1. Introduction
Water treatment sludge (WTS) is the residue generated at water treatment plants (WTPs) by the regular washing of decanters and filters. The main treatment processes to transform raw water into potable water in a conventional WTP are coagulation, flocculation, decantation, filtration, pH correction, disinfection, and fluoridation. During these processes, several chemicals are added to the water, e.g., chlorine, coagulants, lime, and fluorine. Coagulants (ferric, alum, polymeric) cause impurities to accumulate at the bottom of sedimentation basins and filters, which are periodically washed, producing WTS. Considering that WTS generation amounts to 0.2% to 5% of the volume of treated water [
1] and the estimated increase in global demand for potable water is of 1% per year [
2], WTS figures as a major waste stream, presently and for the foreseeable future.
WTS is composed of more than 97% water, chemical compounds from the treatment process, and suspended solids, mainly soil particles—sand, silt, and clay, but may also present organic matter, algae, bacteria, and viruses. Dewatering usually raises the solids content to 20–30%, which corresponds to 250–400% gravimetric water content, i.e., a suspension.
In most developing countries, WTS is still released in water bodies—a practice no longer allowed in countries with sound environmental regulations—causing silting and deterioration of water quality. Environment-friendly alternatives, such as disposal in sanitary or dedicated landfills or discharge in sewage treatment plants (STPs), still pose sustainability concerns: WTS impairs the structural stability of sanitary landfills and overloads STPs, by themselves insufficient in most developing countries, while dedicated landfills conflict with the global environmental goal of reducing land disposal of waste. On the other hand, reuse may introduce WTS in the circular economy and also substitute natural resources in several production processes. The percentage of reused or recycled WTS is an indicator proposed by the standard ISO 24512:2007 for the evaluation of water supply services management. Sustainable management of WTS is also encompassed by UN Sustainable Development Goal 6—Water and Sanitation [
3].
Some techniques aiming at WTS reuse have been investigated: precast concrete elements, brick, ceramic, and cement production [
4,
5,
6,
7,
8]; composting [
9]; removal of phosphorous from residual waters [
10,
11,
12]; crop production [
13] and forestry [
14]; absorption of heavy metals [
15,
16]; coagulant recovery [
17,
18]; landfill lining [
19,
20]; geotechnical material [
21,
22,
23,
24], among others. Reviews about the beneficial reuse/recycling alternatives for WTS have been presented by some authors [
25,
26,
27]. Despite the significant number of studies, worldwide cases of WTS reuse are rare in the literature. Novel management practices, such as agriculture, forestry, land reclamation, incorporation into soils, soil improvement, and incorporation into construction materials have been reported in the 2000s by governmental agencies in some countries (e.g., UK, Japan, France, Germany, USA), still representing low percentages of the total mass generated. However, information has not been updated in recent years on the respective websites or in regulations or technical reports. Reuse of wastewater and sewage sludge, i.e., biosolids, which are much more voluminous and with a wider range of applications, may have overshadowed the use of WTS. This does not mean that WTS reuse is not taking place; for example, WTS is used as an additive for sewage treatment in Portugal, and USEPA established directives for WTS reuse in 2011. Developing countries, however, still need sound research to enhance WTS reuse under their specific conditions and need information on the performance of practical applications already under way. Though still scarce, research on the geotechnical properties and practical applications of WTS has increased in the last years. This paper investigates the feasibility of employing WTS at as-collected water content in geotechnical applications, such as covers and bottom liners of sanitary and industrial landfills, backfill for trenches, bridge abutments and geosynthetic-reinforced earth walls, pavement and buildings subbases, reinforcement for soft soils, and embankments. Additionally, it discusses the sustainability of this approach based on experimental results, aiming at the beneficial reuse of waste and the preservation of natural geomaterials.
Two approaches are envisaged: (1) the partial substitution of soils with adequate geotechnical properties by WTS in order to preserve natural resources; (2) the mixing of WTS with additives to design a new geomaterial, aiming at beneficial reuse.
WTS addition may reduce the shear strength, increase the compressibility, or impair the workability of soils; therefore, the maximum allowable content of WTS was sought in the first approach. Two sludges and two soils were mixed in different proportions, and geotechnical properties were determined for the mixtures.
The second approach investigated WTS-additive mixtures that could reach a minimum undrained strength for workability and spreading in the field. In this case, a sludge was mixed separately with lime and rock powder to obtain a workable material for applications involving low soliciting stresses. Experimental adaptations to deal with materials with shear strength lower than that of soft clays are presented. The scientific background to integrate rheology into geotechnical tests discussed in [
28] is here first applied to WTS. Subsequent steps will be to produce materials with good geotechnical properties for general earthworks.
The experimental results of both approaches are finally discussed in the light of technical feasibility, as well as environmental, economic, and social sustainability. The discussion perspective focuses on developing countries, where environmental regulations and new business models for water and sanitation are still being implemented.
The new approaches and the scientific contribution of this research are (1) the geotechnical utilization of as-collected WTS, without any previous treatment such as drying or chemical addition, which would drastically reduce the economic feasibility of reuse (air or oven-drying improves the geotechnical properties of WTS, but is time, space, and energy consuming); (2) the determination of geotechnical properties for multipurpose applications—while most investigations are directed toward a specific use and therefore may discard suitable materials for geotechnical applications other than those previously envisioned, the multipurpose approach can itself indicate the best alternative of reuse; and (3) the integration of geotechnical and rheological tests to understand the behavior of geomaterials and to discuss new possibilities of transport and manipulation in the light of sustainability.
2. Materials and Methods
2.1. Materials
Two WTSs were investigated, Cubatão-WTS and Taiaçupeba-WTS, both generated at conventional-treatment WTPs located in São Paulo State, Brazil (
Figure 1). Samples of both WTSs were collected directly after centrifuge dewatering. The protocol to obtain representative samples was designed according to the Theory of Sampling [
29].
Cubatão-WTP collects raw water with turbidity of 800 NTU from the Cubatão River and supplies 4.5 m3/s of potable water to a 1.5 million population. The water passes through desanders before being submitted to the conventional treatment, which uses ferric chloride as a coagulant. WTS produced by washing sedimentation basins and filters is sent to a thickening tank (2% to 4% solids) and then dewatered by centrifuges, generating circa 60 tons/day of WTS with 20% to 25% solids. Cubatão-WTS is presently sent to a private waste disposal site.
Taiaçupeba-WTP collects raw water from the Taiaçupeba reservoir and produces 15 m3/s of potable water for the São Paulo Metropolitan Region (21 million inhabitants). The coagulation process employs aluminum sulfate and a polymer (superfloc 8392). Residues collected from the sedimentation basins and filters backwashing are sent to an equalization tank (2% solids content), then to a thickening tank (4% solids content), and finally to centrifuges (16% to 18% solids content). WTS is further air-dried and disposed of in engineered cells inside the WTP or sent to an external landfill.
Two tropical lateritic soils widely used in geotechnical works were selected for the research: Botucatu clayey sand and Campinas clay, both largely occurring soils in Sao Paulo State, Brazil. Additives were a commercial high-purity calcium hydrated lime and granite–gneiss rock powder collected in a quarry in Cubatão, São Paulo State.
All mixtures were prepared with WTS at as-collected water content (after centrifuge-dewatering), and soils, lime, and rock powder were prepared at hygroscopic water content. Soils were air-dried, a usual practice in soil mechanics laboratories, while lime and rock powder were already obtained in a dry state. The proportions of WTS and mixed material by wet mass were selected according to an arbitrary criterion of workability/compactability of the resulting mixture. For the analysis of test results, WTS content was expressed by dry mass basis (mass of WTS solids divided by mass of soil, lime, or rock powder solids).
Three soil:WTS ratios by wet mass were selected between 1.5:1 and 5:1, resulting in 12 different mixtures. Four lime:WTS ratios by wet mass, varying between 1:1 and 1.5:1, and four rock powder:WTS ratios, between 1:1 and 5:1, were also tested. Mixtures were named with letters sequentially indicating soil or additive, WTS, and soil:WTS or additive:WTS ratio, as presented in
Table 1.
2.2. Chemical and Mineralogical Characterization of the Investigated Materials
Chemical composition was obtained by X-ray fluorescence using a spectrometer (Axios-Advanced PANalytical; standardless analysis from fluor to uranium) and loss-on-ignition (LOI) at 1020 °C for two hours. Analyses were carried out on powder of oven-dried samples (35 °C). Concentrations of elements were semiquantitative and presented in the form of oxides normalized to the value of 100%. Chemical parameters, pH in water and KCl, P, K, Ca, Mg, Al, Al+H, exchangeable bases, cation exchange capacity, saturation by exchangeable bases, saturation by aluminum, organic carbon, and organic matter by titrimetric method were determined using air-dried samples according to methods of the Brazilian Agricultural Research Corporation [
30]. In order to determine organic matter content, 100 g samples were oven dried at 105 °C and then ignited using a muffle furnace at 440 °C during 24 h, in accordance with ASTM D2974 standard.
Mineral composition was determined by X-ray diffraction using Phillips diffractometer MPD 1880 and scanning electron microscopy (SEM) using FEI Quanta m600 FEG microscope, equipped with a Bruker X-ray energy dispersion spectrometer (EDS) Quantax 400 (technology SDD—Silicon Drift Detector) and data analysis using Sprit software. The analyses were conducted on samples oven-dried at 35 °C. Crystalline phases were identified by comparing obtained diffractograms with those of the International Centre of Diffraction Data and the PANalytical Inorganic Crystal Structure Database. Microscopic analyses were carried out by collection of backscattered electron images and specific chemical analyses by EDS for the compositional characterization of particles. The SEM analyses were conducted on pulverized samples (powder) glued to a double-sided carbon tape and coated with platinum.
2.3. Geotechnical Characterization of the Materials
Geotechnical characterization comprised determination of water content (w), particle-size distribution (PSD), liquid limit (wL) and plastic limit (wP), specific gravity of solids (Gs), and organic matter content (OM), following ASTM standards: ASTM-D2974-14, ASTM-D422-07, ASTM-D4318-17, ASTM-D854-14, and ASTM-D2974-14, respectively.
For the sludges, solids content (SC) and dehydration over time were also determined: 2 kg samples were air-dried and monitored over time until reaching the residual water content. Water content was determined at 105 °C following the recommendation of [
31] for organic sludges. For the other characterization tests, WTS samples were tested at as-collected water content since several authors have reported significant alterations in WTS caused by previous air-drying [
32,
33,
34,
35]. Atterberg limits were determined by the wet method (from wet to dry) following ASTM D4318-17. PSD of the sludges was also determined by laser analyses using wet and dry (powder) samples.
2.4. Geotechnical Properties of the Investigated Materials
Compaction tests at standard Proctor effort followed ASTM-D698-12e2 with air-dried samples (Method A) and material reuse (necessary due to the great number of compaction tests since each test uses ~3 kg of material). Compaction of additive:WTS mixtures was carried out after previous drying to hygroscopic moisture. Compaction of soil:WTS mixtures was carried out with and without previous drying. Refs. [
35,
36] showed that previous air-drying alters compaction parameters (maximum dry unit weight and optimum water content) of soil:WTS mixtures and that there is a linear correlation between compaction parameters and desiccation ratio, defined according to Equation (1). Compaction tests for each soil:WTS mixture were conducted at three different desiccation ratios.
where w
0 = as-mixed water content, and w
i = water content after air-drying.
Soils and soil:WTS mixtures specimens were submitted to oedometric compression, permeability, unconfined compression, and triaxial compression tests. Specimens were compacted at optimum compaction parameters at Proctor standard effort. However, some mixtures (those with higher WTS content) were tested at as-mixed moisture, as they already were slightly wet-of-optimum. Additive:WTS mixtures were submitted to unconfined compression tests on specimens compacted at as-mixed water content at Proctor standard effort. When the stress–strain curve did not present a peak, i.e., the axial stress continuously increased with strain, the adopted failure criterion was 15% (maximum) deformation.
Oedometric compression tests were carried out according to ASTM- D2435-11a, with the specimen inside a stainless-steel ring of 71.3 mm diameter and 20.0 mm height, inundation with distilled water at initial loading, incremental loading (load increment ratio of 1), subsequent unloading, and loading interval of 24 h. The applied vertical stresses were: 10, 20, 40, 80, 160, 320, 640, 1280, and 2560 kPa.
The hydraulic conductivity of compacted soils and soil:WTS mixtures was determined by constant head permeability tests in flexible-wall permeameter, following ASTM-D5084-16, with specimens of 70 mm height and 70 mm diameter. Saturation was achieved by backpressure ranging from 500 to 700 kPa to reach B-value equal or higher than 0.96.
For each soil and soil:WTS mixture, isotropically consolidated undrained (CIU) triaxial compression tests with measurement of pore pressure were carried out with confining pressures of 50, 100, and 200 kPa on specimens of 38 mm diameter and 76 mm height, following ASTM-D4767-11. The undrained strength was defined as the maximum deviator stress till axial strain of 17%.
Unconfined compression tests were carried out following ASDTM-D2166-16 at 1.0 %/min strain rate with triplicate specimens of 50 mm diameter and 50 mm height (compacted by mini-MCV equipment) for each material. Since the L/D ratio of the specimens was 1, a correction factor of 0.69 was applied to the maximum axial stress in order to obtain the equivalent axial stress for L/D = 2, based on the correction equation suggested by [
37].
where UCS
(L/D = 2) = standard unconfined compression strength, and UCS
(L/D) = measured UCS for tested samples with L/D ratio.
2.5. Environmental Characterization of Cubatão-WTS and Taiaçupeba-WTS
The environmental characterization of Cubatão-WTS was based on the chemical analysis of four different samples submitted to X-ray fluorescence in two laboratories. The Brazilian standard for waste classification NBR 10,004 [
38] uses specific properties (radioactivity, inflammability, pathogenicity, and corrosivity) or results of solubilization and leaching tests to classify waste in three classes—hazardous, non-hazardous non-inert, and non-hazardous inert. NBR 10,004 implicitly considers WTS, municipal solid waste, and sewage treatment sludge as non-hazardous non-inert. Even so, since the quality of the raw water of Taiaçupeba Reservoir posed some concern, solubilization and leaching tests were carried out for Taiaçupeba-WTS following Brazilian standards NBR 10,006 [
39] and NBR 10,005 [
40], respectively. Ongoing research aims to analyze the chemical impact of WTS reuse at each specific geotechnical application.
Biological characterization of WTS is not required yet, despite the probable presence of microorganisms, hormones, and nano plastics that are not destroyed by the conventional treatment. Further research is necessary to address this topic.
2.6. Rheological Behavior of Cubatão-WTS
A sample of Cubatão-WTS at water content of 240% (solids content of 30%) was mechanically mixed for 1 min at 10,000 rpm before the rotational rheometry tests. Stepped flow tests were performed using a Haake Mars 60 Rheometer with steel parallel plate geometry (diameter of 35 mm, gap of 1.0 mm) at a constant temperature of 23 °C. Shear strain rate (usually named “shear rate” at rotational tests) was twice increased (acceleration) from 0 to 50 s
−1 (3000 rpm) and subsequently decreased (deceleration)—i.e., two cycles of shear rate acceleration–deceleration were performed, totalizing 400 s of test (
Figure 2).
2.7. Particular Aspects of WTS Characterization
Characterization of WTS is challenging because quantities and characteristics vary not only among different WTPs but also within the same WTP along any given year. Great variations in WTS composition (organic matter, clay, and sand particles) due to seasonality of raw water quality have been reported [
6]. The sampling procedure of both sludges was based on the Theory of Sampling to warrant a homogeneous sample representative of one month of WTS generation [
42].
WTS characterization has been discussed in a recent technical event in Brazil, LETA 2021 (First Meeting on Water Treatment Sludge: Connections for Technology Innovation), which brought together professionals and researchers dealing with WTS to disclose the state-of-the-art in this subject and to propose new lines of action. Our position, which was in accordance with that of many colleagues who deal with WTS, is that WTS should be characterized according to the desired application. For instance, grain size distribution is fundamental for use in the ceramics industry since different ceramic elements demand suitable ranges of clay and sand fractions. On the other hand, mineralogical characterization is necessary for the cement industry since predominance of amorphous material disqualifies WTS for this application. Mineralogical classification is also important to identify active clay minerals for coagulant, phosphorous, or heavy metals recuperation. Micro and macro properties of WTS are intrinsically related [
43] and should be selected for characterization according to each potential use.
Environmental characterization, on the other hand, should be related to WTS conditioning when reused. A WTS that presents heavy metals might release excessive concentrations if used in a compacted soil layer exposed to weather; however, leaching of these metals might not occur if the WTS is encapsulated in a concrete–bitumen matrix.