decrease in hardness by removing Ca
2+
and Mg
2+
.
Processes such as soda lime treatment and ion exchange can be used for removal of these ions [23]. The presence of NH
4
+ ions is undesirable in industrial waters because it is corrosive and in potable waters is an indication for pollution even at very low concentrations. Their removal may be done using either the chlorination process can also be partially removed by degassing.
This study was conducted during a low amount of precipitation resulting in lesser amounts of samples, but during dry periods the accumulation of pollutants in the atmosphere is higher than in rainy periods.
A more comprehensive and more representative study may be made in the future by extending the period of sample collection to
12 months, exploring the dry and the rainy season. Upon completion of the study of quality rainwater other work can be performed in order to study the economic viability and development of effective collection and storage of water on a large scale.
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