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Utilization of sediments dredged from marine ports as a principal component of composite material
Journal of Cleaner Production xxx (2016) 1e9
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Utilization of sediments dredged from marine ports as a principal component of composite material Vsevolod Mymrin*, Jacqueline C. Stella, Cristofer B. Scremim, Roberto C.Y. Pan, Filipe G. Sanches, Kirill Alekseev, Daniela E. Pedroso, Andrea Molinetti, Otavio M. Fortini Department of Civil Construction, Federal Technological University of Parana, St. Hector Alencar Furtado, 4900, Campus Curitiba, CEP: 81280-340, Ecoville, , Brazil Parana
a r t i c l e i n f o
a b s t r a c t
Article history: Received 30 April 2016 Received in revised form 6 October 2016 Accepted 9 October 2016 Available online xxx
The main purpose of this research is to develop technically, economically, and environmentally attractive construction materials from sediments dredged from Brazilian seaports. The final composite material contains 50 to 60 wt% in mass of sediments and thus creates an opportunity to diminish the pollution of the Atlantic Ocean. Construction and demolition debris (20e35%) and lime production wastes (15e30%) were used as components of the composite materials. Uniaxial compressive strength values reach 6.3 MPa on the 3rd day and 14.5 MPa on the 90th day; linear shrinkage varied between 0.07% and 0.35%, water absorption - between 11.0 and 13.4%. These values attend the demands of Brazilian norms on conventional bricks, blocks, etc. XRD, XRF, SEM, EDS, AAS and LAMMA analysis showed that amorphous new formations are responsible for material strengthening. © 2016 Elsevier Ltd. All rights reserved.
Keywords: Atlantic ocean pollution Dredging sediment utilization Structure formation processes Cement-less solid materials Mechanical properties Ocean environment protection
1. Introduction This study is dedicated to the development of construction material composites based on three industrial wastes: sediments dredged from ports on the Atlantic Ocean (SDS), construction and demolition debris (CDD), and lime production waste (LPW). The release of sediments from dredging of seaports is an old solution in practically every port worldwide (Brown et al., 1990; Pagliai et al., 1985). The disposal of large amounts of materials dredged from the port is a new, environmentally serious problem. For example, in the US, volumes of dredged sediment for the period from 2011 to 2018 were close to 2.4 million m3 annually (Krause and McDonnell, 2000; Rehmat and Mensinger, 1999). At the Port of Bremen, Germany, approximately 600,000 m3 of dredging sediment are removed annually (Kay and Volker, 2002). In Brazil alone, 80,313,000 m3 of sediment were dredged from ports in 2009 (Brasil, 2009). The main raw material source for this research was the sea port in Parana State, Brazil, which is the second most of Paranagua
* Corresponding author. E-mail address: [email protected] (V. Mymrin).
important port in Brazil. This port has a total area of 2,350,000 m2 with maritime access 150e200 m wide, 20 miles long, and 13e15 m deep (APPA, 2012). The volumes dredged from the ports of Para and Antonina in Parana State were 3,700,000 m3 in 2009; nagua 3 110,000 m in 2011; 3,700,000 m3 in 2012; and 8,000,000 m3 in 2013. These large amounts of sediment were sent to final offshore disposition in high seas (IBAMA, 2013; APPA, 2012, 2009). In Brazil, it is illegal to store of contaminated sediments in the ocean (CONAMA, Resolution 454, 2012). Therefore, the ability to reuse the dredged material in combination with contaminated debris would be a means to achieve legal compliance, reduce the amounts of material send to landfills, and an incentive to reduce maritime pollution (Yozzo et al., 2004). In the international scientific literature, there are many studies showing that dredged sediment can be used as a raw material for the development of different materials in construction (Gutt and Collins, 1987), the manufacture of concrete (Limeira et al., 2010), the construction of roads (Dubois et al., 2008), the production of bricks (Hamer and Karius, 2002), the construction and restoration of beaches and coastlines, for protection and land reclamation (ICES, 2011), and in the manufacture of glass tiles, cement blocks, bricks, etc. (Krause and McDonnell, 2000). The present study provides a new solution to this problem by
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offering a new, technologically simple and economically attractive method of disposing of SDS in combination with two other construction materials, which also considers industrial wastes: CDD and LPW. CDD includes aggregates such as bricks, concrete, plaster, glass, asphalt, tiles, gypsum wallboard, wood, metals, and different types of plastics. The Construction & Demolition Recycling Association (CDRA) states that in the USA, more than 325 million tons of CCD are produced annually. It makes up 25e45% of the waste that goes to USA landfills, thus contributing to the reduced life and increased environmental impact across the country (Leigh and Patterson, 2004). The most common and viable solution for the disposal of CDD is to incorporate them into the base and sub-base of road construction (Bennert et al., 2007). In the opinion of John et al. (1996) and Mymrin (2012), CDD can be used as the main raw material (up to 85 wt %) in different manufacturing construction materials, such as solid and hollow bricks or in compositions. Lime production waste (LPW) is poorly burnt lime, where the combustion process has not occurred at a sufficient temperature and to completion (Garcia, 2008), or is the result of burnt lime storage under inappropriate conditions (without sufficient insulation and air humidity). LPW can be used (Bhatty and Gajda, 2004) ^a and Mymrin (2005) used LPW as a by the cement industry. Corre waste concrete binder. Mymrin (2012) used LPW as a binder of many types of industrial wastes: phosphor-gypsum, cement, pulp for paper production, wastewater sludge, wood ash, steel slag, asbestos tiles, porcelain, and natural rock waste. Al-Sayed et al. (2004) and Do et al. (2007) determined that the use of LPW increases the physical and chemical properties of the asphalt mixture. Arce et al. (2009) employed LPW to immobilize the waste generated in the painting process. Al-Khaja et al. (2003) studied the use of LPW as a mineral aggregate in mortar mixtures. Bulewicza et al. (2008) reached over 70% desulfurization of flue gases from coal being burnt for power by incorporating to an LPW oven. Kumar (2003) and Marinkovic et al. (2010) made possible the use of LPW as raw material for the manufacture of bricks. The objectives of this research were to develop composite materials for civil construction using the dredged sediments contaminated with marine saltwater to achieve mechanical properties within Brazilian standards (NBR), research the physical and chemical processes of structure formation in these materials with predetermined properties, and decrease the cost of production of construction materials using three types of industrial wastes as raw materials, completely replacing traditional natural materials that have a much higher price. The ultimate goal of this research is to develop a technically, economically, and environmentally attractive construction material and thus create an opportunity to stop polluting the Atlantic Ocean with sediments dredged from Brazilian sea ports.
granulometric composition was determined by sieve and Wagner methods; the uniaxial resistance strength by uniaxial compression with an EMIC press model DL10,000; water absorption (WA) was measured with an Instrutherm BD 200, and the linear shrinkage (LS) with a Mitutoyo linear scale system. 2.2. Calculations The values of the water absorption coefficient (CWA) were determined on the 28th and 90th days of the TSs curing, following the Brazilian standards NBR 9778/2009 and NBR 8492, which uses the following equation: WA ¼ [(MSAT MD)/MD] 100,
(1)
where MSAT is the mass of the saturated TS after 24 h of immersion in water and MD is the mass of the TSs oven-dried at 100 C for 24 h. The values for the apparent density DA (g/cm3) are obtained by the equation DA ¼ PD/(PH PI),
(2)
where, PD is the mass of the TSs, PD is the dry mass of the TSs ovendried at 100 C (g), PH is the mass of the humid TSs oven-dried at 100 C (g), and PI is the mass of the humid TSs oven-dried at 100 C and immersed in water (g). 2.3. Raw materials A representative sample of the SDS was obtained with assistance from the company DTA Engineering during a harbor dredging at Paranagu a, Paran a state, Brazil. The area used for disposal of and Antonina material dredged (Fig. 1) from the ports of Paranagua is located more than 20 miles from Island of Galheta and the Island of Mel in the stretch. Bravo 1 (APPA, 2012). The CDD and LPW samples were collected in the enterprises of the metropolitan region of Curitiba, Brazil. 3. Results and discussion 3.1. Raw materials characterization Port The initial moisture content of the SDS from the Paranagua
2. Research methods and raw materials 2.1. Methods The raw and final materials were characterized by various complementary methods. The chemical composition was determined using X-ray fluorescence (XRF) with a Marc Philips/PAnalytical model PW 2400, and by atomic absorption analysis (AAA) with a Perkin Elmer 4100 spectrometer; the mineral composition was determined by X-ray diffraction (XRD) with a Philips machine model PW 1830; the morphological structure was analyzed with a scanning electron microscopy (SEM) FEI model Quanta 200 LV; the micro\chemical analysis by the method of energy dispersive spectroscopy (EDS) with an Oxford, Penta FET Precision model X-ACT, and by micro-mass analyses with a laser micro-mass analyzer LAMMA-1000 model X-ACT; the
, Brazil Fig. 1. Area of disposal of dredged material from sea ports of the state Parana (APPA, 2012).
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was 12.54% with a specific mass 2.54 kg/dm3, which is classified as normal (between 2 and 3 kg/dm3). The particle size distributions of the SDS and the CDD were obtained by sieving the materials, and the average result of the two samples of the materials show (Table 1) that most of the SDS (76.72%) are particles nearly 0.149 mm diameter, only 10.3% of particles being larger than 0.149 mm, and only 10.62% smaller than 0.149 mm. According to the Brazilian NBR 7211:2009 classification, such sand is included in the category of small sands. The smallest component is LPW containing about 85% of the particles smaller than 0.2 mm. The particle size distribution of the CDD is not as uniform because 73.23% of the CDD remains on the 0.42, 0.297 and 0.149 mm sieves. The sieve method shows that the largest SDS particles are seashell fragments, the percentage of which is reduced in finer fractions. The smaller fraction (0.42 mm and smaller) are mainly represented by sand with rare, small inclusions, of crushed seashells. Essentially, SDS has no clay and silt, which is explained by the repeated dredging of the port channel. The particle size distribution of LPW, determined by Wagner method of cone immersion, was near 1400 cm2/g. The chemical compositions of the raw materials (Table 2) determined through the XRF analysis shows that the SDS is mainly represented by SiO2 (71.0%), Al2O3 (10.1%), Fe2O3 (3.8%), K2O (3.4%), CaO (2.6%), Na2O (1.4%), MgO (1.1%) and SO3 (1.0%). CDD consists mainly of SiO2 (67.02%) and CaO 11.54%. The chemical composition of LPW (Table 2) includes 48.4% CaO and 25.18% MgO, with the impurity total content of SiO2 þ Al2O3 þ Fe2O3 equal to 2.3%. A carbonate content of 54.7% was determined from mass loss (24.1%) after calcination at 1,000 C of a sample pre-dried at 100 C, by recalculation to the formula of calcite CaCO3. The total levels of carbonates and the impurity content were 57.0%. Therefore, the peaks of calcite CaCO3 have two maximum intensities in the diffractogram pattern (Fig. 2-C). The Brazilian standard NBR 6453 (2003) enables the use of quicklime with a maximum content of impurities and limestone of 12% as a binder in construction. Because of this limitation, the material used should be called “lime production waste” (LPW). The presence of calcium carbide CaC2 is due to the firing of limestone in an open fire. The mineralogical composition of the SDS determined by XRD (Fig. 2-A) includes quartz SiO2, microcline KAlSi3O8 and halite NaCl; CDD was determined (Fig. 2-B) to include quartz (SiO2), calcite (CaCO3) and albite (Na,Ca)(Si,Al)4O8. Mineral composition of LPW (Fig. 2-D) is presented by quicklime CaO, portlandite Ca(OH)2, calcite CaCO3, magnesite MgCO3 and quartz SiO2. The presence of significant amounts of amorphous materials in the diffractogram patterns is also evident. In the SEM images of the SDS (Fig. 3-C), classic hex-octahedron forms typical of halite are clearly visible. EDS analysis of these
4.8 2.4 1.2 0.6 0.42 0.297 0.149 0.075 <0.075 Total
Content of fractions, % CDD
SDS
0 0 0 10.45 17.33 26.78 29.12 9.71 6.20 99.73
0.09 0.13 0.39 1.32 2.91 5.46 76.72 8.58 4.04 99.63
Table 2 Chemical composition of raw materials used (by method of XRF). Elements
SiO2 Al2O3 CaO MgO Fe2O3 TiO2 SO3 P2O5 Na2O MnO K2O Cl C.L.
Chemical composition, wt % SDS
CDD
LPW
71.0 10.1 2.6 1.1 3.8 0.8 0.1 0.1 4.5 0.1 3.4 0.6 3.6
67.02 6.3 11.54 1.37 3.85 0.64 0.58 0.11 0.29 e 0.67 e 7.57
1.89 0.19 48.41 25.18 0.23 e e e e e e e 24.07
C.L. e Calcination Loss.
crystalline bodies confirmed this assumption (Table 3, points 1e4). The morphological structure of the SDS shows rather rounded grains, without sharp edges, of sand (Fig. 3 - A and B) of similar dimensions. In the photo at 1000-times magnification (Fig. 3-B), abrasion of sand particle surfaces is clearly visible, including peeling as a result of friction during the millions of years of geological history of each particle. Such abrasion may enhance the dissolution of the surface layer in an alkaline environment (Iler, 1979), especially in the early stages of hydration of the initial mixture, with the formation of groups of amorphous minerals of calcium silicate hydrate (CSH). The synthesis of these amorphous minerals significantly increases the mechanical properties of the materials developed in this research (Mymrin, 1998). The micro chemical compositions of the SDS sample obtained by the EDS method (Table 3) are in good agreement with the results of the XRF (Table 2). The slight discrepancies in them can be attributed to differences in the sensibility of the research methods and of the methods of the TSs preparation. The substantial complexity in mineral composition at the micro level is confirmed by the EDS analysis of smaller surface areas (1e3, Fig. 3-C) at all points 1e4. The analysis of these areas is substantially different from the analysis obtained with bulk-methods such as XRD (Table 2) and XRF. The particles of the CDD micro-level (Fig. 4 e A and B) have greater dimensions and variety of sizes and therefore lower porosity between them. The chemical composition of the CDD obtained by EDS also includes SiO2 (67.0%) as the main component as well as CaO (11.5%), Al2O3 (6.3%), Fe2O3 (3.9%), and MgO (1.4%); the other elements have levels lower than 1%. The LPW particles (Fig. 4 - C and D) have different shapes and sizes but are rounded, which is typical for amorphous substances. 3.2. Preparation of test samples (TSs)
Table 1 Granulometry compositions of CDD and SDS. Sieve, mm
3
Estimate visual of SDS
Shells Shells 90% shells 50% shells 20% shells 5% shells Sand Sand Sand þ Silt
The preparation of the TSs includes the following operations: collecting representative samples, sieving with a 1.19 mm mesh sieve, weighing in advance certain percentages (Table 4), mixing and homogenization of the components, hydrating and compacting the cylindrical samples to a height and diameter of 20 mm at 10 MPa pressure and curing the TSs in open air. The following properties of the TSs were investigated after 3, 7, 14, 28, 60, 90, and 180 days by means of mechanical properties: the uniaxial compression strength, linear expansion, water absorption and density. The values of the mechanical properties and standard deviation were obtained as an average of 10 sample measurements; therefore, the total quantity of the TSs was 540 pieces.
Please cite this article in press as: Mymrin, V., et al., Utilization of sediments dredged from marine ports as a principal component of composite material, Journal of Cleaner Production (2016), http://dx.doi.org/10.1016/j.jclepro.2016.10.035
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Fig. 2. Diffractogram patterns of the raw materials used: A e SDS, B e CDD, C e LPW.
Fig. 3. SEM micro images of the SDS with different magnifications.
Table 3 Chemical micro analyses by EDS method of areas and points of SDS (Fig. 3). Spectrum
Values of elements, wt % C
Na
Mg
Al
Si
Cl
K
Fe
Total
Total area Point 1 Point 2 Point 3 Point 4 Area 1 Area 2 Area 3
20.37 31.86 31.08 e 29.19 32.26 32.90 30.97
4.43 24.13 22.26 33.20 24.14 1.43 e 1.34
1.53 e e e 0.59 1.41 0.64 e
10.33 0.46 1.18 0.96 1.15 7.79 1.41 1.70
34.58 1.68 5.16 3.32 3.44 41.46 62.93 59.48
11.64 41.87 39.57 61.35 40.21 4.37 2.13 4.09
12.96 e 0.76 0.47 0.28 9.32 e 0.83
4.17 e e 0.70 1.00 1.97 e 1.60
100.00 100.00 100.00 100.00 100.00 100.00 100.00 100.00
3.3. Mechanical properties of TSs The values of the uniaxial compressive strength of the TSs (Fig. 5) increase in open air and regularly depend on the cure time and the amount of the binder e the LPW. The higher compressive strength of the TSs at all stages of hydration and curing are found for composition 4 with LPW content of 30%. On the 3rd day of curing, the resistance reached 6.3 MPa; on day 7, 8.2 MPa; on day 28, 13.7 MPa; and on day 180, 15.4 MPa. According to NBR 7170, the uniaxial strength of the fired solid bricks shall be as follows: class A < 1.5 MPa, Class B < 2.5 MPa, Class C < 4.0 MPa. On the 3rd day of curing without firing, the strength (6.3 MPa) of composite material 4 exceeded the demands of Class C by 1.58 times, on the 14th day (11.04 MPa) by 2.06 times and on the
180th day (15.39 MPa) by 3.85 times. After 7 days of curing, the values of mechanical strength of all TSs were above the requirements of Class A standard values, and on the 180th day of curing, all compositions met the requirements of Class C. The lower strength values in all ages of hydration were determined in compositions 1 and 5 to be a result of their lower concentration of LPW (15%). Among them, the highest values of resistance, except on the 3rd and 180th days, belong to composition 1, which had a lower content of SDS (50% versus 60%) and higher content of CDD (35% versus 25%). It appears that 15% LPW is not sufficient to neutralize the existing acid salts (Fig. 3-E and F) in 60% SDS (composition 5) water, but replacing 10% SDS by 10% CDD (composition 1) can improve the resistance values, especially until 90 days of curing. However, between compositions 2 and 6 with 20% LPW, most of the best resistance values belong to composition 6, although with higher levels of SDS (60% vs. 50%) and lower levels of CDD (20% vs. 30%). This may mean that the 20% LPW compared to 15% LPW is less sensitive to substituting 10% CDD by 10% SDS. The increase in LPW content to 25% (composition 3) provided high strength (4.1 MPa) on the 7th day of hydration and 8.9 MPa on the 180th day of curing. The TSs of all the compositions shows very low and highly unstable dilatation values (between 0.07 and 0.96%) during curing. A common tendency was the increase in values until the 28th day of curing, with a slow decrease until the 180th day. The TSs of composition 4 had the lowest amplitude changes between 0.07 and 0.20%, which confirms the stability of the processes of hydrating
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Fig. 4. SEM micro images of the CDD and LPW at different magnifications.
Table 4 Substantial compositions of materials under study. NO
1 2 3 4 5 6
Compositions, wt. % SDS
CDD
LPW
50 50 50 50 60 60
35 30 25 20 25 20
15 20 25 30 15 20
and curing the material. The apparent average density of the TSs of composition 4 on day 3 was 1.748 kg/m3, on day 14, it increases up to 1.795 kg/m3, after 60 days, up to 1.834 kg/m3 and after 180 days, to 1.881 kg/m3. Such changes in the values of the density and of the dilatation of the TSs indicate an increase in the amount of new growths in pore space and reinforcing to 15.39 MPa until 180 days of hydration. 3.4. Physical processes of chemical structure formation The physical and chemical processes of interaction between the hydrated and compacted raw materials accompanying the formation of structures in the new materials were investigated by means of XRD, SEM with EDS and LAMMA methods in the TSs of composition 4, due to high mechanical properties of the samples. 3.4.1. Changes of mineralogical composition Deciphering the X-ray diffractogram patterns (Fig. 6) of the
material at different ages with numerous mineral components is rather difficult because of their coinciding peaks. However, it is possible to discuss some peaks that are free of such coincidence and which changed intensities during the material curing. The intensities of the portlandite peaks are constantly decreasing during the cure time. The peaks of calcite, on the contrary, are increasing in intensity, some of them appear on the 28th day, others appear and on the 60th day, or even only on the 180th day. Therefore, it is possible to surmise the existence of carbonates under the amorphous condition as well. In the initial mix of composition 4, quartz SiO2 is the principal mineral (Fig. 6-A); at higher magnifications of the diffractogram pattern, it is clearly visible that almost all quartz XRD peaks have duplications. These duplications appeared due to processes of the mechanical destructions (cracks, exfoliations, abrasions, etc.) during the geological history of the SDS sand particles. After the dissolution of these defective layers on the sand grains in a high alkaline environment (close to pH ¼ 13), the intensities of the peaks of quartz increased since more perfect surfaces of the mineral structure were exposed. For large amounts of free CaO in the LPW and the CDD, this dissolved amorphous SiO2 can precipitate as in sol-gel synthesis of amorphous materials with unstable chemical composition. As shown elsewhere, such as calcium silicate hydrates CSH becoming a binder between the solid particles of the material (Mymrin, 1998). The role of CSH formations is well-known in the chemistry of hydrated Portland cement. The growth of crystalline and amorphous substances of carbonates and CSH formation may be responsible for the gain in mechanical properties of the materials developed.
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Fig. 5. Change of uniaxial compressive strength values during the curing.
Fig. 6. Comparison of XRD patterns of the composition 4: A - Initial dry mixture, B - on the 28th day, C - on the 60th, D - on the 180th day of hydration.
3.4.2. Processes of structure formation The structure of the initial dry composition 4 by the SEM method (Fig. 7) shows particles with a wide variety of sizes and shapes. In Fig. 7-A at 50-times magnification, numerous and protruding rounded particles of relevant dimensions emerge from the surface layer of the TSs, which are very smooth and dense. However, at 1000- and 5000-times magnification, the presence of large
numbers of pores between particles of different sizes, depths and configurations becomes especially visible. In the images of the 28th day of curing structure (Fig. 7-A, B and C), there are differences in the morphological structure compared to the non-hydrated sample (Figs. 3 and 4). In the image at 500times magnification (Fig. 7-A), in contrast to Fig. 3-A, the sand particles were not visible because they were covered by the layer of
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Fig. 7. SEM micro images of the TSs' structure of the composition 4: A, B and C on the 28th day; D, E and F e on 180th day of cure.
new formations. These new formations effectively cover and act as links between particles. Images at 3000-times magnification (Fig. 7-B) there showed a much denser structure with few string fissures. These changes in the structure of the material may explain the growth of the uniaxial resistance up to 11.0 MPa during the 28 days of curing (Fig. 5). At 6000-times magnification (Fig. 7-C), pore sizes from 5 to 10 mm were observed. The pore chains are linked to each block of material and connected to the large particle size below the coverage of new formations. In Fig. 7-C, the remains of organic material of plant origin can be observed. These materials do not interact chemically with other components of the mixture, and, therefore, during the endurance tests of the TSs, they most likely promoted the development of cracks, thereby significantly reducing the mechanical properties of the materials. It is quite possible that a preliminary separation of plant materials can significantly increase the strength values of the material. The representative images of the TSs structure on the 180th day (Fig. 7-D, E and F) demonstrate the further increasing of the density of the material structure compared to samples on the 28th day: it had almost no pores and cracks and was similar to the images of dense concrete. Only the images at 5000-times magnification show networks of micro pores with diameters from 0.1 to 0.2 mm and rare micro pores with a diameter of 1 mm. Virtually all of them are connected to each other, and most of them are gathered in dense layers without pores or with small and superficial pores.
3.4.3. Chemical composition of new micro formations During the SEM analysis, non-crystalline bodies were found through XRD. This is possible in two variants or in a combination of them: 1. The crystalline bodies have extremely small, invisible
facets at 10,000-times or even higher magnification, or 2. The content of the crystalline bodies of the new formations is negligible and can be detected only by the XRD method (Fig. 6). Measurements of EDS chemical compositions of newly formed material in two total areas, two small areas, and four points (Fig. 7) confirmed (Table 5) the results of the XRD and SEM methods. The absence of new crystalline forms determined by XRD, in the SEM images, and in the EDS results can be explained by the following reasons: 1. it is impossible to completely homogenize the components in the initial mixtures at the micro level; 2. The chemical composition in areas near the sol-gel formations may differ significantly from the bulk system composition; and 3. in accordance with the crystal chemistry law of Groth-Fedorow the number of possible phases in the intra-pore subsystem should be smaller than in the total system (syngony). Therefore, most likely, the extreme complexity of the chemical composition of the TSs under study does not allow the synthesis of new crystalline bodies - all possible crystals should already be present in the starting material. The presence of typical amorphous micro structures in SEM images was also confirmed through the results of the EDS analyses. The high carbon content can be explained by the C content in the organic materials in the sediment, by the calcium carbide in the LPW, and by the growth in the number of carbonates during the TS curing process. The results of the laser micro-mass analysis by the “LAMMA1000” (Fig. 8) are similar to results of the EDS analysis. All the isotopes' spectra obtained for the chemical compositions of all the nearest points of the new formations at the 180th curing day show quite dissimilar combinations of isotopes and their quantities (intensity of LAMMA peaks). New materials can be used as solid or holed bricks or as blocks. It
Please cite this article in press as: Mymrin, V., et al., Utilization of sediments dredged from marine ports as a principal component of composite material, Journal of Cleaner Production (2016), http://dx.doi.org/10.1016/j.jclepro.2016.10.035
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Table 5 Chemical compositions of areas and points (Fig. 7). Spectrum
Total area 1 Total area 2 Area 1 Area 2 Point 1 Point 2 Point 3 Point 4
Chemical composition, wt. % C
Na
Mg
Al
Si
Cl
K
Ca
Fe
Total
30.15 29.92 21.14 23.08 24.86 28.15 28.30 24.15
e e 1.25 1.07 1.12 0.81 e e
14.85 3.51 5.19 9.58 5.52 6.45 3.28 3.58
2.50 15.59 36.38 3.20 6.80 8.97 12.27 9.20
13.77 33.85 16.54 30.34 29.62 29.49 34.96 31.67
0.95 e 0.85 1.33 e 1.17 e e
e 3.10 2.13 1.50 1.84 1.70 3.87 3.48
35.64 6.33 14.33 17.90 22.33 19.02 8.42 13.83
2.14 7.70 2.19 12.0 7.91 4.24 8.90 14.0
100.0 100.0 100.0 100.0 100.0 100.0 100.0 100.0
Fig. 8. Set of isotopes of the composition 4 new formations at the 180th curing day by laser micro-mass analysis (LAMMA).
is possible to affirm, based on the considerable world technical literature, that materials developed in this study at the end of their service life can be successfully recycled as valuable and environment friendly components of new materials. Preliminary economic calculations of the bricks manufacturing cost showed a decrease of approximately 25% in comparison with conventional composites. This decrease is mostly achieved due to using dredged sediments, which can be obtained free of charge, as main component in the mixture. Indeed, near-shore utilization of dredge sediment may significantly reduce costs to dredging contractors, which add to value savings. Final calculations can be executed in each case depending on the specific conditions of production. 4. Conclusions 1. The possibility of using dredged sediment sediments of Atlantic Ocean ports as the main (up to 60 wt %) component of construction materials such as bricks and blocks without structural purposes was experimentally confirmed. Dredged sediments can be used in combination with construction and demolition waste (debris) in the amount of 20e35%, with lime production waste as a binder in the amount of 15e30%. 2. The mechanical properties of the developed materials attend the demands of Brazilian standards with values of the maximum uniaxial compressive strength of 6.3 MPa on the 3rd day of curing, 8.2 MPa on the 7th day, 11.0 MPa on the 14th day, 15.4 MPa on the 180th day, and continually increasing over time. The coefficients of linear expansion during curing vary between 0.07 and 0.35%, the water absorption varied between 11.1 and
13.4% after 28 days and between 11.0 and 13.3% on the 90th day of curing. 3. In moist and alkaline environments, the surfaces of as-received material particles are dissolved through a primarily amorphous process, with the synthesis of new sol-gel calcium silicate hydrates (CSH) in particle pores, as determined through the methods of XRD, XRF and SEM with EDS. The amorphous CSH new formations with the inclusion of amorphous and crystal bodies of minerals such as quartz, some carbonates (calcite and dolomite) and calcium silicates, which play the role of binder materials between the solid particles of the TSs. Their strengthening through the sol-gel process can explain the increasing uniaxial resistance of these materials up to the above mentioned values. 4. The techniques used to manufacture these new composites are relatively simple and economical because the materials used here do not require pretreatment such as drying, grinding, or other large transformation processes. 5. The main benefit from using the technology developed here at industrial scale is the avoidance of environmental degradation achieved through recycling large amounts of three types of waste as principal raw materials. The use of dredged sludge could reduce the degradation of Oceans and seas by stopping the current practice of ocean dumping. The utilization of construction and demolition waste and lime production wastes prevents the contamination of municipal and industrial landfills. The industrial use of these three types of waste can replace traditional raw materials, minimizing the extraction of natural resources by industry and the irreversible destruction of natural quarries.
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Acknowledgements The company DTA Engineering for their help in obtaining Port, LAMIR from UTFPR for dredged sediments in the Paranagua technical assistance in the XRF and XRD analyzes, the BOSCH branch in Curitiba for technical help in conducting SEM with EDS analysis, CAPES for the scholarships, and the head of the laboratory Gustavo Macioski (DACOC e UTFPR, Brazil). References Al-Khaja, W.A., Madany, I.M., Al-Sayed, M.H., Darwish, A.A., 2003. The mechanical and drying shrinkage properties of cement mortars containing carbide lime waste. Resour. Conserv. Recycl. 6, 179e190. Al-Sayed, M.H., Madany, I.M., Al-Khaja, W.A., Darwish, A.A., 2004. Properties of asphaltic paving mixes containing hydrated lime waste. Waste Manag. Res. 10, 183e194. E Antonina 2009. Site. http:// APPA, 2012. Administraç~ ao dos Portos de Paranagua www.portosdoparana.pr.gov.br/. n, B., Coz, A., Andre s, A., Viguri, J.R., 2009. Stabilization/solidification of Arce, R., Gala an alkyd paint waste by carbonation of waste-lime based formulations. J. Haz. Mat. 177, 428e436. Bennert, T., Papp, W.J., Maher, A., Gucunski, N., 2007. Utilization of construction and demolition debris under traffic-type loading in base and subbase applications. J. Transp. Res. Rec. 1714, 33e39. http://dx.doi.org/10.3141/1714-05. Bhatty, J.I., Gajda, J., 2004. Alternative materials. World Cem. 35 (12), 41e48. Brasil, 2009. Federal Government. PAC (Growth Acceleration Program), 2012. National Report. Infrastructure balance. Available at: http://www.brasil.gov.br/ pac/relatorios/nacionais/8o-balanco/parte-2c-infraestrutura-logistica (Accessed 12 May 2012). Brown, B.E., Letissier, M.D.A., Scoffin, T.P., Tudhope, A.W., 1990. Evaluation of the environmental impact of dredging on intertidal coral reefs at Ko Phuket, Thailand, using ecological and physiological parameters. In: Marine Ecology Progress Series, vol. 65. Oldendorf, pp. 3273e3281. Available in: http://md1.csa. com/partners/viewrecord.php?requester¼gs&collec tion¼ENV&recid¼23705 42&qenvironmentalþimpactþdredging&uid¼792071791&setcookie¼yes (Accessed 19 April 2013). Bulewicza, E.M., Jurysa, C., Kandefer, S., 2008. Flue gas desulphurization using lime waste, studies in environmental. Stud. Environ. Sci. 23, 589e595. CDRA-Construction & Demolition Recycling Association. http://www.cdrecycling. org/. CONAMA 454, 2012. National Council of Environment - CONAMA. Resolution No. 454, from 01 November 2012 and Lays Down the General Guidelines and Reference Procedures for Managing the Material to Be Dredged in Waters under National Jurisdiction. DOI publication of 08/11/2012, Section 1, p. 66. Available in: http://www.mma.gov.br/port/conama/legiabre.cfm?codlegi¼693 (Accessed 6 September 2013). ^a, S.M., Mymrin, V., 2005. New construction material from concrete producCorre tion and demolition wastes and lime production waste. Constr. Build. Mat. 21, 578e582. Do, H.S., Muna, P.H., Keun, R.S., 2007. A study on engineering characteristics of asphalt concrete using filler with recycled waste lime. Waste Manag. 28, 191e199. Dubois, V., Abriak, N.E., Zentar, R., Ballivy, G., 2008. The Use of Marine Sediments as a Pavement Base Material. Ecole des Mines of Douai, Civil Engineering de Sherbrooke, Faculty of Engineering, Quebec, Department, France; Universite es, France. Canada; Laboratoire Central des Ponts et Chausse Garcia, A., 2008. Cement and Lime Manufacturing Sector. General Inspection of Environment and Spatial Planning (Lisbon). Gutt, W., Collins, R.J., 1987. Sea-dredged Aggregates in Concrete. Building Research Establishment, Watford (UK).
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Hamer, K, Karius, V., 2002. Brick production with dredged harbor sediments. An industrial-scale experiment. University of Bremen. Germany Waste Manag. 22 (5), 521e530. Disponível em: http://www.sciencedirect.com/science/article/pii/ S0956053X01000484. Access in: 20/08/13. IBAMA, 2013. Available in:http://www.ibama.gov.br/publicadas/emitida-licencaprevia-do-ibama-para-dragagem-do-porto-de-paranagua-e-antonina. (Accessed 2 August 2013). ICES, 2011. Report of the Working Group on the Effects of Extraction of Marine Sediments on the Marine Ecosystem (WGEXT), 5e8 April, San Sebastian, Spain. 2005. ICES CM 2005/E: 06. 102 pp. Available in: http://www.ices.dk/reports/ mhc/2005/wgext05.pdf (Accessed 26 September 2012). Iler, R.K., 1979. The Chemistry of Silica. John Wiley & Sons Inc., USA., p. 866. Available in: http://www.amazon.com/Chemistry-Silica-SolubilityPolymerization-Biochemistry/dp/047102404X (Accessed 4 May2013). John, V.M., Rocha, J.C., Savastano Jr., H., Cincotto, M.A., 1996. Recycling of waste of building materials. In: Jonh, V.M., Cavalcante, J.R. (Eds.), Workshop on Waste Recycling and Reuse as Construction Material, S~ ao Paulo, anal/coord. EPUSP/ ANTAC, S~ ao Paulo, 1997, 184. Kay, H., Volker, K., 2002. Brick production with dredged harbour sediments. An industrial-scale experiment. Bremen. University of Bremen. Germany Waste Manag. 22 (5), 521e530. Available in: http://www.sciencedirect.com/science/ article/pii/S0956053X01000484 (Accessed 20 August 2013). Krause, P.R., McDonnell, K.A., 2000. The Beneficial Reuse of Dredged Material for Upland Disposal. HLA Project No. 4888. HLA (Harding Lawson Associates), Port of Long Beach. Long Beach, California. EUA, 23 pp. Available in: http://www. coastal.ca.gov/sediment/reusepaper.pdf (Accessed 16 August 2012). Kumar, S., 2003. Fly ash-lime-phosphogypsum hollow blocks for walls and partitions. Build. Environ. 38, 291e295. Leigh, N.G., Patterson, L.M., 2004. Construction & Demolition Debris Recycling for Environmental Protection and Economic Development. Practice Guide University of Louisville. EPA Region 4. Limeira, J., Etxeberria, M., Agullo, L., Molina, D., 2010. Mechanical and Durability Properties of Concrete Made with Dredged Marine Sand. Department of Construction Engineering, Polytechnic University of Catalonia, Barcelona, Spain. Marinkovic, S., Radonjanin, V., Malesev, M., Ignjatovic, I., 2010. Comparative environmental assessment of natural and recycled aggregate concrete. Waste Manag. 30, 2255e2264. Mymrin, V.A., 1998. Empleo de residuos industriales siderúrgicos como materiales n. Revista de Metalurgia, Madrid, pp. 34,441e445. aglomerantes en construccio http://revistademetalurgia.revistas.csic.es/index.php/revistademetalurgia/ article/viewFile/789/800. Mymrin, V., 2012. Industrial and Municipal Wastes Utilization as Economical and Environment Efficient Raw Materials. Available in. http://paginapessoal.utfpr. edu.br/mymrinev. NBR 6453, 2003. Building Quicklime - Requirements. Rio de Janeiro, 3. NBR 7170, 1983. Ceramic Solid Brick Masonry. Rio de Janeiro. NBR 8492, 2012. Soil-cement Brick. Dimensional Analysis, Compressive Strength Determination and Water Absorption. Test method. Rio de Janeiro. NBR 9778, 2009. Hardened Mortar and Concrete - Determination of Absorption, Voids and Specific Gravity. Pagliai, A.M.B., Cognetti Varriale, A.M., Crema, R., Curini Galletti, M., Vandini, R., 1985. Environmental impact of extensive dredging in a coastal marine area. Mar. Pollut. Bull. 16, 12,483e488. Fonte. http://www.sciencedirect.com/science/ article/pii/0025326X85903819. Rehmat, G.A., Mensinger, M.C., 2012. Remediation and Beneficial Reuse of PCB e Containing Waste Using the CEMENT-LOCK® TECHNOLOGY. Institute of GAS Technology, Chicago e USA, 1999. Available in: http://www.bnl.gov/wrdadcon/ publications/reports/GTI-FR-11-2008/AppendixD-CB-surrogate.pdf (Accessed 4 September 2012). Yozzo, D.J., Wilber, P., Will, R.J., 2004. Beneficial use of dredged material for habitat creation, enhancement, and restoration in New YorkeNew Jersey Harbor. J. Env. Manag. 73 (1), 39e52. Disponível em: http://www.sciencedirect.com/science/ article/pii/S0301479704001148 (Accessed 20 August 2013).
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Utilization of sediments dredged from marine ports as a principal component of composite material Vsevolod Mymrin*, Jacqueline C. Stella, Cristofer B. Scremim, Roberto C.Y. Pan, Filipe G. Sanches, Kirill Alekseev, Daniela E. Pedroso, Andrea Molinetti, Otavio M. Fortini Department of Civil Construction, Federal Technological University of Parana, St. Hector Alencar Furtado, 4900, Campus Curitiba, CEP: 81280-340, Ecoville, , Brazil Parana
a r t i c l e i n f o
a b s t r a c t
Article history: Received 30 April 2016 Received in revised form 6 October 2016 Accepted 9 October 2016 Available online xxx
The main purpose of this research is to develop technically, economically, and environmentally attractive construction materials from sediments dredged from Brazilian seaports. The final composite material contains 50 to 60 wt% in mass of sediments and thus creates an opportunity to diminish the pollution of the Atlantic Ocean. Construction and demolition debris (20e35%) and lime production wastes (15e30%) were used as components of the composite materials. Uniaxial compressive strength values reach 6.3 MPa on the 3rd day and 14.5 MPa on the 90th day; linear shrinkage varied between 0.07% and 0.35%, water absorption - between 11.0 and 13.4%. These values attend the demands of Brazilian norms on conventional bricks, blocks, etc. XRD, XRF, SEM, EDS, AAS and LAMMA analysis showed that amorphous new formations are responsible for material strengthening. © 2016 Elsevier Ltd. All rights reserved.
Keywords: Atlantic ocean pollution Dredging sediment utilization Structure formation processes Cement-less solid materials Mechanical properties Ocean environment protection
1. Introduction This study is dedicated to the development of construction material composites based on three industrial wastes: sediments dredged from ports on the Atlantic Ocean (SDS), construction and demolition debris (CDD), and lime production waste (LPW). The release of sediments from dredging of seaports is an old solution in practically every port worldwide (Brown et al., 1990; Pagliai et al., 1985). The disposal of large amounts of materials dredged from the port is a new, environmentally serious problem. For example, in the US, volumes of dredged sediment for the period from 2011 to 2018 were close to 2.4 million m3 annually (Krause and McDonnell, 2000; Rehmat and Mensinger, 1999). At the Port of Bremen, Germany, approximately 600,000 m3 of dredging sediment are removed annually (Kay and Volker, 2002). In Brazil alone, 80,313,000 m3 of sediment were dredged from ports in 2009 (Brasil, 2009). The main raw material source for this research was the sea port in Parana State, Brazil, which is the second most of Paranagua
* Corresponding author. E-mail address: [email protected] (V. Mymrin).
important port in Brazil. This port has a total area of 2,350,000 m2 with maritime access 150e200 m wide, 20 miles long, and 13e15 m deep (APPA, 2012). The volumes dredged from the ports of Para and Antonina in Parana State were 3,700,000 m3 in 2009; nagua 3 110,000 m in 2011; 3,700,000 m3 in 2012; and 8,000,000 m3 in 2013. These large amounts of sediment were sent to final offshore disposition in high seas (IBAMA, 2013; APPA, 2012, 2009). In Brazil, it is illegal to store of contaminated sediments in the ocean (CONAMA, Resolution 454, 2012). Therefore, the ability to reuse the dredged material in combination with contaminated debris would be a means to achieve legal compliance, reduce the amounts of material send to landfills, and an incentive to reduce maritime pollution (Yozzo et al., 2004). In the international scientific literature, there are many studies showing that dredged sediment can be used as a raw material for the development of different materials in construction (Gutt and Collins, 1987), the manufacture of concrete (Limeira et al., 2010), the construction of roads (Dubois et al., 2008), the production of bricks (Hamer and Karius, 2002), the construction and restoration of beaches and coastlines, for protection and land reclamation (ICES, 2011), and in the manufacture of glass tiles, cement blocks, bricks, etc. (Krause and McDonnell, 2000). The present study provides a new solution to this problem by
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offering a new, technologically simple and economically attractive method of disposing of SDS in combination with two other construction materials, which also considers industrial wastes: CDD and LPW. CDD includes aggregates such as bricks, concrete, plaster, glass, asphalt, tiles, gypsum wallboard, wood, metals, and different types of plastics. The Construction & Demolition Recycling Association (CDRA) states that in the USA, more than 325 million tons of CCD are produced annually. It makes up 25e45% of the waste that goes to USA landfills, thus contributing to the reduced life and increased environmental impact across the country (Leigh and Patterson, 2004). The most common and viable solution for the disposal of CDD is to incorporate them into the base and sub-base of road construction (Bennert et al., 2007). In the opinion of John et al. (1996) and Mymrin (2012), CDD can be used as the main raw material (up to 85 wt %) in different manufacturing construction materials, such as solid and hollow bricks or in compositions. Lime production waste (LPW) is poorly burnt lime, where the combustion process has not occurred at a sufficient temperature and to completion (Garcia, 2008), or is the result of burnt lime storage under inappropriate conditions (without sufficient insulation and air humidity). LPW can be used (Bhatty and Gajda, 2004) ^a and Mymrin (2005) used LPW as a by the cement industry. Corre waste concrete binder. Mymrin (2012) used LPW as a binder of many types of industrial wastes: phosphor-gypsum, cement, pulp for paper production, wastewater sludge, wood ash, steel slag, asbestos tiles, porcelain, and natural rock waste. Al-Sayed et al. (2004) and Do et al. (2007) determined that the use of LPW increases the physical and chemical properties of the asphalt mixture. Arce et al. (2009) employed LPW to immobilize the waste generated in the painting process. Al-Khaja et al. (2003) studied the use of LPW as a mineral aggregate in mortar mixtures. Bulewicza et al. (2008) reached over 70% desulfurization of flue gases from coal being burnt for power by incorporating to an LPW oven. Kumar (2003) and Marinkovic et al. (2010) made possible the use of LPW as raw material for the manufacture of bricks. The objectives of this research were to develop composite materials for civil construction using the dredged sediments contaminated with marine saltwater to achieve mechanical properties within Brazilian standards (NBR), research the physical and chemical processes of structure formation in these materials with predetermined properties, and decrease the cost of production of construction materials using three types of industrial wastes as raw materials, completely replacing traditional natural materials that have a much higher price. The ultimate goal of this research is to develop a technically, economically, and environmentally attractive construction material and thus create an opportunity to stop polluting the Atlantic Ocean with sediments dredged from Brazilian sea ports.
granulometric composition was determined by sieve and Wagner methods; the uniaxial resistance strength by uniaxial compression with an EMIC press model DL10,000; water absorption (WA) was measured with an Instrutherm BD 200, and the linear shrinkage (LS) with a Mitutoyo linear scale system. 2.2. Calculations The values of the water absorption coefficient (CWA) were determined on the 28th and 90th days of the TSs curing, following the Brazilian standards NBR 9778/2009 and NBR 8492, which uses the following equation: WA ¼ [(MSAT MD)/MD] 100,
(1)
where MSAT is the mass of the saturated TS after 24 h of immersion in water and MD is the mass of the TSs oven-dried at 100 C for 24 h. The values for the apparent density DA (g/cm3) are obtained by the equation DA ¼ PD/(PH PI),
(2)
where, PD is the mass of the TSs, PD is the dry mass of the TSs ovendried at 100 C (g), PH is the mass of the humid TSs oven-dried at 100 C (g), and PI is the mass of the humid TSs oven-dried at 100 C and immersed in water (g). 2.3. Raw materials A representative sample of the SDS was obtained with assistance from the company DTA Engineering during a harbor dredging at Paranagu a, Paran a state, Brazil. The area used for disposal of and Antonina material dredged (Fig. 1) from the ports of Paranagua is located more than 20 miles from Island of Galheta and the Island of Mel in the stretch. Bravo 1 (APPA, 2012). The CDD and LPW samples were collected in the enterprises of the metropolitan region of Curitiba, Brazil. 3. Results and discussion 3.1. Raw materials characterization Port The initial moisture content of the SDS from the Paranagua
2. Research methods and raw materials 2.1. Methods The raw and final materials were characterized by various complementary methods. The chemical composition was determined using X-ray fluorescence (XRF) with a Marc Philips/PAnalytical model PW 2400, and by atomic absorption analysis (AAA) with a Perkin Elmer 4100 spectrometer; the mineral composition was determined by X-ray diffraction (XRD) with a Philips machine model PW 1830; the morphological structure was analyzed with a scanning electron microscopy (SEM) FEI model Quanta 200 LV; the micro\chemical analysis by the method of energy dispersive spectroscopy (EDS) with an Oxford, Penta FET Precision model X-ACT, and by micro-mass analyses with a laser micro-mass analyzer LAMMA-1000 model X-ACT; the
, Brazil Fig. 1. Area of disposal of dredged material from sea ports of the state Parana (APPA, 2012).
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V. Mymrin et al. / Journal of Cleaner Production xxx (2016) 1e9
was 12.54% with a specific mass 2.54 kg/dm3, which is classified as normal (between 2 and 3 kg/dm3). The particle size distributions of the SDS and the CDD were obtained by sieving the materials, and the average result of the two samples of the materials show (Table 1) that most of the SDS (76.72%) are particles nearly 0.149 mm diameter, only 10.3% of particles being larger than 0.149 mm, and only 10.62% smaller than 0.149 mm. According to the Brazilian NBR 7211:2009 classification, such sand is included in the category of small sands. The smallest component is LPW containing about 85% of the particles smaller than 0.2 mm. The particle size distribution of the CDD is not as uniform because 73.23% of the CDD remains on the 0.42, 0.297 and 0.149 mm sieves. The sieve method shows that the largest SDS particles are seashell fragments, the percentage of which is reduced in finer fractions. The smaller fraction (0.42 mm and smaller) are mainly represented by sand with rare, small inclusions, of crushed seashells. Essentially, SDS has no clay and silt, which is explained by the repeated dredging of the port channel. The particle size distribution of LPW, determined by Wagner method of cone immersion, was near 1400 cm2/g. The chemical compositions of the raw materials (Table 2) determined through the XRF analysis shows that the SDS is mainly represented by SiO2 (71.0%), Al2O3 (10.1%), Fe2O3 (3.8%), K2O (3.4%), CaO (2.6%), Na2O (1.4%), MgO (1.1%) and SO3 (1.0%). CDD consists mainly of SiO2 (67.02%) and CaO 11.54%. The chemical composition of LPW (Table 2) includes 48.4% CaO and 25.18% MgO, with the impurity total content of SiO2 þ Al2O3 þ Fe2O3 equal to 2.3%. A carbonate content of 54.7% was determined from mass loss (24.1%) after calcination at 1,000 C of a sample pre-dried at 100 C, by recalculation to the formula of calcite CaCO3. The total levels of carbonates and the impurity content were 57.0%. Therefore, the peaks of calcite CaCO3 have two maximum intensities in the diffractogram pattern (Fig. 2-C). The Brazilian standard NBR 6453 (2003) enables the use of quicklime with a maximum content of impurities and limestone of 12% as a binder in construction. Because of this limitation, the material used should be called “lime production waste” (LPW). The presence of calcium carbide CaC2 is due to the firing of limestone in an open fire. The mineralogical composition of the SDS determined by XRD (Fig. 2-A) includes quartz SiO2, microcline KAlSi3O8 and halite NaCl; CDD was determined (Fig. 2-B) to include quartz (SiO2), calcite (CaCO3) and albite (Na,Ca)(Si,Al)4O8. Mineral composition of LPW (Fig. 2-D) is presented by quicklime CaO, portlandite Ca(OH)2, calcite CaCO3, magnesite MgCO3 and quartz SiO2. The presence of significant amounts of amorphous materials in the diffractogram patterns is also evident. In the SEM images of the SDS (Fig. 3-C), classic hex-octahedron forms typical of halite are clearly visible. EDS analysis of these
4.8 2.4 1.2 0.6 0.42 0.297 0.149 0.075 <0.075 Total
Content of fractions, % CDD
SDS
0 0 0 10.45 17.33 26.78 29.12 9.71 6.20 99.73
0.09 0.13 0.39 1.32 2.91 5.46 76.72 8.58 4.04 99.63
Table 2 Chemical composition of raw materials used (by method of XRF). Elements
SiO2 Al2O3 CaO MgO Fe2O3 TiO2 SO3 P2O5 Na2O MnO K2O Cl C.L.
Chemical composition, wt % SDS
CDD
LPW
71.0 10.1 2.6 1.1 3.8 0.8 0.1 0.1 4.5 0.1 3.4 0.6 3.6
67.02 6.3 11.54 1.37 3.85 0.64 0.58 0.11 0.29 e 0.67 e 7.57
1.89 0.19 48.41 25.18 0.23 e e e e e e e 24.07
C.L. e Calcination Loss.
crystalline bodies confirmed this assumption (Table 3, points 1e4). The morphological structure of the SDS shows rather rounded grains, without sharp edges, of sand (Fig. 3 - A and B) of similar dimensions. In the photo at 1000-times magnification (Fig. 3-B), abrasion of sand particle surfaces is clearly visible, including peeling as a result of friction during the millions of years of geological history of each particle. Such abrasion may enhance the dissolution of the surface layer in an alkaline environment (Iler, 1979), especially in the early stages of hydration of the initial mixture, with the formation of groups of amorphous minerals of calcium silicate hydrate (CSH). The synthesis of these amorphous minerals significantly increases the mechanical properties of the materials developed in this research (Mymrin, 1998). The micro chemical compositions of the SDS sample obtained by the EDS method (Table 3) are in good agreement with the results of the XRF (Table 2). The slight discrepancies in them can be attributed to differences in the sensibility of the research methods and of the methods of the TSs preparation. The substantial complexity in mineral composition at the micro level is confirmed by the EDS analysis of smaller surface areas (1e3, Fig. 3-C) at all points 1e4. The analysis of these areas is substantially different from the analysis obtained with bulk-methods such as XRD (Table 2) and XRF. The particles of the CDD micro-level (Fig. 4 e A and B) have greater dimensions and variety of sizes and therefore lower porosity between them. The chemical composition of the CDD obtained by EDS also includes SiO2 (67.0%) as the main component as well as CaO (11.5%), Al2O3 (6.3%), Fe2O3 (3.9%), and MgO (1.4%); the other elements have levels lower than 1%. The LPW particles (Fig. 4 - C and D) have different shapes and sizes but are rounded, which is typical for amorphous substances. 3.2. Preparation of test samples (TSs)
Table 1 Granulometry compositions of CDD and SDS. Sieve, mm
3
Estimate visual of SDS
Shells Shells 90% shells 50% shells 20% shells 5% shells Sand Sand Sand þ Silt
The preparation of the TSs includes the following operations: collecting representative samples, sieving with a 1.19 mm mesh sieve, weighing in advance certain percentages (Table 4), mixing and homogenization of the components, hydrating and compacting the cylindrical samples to a height and diameter of 20 mm at 10 MPa pressure and curing the TSs in open air. The following properties of the TSs were investigated after 3, 7, 14, 28, 60, 90, and 180 days by means of mechanical properties: the uniaxial compression strength, linear expansion, water absorption and density. The values of the mechanical properties and standard deviation were obtained as an average of 10 sample measurements; therefore, the total quantity of the TSs was 540 pieces.
Please cite this article in press as: Mymrin, V., et al., Utilization of sediments dredged from marine ports as a principal component of composite material, Journal of Cleaner Production (2016), http://dx.doi.org/10.1016/j.jclepro.2016.10.035
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V. Mymrin et al. / Journal of Cleaner Production xxx (2016) 1e9
Fig. 2. Diffractogram patterns of the raw materials used: A e SDS, B e CDD, C e LPW.
Fig. 3. SEM micro images of the SDS with different magnifications.
Table 3 Chemical micro analyses by EDS method of areas and points of SDS (Fig. 3). Spectrum
Values of elements, wt % C
Na
Mg
Al
Si
Cl
K
Fe
Total
Total area Point 1 Point 2 Point 3 Point 4 Area 1 Area 2 Area 3
20.37 31.86 31.08 e 29.19 32.26 32.90 30.97
4.43 24.13 22.26 33.20 24.14 1.43 e 1.34
1.53 e e e 0.59 1.41 0.64 e
10.33 0.46 1.18 0.96 1.15 7.79 1.41 1.70
34.58 1.68 5.16 3.32 3.44 41.46 62.93 59.48
11.64 41.87 39.57 61.35 40.21 4.37 2.13 4.09
12.96 e 0.76 0.47 0.28 9.32 e 0.83
4.17 e e 0.70 1.00 1.97 e 1.60
100.00 100.00 100.00 100.00 100.00 100.00 100.00 100.00
3.3. Mechanical properties of TSs The values of the uniaxial compressive strength of the TSs (Fig. 5) increase in open air and regularly depend on the cure time and the amount of the binder e the LPW. The higher compressive strength of the TSs at all stages of hydration and curing are found for composition 4 with LPW content of 30%. On the 3rd day of curing, the resistance reached 6.3 MPa; on day 7, 8.2 MPa; on day 28, 13.7 MPa; and on day 180, 15.4 MPa. According to NBR 7170, the uniaxial strength of the fired solid bricks shall be as follows: class A < 1.5 MPa, Class B < 2.5 MPa, Class C < 4.0 MPa. On the 3rd day of curing without firing, the strength (6.3 MPa) of composite material 4 exceeded the demands of Class C by 1.58 times, on the 14th day (11.04 MPa) by 2.06 times and on the
180th day (15.39 MPa) by 3.85 times. After 7 days of curing, the values of mechanical strength of all TSs were above the requirements of Class A standard values, and on the 180th day of curing, all compositions met the requirements of Class C. The lower strength values in all ages of hydration were determined in compositions 1 and 5 to be a result of their lower concentration of LPW (15%). Among them, the highest values of resistance, except on the 3rd and 180th days, belong to composition 1, which had a lower content of SDS (50% versus 60%) and higher content of CDD (35% versus 25%). It appears that 15% LPW is not sufficient to neutralize the existing acid salts (Fig. 3-E and F) in 60% SDS (composition 5) water, but replacing 10% SDS by 10% CDD (composition 1) can improve the resistance values, especially until 90 days of curing. However, between compositions 2 and 6 with 20% LPW, most of the best resistance values belong to composition 6, although with higher levels of SDS (60% vs. 50%) and lower levels of CDD (20% vs. 30%). This may mean that the 20% LPW compared to 15% LPW is less sensitive to substituting 10% CDD by 10% SDS. The increase in LPW content to 25% (composition 3) provided high strength (4.1 MPa) on the 7th day of hydration and 8.9 MPa on the 180th day of curing. The TSs of all the compositions shows very low and highly unstable dilatation values (between 0.07 and 0.96%) during curing. A common tendency was the increase in values until the 28th day of curing, with a slow decrease until the 180th day. The TSs of composition 4 had the lowest amplitude changes between 0.07 and 0.20%, which confirms the stability of the processes of hydrating
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Fig. 4. SEM micro images of the CDD and LPW at different magnifications.
Table 4 Substantial compositions of materials under study. NO
1 2 3 4 5 6
Compositions, wt. % SDS
CDD
LPW
50 50 50 50 60 60
35 30 25 20 25 20
15 20 25 30 15 20
and curing the material. The apparent average density of the TSs of composition 4 on day 3 was 1.748 kg/m3, on day 14, it increases up to 1.795 kg/m3, after 60 days, up to 1.834 kg/m3 and after 180 days, to 1.881 kg/m3. Such changes in the values of the density and of the dilatation of the TSs indicate an increase in the amount of new growths in pore space and reinforcing to 15.39 MPa until 180 days of hydration. 3.4. Physical processes of chemical structure formation The physical and chemical processes of interaction between the hydrated and compacted raw materials accompanying the formation of structures in the new materials were investigated by means of XRD, SEM with EDS and LAMMA methods in the TSs of composition 4, due to high mechanical properties of the samples. 3.4.1. Changes of mineralogical composition Deciphering the X-ray diffractogram patterns (Fig. 6) of the
material at different ages with numerous mineral components is rather difficult because of their coinciding peaks. However, it is possible to discuss some peaks that are free of such coincidence and which changed intensities during the material curing. The intensities of the portlandite peaks are constantly decreasing during the cure time. The peaks of calcite, on the contrary, are increasing in intensity, some of them appear on the 28th day, others appear and on the 60th day, or even only on the 180th day. Therefore, it is possible to surmise the existence of carbonates under the amorphous condition as well. In the initial mix of composition 4, quartz SiO2 is the principal mineral (Fig. 6-A); at higher magnifications of the diffractogram pattern, it is clearly visible that almost all quartz XRD peaks have duplications. These duplications appeared due to processes of the mechanical destructions (cracks, exfoliations, abrasions, etc.) during the geological history of the SDS sand particles. After the dissolution of these defective layers on the sand grains in a high alkaline environment (close to pH ¼ 13), the intensities of the peaks of quartz increased since more perfect surfaces of the mineral structure were exposed. For large amounts of free CaO in the LPW and the CDD, this dissolved amorphous SiO2 can precipitate as in sol-gel synthesis of amorphous materials with unstable chemical composition. As shown elsewhere, such as calcium silicate hydrates CSH becoming a binder between the solid particles of the material (Mymrin, 1998). The role of CSH formations is well-known in the chemistry of hydrated Portland cement. The growth of crystalline and amorphous substances of carbonates and CSH formation may be responsible for the gain in mechanical properties of the materials developed.
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V. Mymrin et al. / Journal of Cleaner Production xxx (2016) 1e9
Fig. 5. Change of uniaxial compressive strength values during the curing.
Fig. 6. Comparison of XRD patterns of the composition 4: A - Initial dry mixture, B - on the 28th day, C - on the 60th, D - on the 180th day of hydration.
3.4.2. Processes of structure formation The structure of the initial dry composition 4 by the SEM method (Fig. 7) shows particles with a wide variety of sizes and shapes. In Fig. 7-A at 50-times magnification, numerous and protruding rounded particles of relevant dimensions emerge from the surface layer of the TSs, which are very smooth and dense. However, at 1000- and 5000-times magnification, the presence of large
numbers of pores between particles of different sizes, depths and configurations becomes especially visible. In the images of the 28th day of curing structure (Fig. 7-A, B and C), there are differences in the morphological structure compared to the non-hydrated sample (Figs. 3 and 4). In the image at 500times magnification (Fig. 7-A), in contrast to Fig. 3-A, the sand particles were not visible because they were covered by the layer of
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Fig. 7. SEM micro images of the TSs' structure of the composition 4: A, B and C on the 28th day; D, E and F e on 180th day of cure.
new formations. These new formations effectively cover and act as links between particles. Images at 3000-times magnification (Fig. 7-B) there showed a much denser structure with few string fissures. These changes in the structure of the material may explain the growth of the uniaxial resistance up to 11.0 MPa during the 28 days of curing (Fig. 5). At 6000-times magnification (Fig. 7-C), pore sizes from 5 to 10 mm were observed. The pore chains are linked to each block of material and connected to the large particle size below the coverage of new formations. In Fig. 7-C, the remains of organic material of plant origin can be observed. These materials do not interact chemically with other components of the mixture, and, therefore, during the endurance tests of the TSs, they most likely promoted the development of cracks, thereby significantly reducing the mechanical properties of the materials. It is quite possible that a preliminary separation of plant materials can significantly increase the strength values of the material. The representative images of the TSs structure on the 180th day (Fig. 7-D, E and F) demonstrate the further increasing of the density of the material structure compared to samples on the 28th day: it had almost no pores and cracks and was similar to the images of dense concrete. Only the images at 5000-times magnification show networks of micro pores with diameters from 0.1 to 0.2 mm and rare micro pores with a diameter of 1 mm. Virtually all of them are connected to each other, and most of them are gathered in dense layers without pores or with small and superficial pores.
3.4.3. Chemical composition of new micro formations During the SEM analysis, non-crystalline bodies were found through XRD. This is possible in two variants or in a combination of them: 1. The crystalline bodies have extremely small, invisible
facets at 10,000-times or even higher magnification, or 2. The content of the crystalline bodies of the new formations is negligible and can be detected only by the XRD method (Fig. 6). Measurements of EDS chemical compositions of newly formed material in two total areas, two small areas, and four points (Fig. 7) confirmed (Table 5) the results of the XRD and SEM methods. The absence of new crystalline forms determined by XRD, in the SEM images, and in the EDS results can be explained by the following reasons: 1. it is impossible to completely homogenize the components in the initial mixtures at the micro level; 2. The chemical composition in areas near the sol-gel formations may differ significantly from the bulk system composition; and 3. in accordance with the crystal chemistry law of Groth-Fedorow the number of possible phases in the intra-pore subsystem should be smaller than in the total system (syngony). Therefore, most likely, the extreme complexity of the chemical composition of the TSs under study does not allow the synthesis of new crystalline bodies - all possible crystals should already be present in the starting material. The presence of typical amorphous micro structures in SEM images was also confirmed through the results of the EDS analyses. The high carbon content can be explained by the C content in the organic materials in the sediment, by the calcium carbide in the LPW, and by the growth in the number of carbonates during the TS curing process. The results of the laser micro-mass analysis by the “LAMMA1000” (Fig. 8) are similar to results of the EDS analysis. All the isotopes' spectra obtained for the chemical compositions of all the nearest points of the new formations at the 180th curing day show quite dissimilar combinations of isotopes and their quantities (intensity of LAMMA peaks). New materials can be used as solid or holed bricks or as blocks. It
Please cite this article in press as: Mymrin, V., et al., Utilization of sediments dredged from marine ports as a principal component of composite material, Journal of Cleaner Production (2016), http://dx.doi.org/10.1016/j.jclepro.2016.10.035
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V. Mymrin et al. / Journal of Cleaner Production xxx (2016) 1e9
Table 5 Chemical compositions of areas and points (Fig. 7). Spectrum
Total area 1 Total area 2 Area 1 Area 2 Point 1 Point 2 Point 3 Point 4
Chemical composition, wt. % C
Na
Mg
Al
Si
Cl
K
Ca
Fe
Total
30.15 29.92 21.14 23.08 24.86 28.15 28.30 24.15
e e 1.25 1.07 1.12 0.81 e e
14.85 3.51 5.19 9.58 5.52 6.45 3.28 3.58
2.50 15.59 36.38 3.20 6.80 8.97 12.27 9.20
13.77 33.85 16.54 30.34 29.62 29.49 34.96 31.67
0.95 e 0.85 1.33 e 1.17 e e
e 3.10 2.13 1.50 1.84 1.70 3.87 3.48
35.64 6.33 14.33 17.90 22.33 19.02 8.42 13.83
2.14 7.70 2.19 12.0 7.91 4.24 8.90 14.0
100.0 100.0 100.0 100.0 100.0 100.0 100.0 100.0
Fig. 8. Set of isotopes of the composition 4 new formations at the 180th curing day by laser micro-mass analysis (LAMMA).
is possible to affirm, based on the considerable world technical literature, that materials developed in this study at the end of their service life can be successfully recycled as valuable and environment friendly components of new materials. Preliminary economic calculations of the bricks manufacturing cost showed a decrease of approximately 25% in comparison with conventional composites. This decrease is mostly achieved due to using dredged sediments, which can be obtained free of charge, as main component in the mixture. Indeed, near-shore utilization of dredge sediment may significantly reduce costs to dredging contractors, which add to value savings. Final calculations can be executed in each case depending on the specific conditions of production. 4. Conclusions 1. The possibility of using dredged sediment sediments of Atlantic Ocean ports as the main (up to 60 wt %) component of construction materials such as bricks and blocks without structural purposes was experimentally confirmed. Dredged sediments can be used in combination with construction and demolition waste (debris) in the amount of 20e35%, with lime production waste as a binder in the amount of 15e30%. 2. The mechanical properties of the developed materials attend the demands of Brazilian standards with values of the maximum uniaxial compressive strength of 6.3 MPa on the 3rd day of curing, 8.2 MPa on the 7th day, 11.0 MPa on the 14th day, 15.4 MPa on the 180th day, and continually increasing over time. The coefficients of linear expansion during curing vary between 0.07 and 0.35%, the water absorption varied between 11.1 and
13.4% after 28 days and between 11.0 and 13.3% on the 90th day of curing. 3. In moist and alkaline environments, the surfaces of as-received material particles are dissolved through a primarily amorphous process, with the synthesis of new sol-gel calcium silicate hydrates (CSH) in particle pores, as determined through the methods of XRD, XRF and SEM with EDS. The amorphous CSH new formations with the inclusion of amorphous and crystal bodies of minerals such as quartz, some carbonates (calcite and dolomite) and calcium silicates, which play the role of binder materials between the solid particles of the TSs. Their strengthening through the sol-gel process can explain the increasing uniaxial resistance of these materials up to the above mentioned values. 4. The techniques used to manufacture these new composites are relatively simple and economical because the materials used here do not require pretreatment such as drying, grinding, or other large transformation processes. 5. The main benefit from using the technology developed here at industrial scale is the avoidance of environmental degradation achieved through recycling large amounts of three types of waste as principal raw materials. The use of dredged sludge could reduce the degradation of Oceans and seas by stopping the current practice of ocean dumping. The utilization of construction and demolition waste and lime production wastes prevents the contamination of municipal and industrial landfills. The industrial use of these three types of waste can replace traditional raw materials, minimizing the extraction of natural resources by industry and the irreversible destruction of natural quarries.
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Please cite this article in press as: Mymrin, V., et al., Utilization of sediments dredged from marine ports as a principal component of composite material, Journal of Cleaner Production (2016), http://dx.doi.org/10.1016/j.jclepro.2016.10.035