Jiakuan Yang*ab,
Shinan Zhanga,
Yafei Shi*ac,
Chao Lia,
Wenbo Yua,
Ruonan Guana,
Jun Xiaoa,
Sha Lianga,
Jingping Hua,
Huijie Houa and
Jiukun Hud
aSchool of Environmental Science and Engineering, Huazhong University of Science and Technology, Wuhan, Hubei 430074, P. R. China. E-mail: jkyang@hust.edu.cn; yfshi@hust.edu.cn; Fax: +86 27 87792101; Tel: +86 27 87792102
bState Key Laboratory of Coal Combustion, Huazhong University of Science and Technology, Wuhan, Hubei 430074, P. R. China
cSchool of Civil Engineering, Architecture and Environment, Hubei University of Technology, Wuhan 430068, Hubei, P. R. China
dDongjiang Environmental Co., Ltd., Shenzhen, Guangdong 518057, P. R. China
First published on 13th January 2017
Two types of deep-dewatered sewage sludge cakes were produced from pilot-scale experiments by using two composite conditioners: FeCl3 + quick lime (Fe–Lime) and Fenton's reagent + red mud (Fenton–RM). The feasibility of direct reuse without any solidifying agents of these two deep-dewatered cakes, with water content of about 60 wt%, as landfill cover materials was investigated. Geotechnical properties of these two sludge cakes were found appropriate for reuse as landfill covers. Their plasticity index values increased significantly from 11.6 (raw sludge) to 23.8 (Fe–Lime) and 35.4 (Fenton–RM). The unconfined compressive strength and direct shear strength of the two deep-dewatered sludge cakes could meet or exceed the requirement of landfill cover materials after a certain curing time. Microstructural analyses of scanning electron microscopy (SEM) and X-ray diffraction (XRD) showed that their microstructures were more porous than that of raw sludge since the skeleton builders played a role in building the rigorous framework. There was negligible leaching of Cu, Zn, Pb, Cd and Cr from the deep-dewatered sludge cake from the toxicity characteristic leaching procedure and column leaching test. Both deep-dewatered sludge cakes could be reused as effective landfill cover materials with a suitable curing time.
Increasing sludge production creates great needs for cost-effective alternatives, in which the most favorable one is beneficial reuse. Reuse of sewage sludge as daily or final cover materials for landfill has attracted substantial attention, and it has been recommended by U.S. EPA.3,4 Commonly, the water content of mechanically dewatered sewage sludge is typically about 75–85 wt% with chemical conditioning with polymers (e.g., polyacrylamide (PAM)). To reduce the high water content of dewatered sludge so that it can be beneficially reused as a landfill cover material, three approaches are often taken. The first approach is sludge drying,5 which is extremely expensive and energy-consuming with a risk of emissions of unpleasant odors. The second approach is blending the dewatered sludge cake with soil. However, the proper type of soil is often not readily available. The third approach is to add solidifying agents into the dewatered sludge cake. With addition of solidifying agents such as Portland cement,6 fluidized bed combustion ash,7 converter slag,8 fly ash and lime,9 calcined aluminum salts,1 or magnesium oxychloride cement,10 the solidified sewage sludge specimens were found effective as landfill cover materials. Unfortunately, the mass ratio of the soil or solidifying agents to the dry solid of the dewatered sludge often needs to be 100–200%. Consequently, the increased volume would take away lots of valuable landfill capacity. Direct reuse of dewatered sewage sludge as landfill cover materials without any soil or solidifying agents is seldom reported in literature.11
For landfill disposal, water content of sludge should be low; and the maximum water content limit is normally 60 wt% in China.12 Many attempts have been made to improve sludge dewatering by employing pretreatment. The pretreatment methods include physical and thermal processes,13,14 chemical processes,15 and biological processes.16 Deep dewatering of sewage sludge using new types of chemical conditioners instead of the traditional polymer conditioners, have been extensively investigated and considered as a cost-effective alternative. In deep dewatering, water content of the dewatered sludge cake could be less than 60 wt%, which makes it more suitable for subsequent reuses or disposal. FeCl3 combined with quick lime (referred as Fe–Lime) is a typical conditioner recommended by U.S. EPA in sewage sludge dewatering.17 In a Fe–Lime system, Fe3+ acts as a coagulant to provide polyvalent cations, and lime plays as a skeleton builder.18–20 Recently, an innovative composite conditioner of combined Fenton's reagent and red mud (referred as Fenton–RM) has been studied by this research group.21 In Fenton–RM system, Fenton reagent acts as an oxidant which destroys the extracellular polymeric substances structure and improves the release of the bond water in sewage sludge; while red mud (RM) plays as a skeleton builder to promote a rigid and permeable structure of dewatered sludge that improves sludge compressibility. In these two conditioning systems, skeleton builders (quick lime and RM) were added during dewatering so that they could be homogeneously dispersed into the dewatered sludge. The skeleton builders also play an important role in the subsequent solidification/stabilization stage for the dewatered sewage sludge. By using either of these two systems, the water content of the treated sludge can be reduced to less than 60 wt%.
In the previous paper,22 pilot-scale sewage sludge dewatering experiments were conducted using both composite conditioners: Fe–Lime and Fenton–RM. Consequently, two types of deep-dewatered sewage sludge cakes were obtained with water content of 52.8 and 47.7 wt%, respectively. It was found that most of the heavy metals in sewage sludge were retained in the dewatered sludge cake.22 However, feasibility of direct reuse of those two deep-dewatered sewage sludge cakes as landfill cover materials has not been fully investigated.
The objective of this study was to evaluate geotechnical properties and heavy metal leaching characteristics of these two deep-dewatered sludge cakes. Two issues would be further investigated in this study: (1) how the skeleton builders would behave to improve the geotechnical properties of sludge cakes; (2) what are the leaching behaviors of heavy metals retained in the sludge cakes. Finally, feasibility of direct reuse of them as landfill cover materials would also be evaluated. The schematic of this study is depicted in Fig. 1.
Batch | pH | Water content (wt%) | VSS/TSS (%) | Cu (mg kg−1)* | Zn (mg kg−1)* | Pb (mg kg−1)* | Cd (mg kg−1)* | Cr (mg kg−1)* |
---|---|---|---|---|---|---|---|---|
a On the dry solid basis. * Milligrams per kilogram of dry solid (mg kg−1). | ||||||||
RS-I | 7.2 | 96.0 ± 0.1 | 41.3 ± 0.3 | 132.1 ± 2.9 | 279.6 ± 12.9 | 39.8 ± 0.5 | 4.5 ± 0.2 | 73.3 ± 0.9 |
RS-II | 6.9 | 96.9 ± 0.1 | 59.6 ± 0.2 | 192.0 ± 2.0 | 1139.3 ± 10.3 | 23.3 ± 0.3 | 2.9 ± 0.1 | 66.7 ± 0.6 |
As presented in Table 1, the volatile suspended solid/total suspended solid (VSS/TSS) of RS-II is higher than that of RS-I since different influent load of sewage mixing with rainwater in various seasons. In the following experiments, RS-I was used in geotechnical tests, and both RS-I and RS-II were used in the leaching properties tests. Both RS samples had a pH close to neutral, and the concentrations of heavy metals (Cu, Zn, Pb, Cd and Cr) are in the order of Zn > Cu > Cr > Pb > Cd.
FeCl3, FeSO4·7H2O and H2O2 (27.5% v/v) of industrial grade were obtained from a commercial company in China. H2SO4 was used to adjust the initial pH of the RS samples to the optimal value of 5.0 before the addition of Fenton's reagent.20 All the acids (including H2SO4, HNO3, HF and HClO4) used for sludge sample digestion were of analytical grade.
Quick lime and RM, which were used as skeleton builders, were dried, milled and sieved to less than 1 mm in particle size before use. The quick lime was obtained from a local factory. The RM was supplied by an alumina plant employing the Bayer process in Zhengzhou, China. Their chemical compositions are presented in Table S1 as ESI.†
Fig. 2 The photo of the pilot-scale facility for sewage sludge conditioning and deep dewatering in the Tangxunhu WWTP. |
Main characteristics of two types of deep-dewatered sludge cakes are presented in Table 2. After the deep-dewatering process, the water contents of the dewatered sludge cakes from both systems were reduced to less than 60 wt%, which is favorable for subsequent disposal, especially for landfilling. VSS/TSS ratios also decreased due to the addition of inorganic skeleton builders. As reported earlier, most of the heavy metals remained in the sludge cake during the dewatering process.22
Conditioning system | Water content (wt%) | VSS/TSS (wt%) | Cu (mg kg−1)* | Zn (mg kg−1)* | Pb (mg kg−1)* | Cd (mg kg−1)* | Cr (mg kg−1)* |
---|---|---|---|---|---|---|---|
a On the dry solid basis. * Milligrams per kilogram of dry solid (mg kg−1). | |||||||
Fe–Lime-I | 52.8 | 35.2 | 91.7 ± 0.9 | 251.3 ± 7.0 | 30.3 ± 1.3 | 2.4 ± 0.4 | 59.9 ± 3.4 |
Fenton–RM-I | 47.7 | 37.8 | 101.6 ± 1.6 | 253.6 ± 5.6 | 36.0 ± 0.0 | 4.8 ± 0.1 | 117.4 ± 0.9 |
Fenton–RM-II | 53.7 | 45.7 | 93.7 ± 0.5 | 797.2 ± 4.3 | 30.5 ± 0.5 | 3.0 ± 0.1 | 77.7 ± 0.3 |
The traditional dewatered sludge after conditioned with PAM (referred to RS-PAM) was comparatively investigated in the geotechnical tests. RS-PAM was produced from a centrifugal dewatering process after conditioning with PAM in the Tangxunhu WWTP. The water content of RS-PAM is 81.7 wt%, and its VSS/TSS is about 41 wt%, which is almost the same as that of the RS-I sample.
The geotechnical tests for the samples were conducted in accordance with the Chinese standards for soil laboratory test methods (GB/T 50123-1999) for water content, liquid limit (LL), plastic limit (PL) and plasticity index (PI).24 The classification of the solidified sludge was determined in accordance with the Unified Soil Classification System.25 The dewatered sludge specimens were molded in a self-made compactor device to determine the optimum moisture content (OMC) and the maximum dry density (MDD). A heavy compaction procedure (5 layers, 27 times compaction for each layer), as specified in Chinese test methods of soils for highway engineering, was used to estimate the characteristics of compaction.26 The permeability of the dewatered sludge specimens under optimum compacted conditions was also measured by a variable-head permeability test following the Chinese standard.24
Mechanical strength properties, i.e., unconfined compressive strength (UCS) and direct shear strength (DSS), were also determined according to the standard.24 The cylinder specimens for the UCS test were 3.91 cm in diameter and 8.0 cm in length, and the ones for the DSS test were 6.18 cm in diameter and 2.0 cm in length with a relative compaction of 90%. The specimens were cured in a standard curing chamber at 20 ± 2 °C with humidity >90 wt%. Triplicate samples were immersed in water for 24 h, and used to evaluate the mechanical strengths of these specimens cured for 0, 3, 7, 14, 21, 28, 60, 90 days.
According to TCLP,27 50 g air-dried sludge specimens (Fe–Lime-I and RS-I) was grinded and sieved to achieve particle sizes smaller than 9.5 mm and then placed in a polyethylene bottle, followed by an addition of one liter acetic acid solution (5.7 mL acetic acid in 1 L of distilled water, pH = 2.88). The bottle was placed in a rotary extractor and rotated for 18 h at 30 ± 2 rpm. After rotation, the sample was filtered through a 0.45 μm membrane filter, and then the filtrate was collected and analyzed for metal concentrations by using an atomic absorption spectrometer (Analytik Jena AG NovAA 400, Germany).
The schematic of the CLT is presented in Fig. S2.† As a dynamic test, CLT reportedly has a better leaching effect.28 Eighty grams of air-dried sludge specimens (Fenton–RM-II and RS-II) were grinded and sieved to achieve particle sizes smaller than 4 mm, and placed in a glass column (5 cm inside diameter and 35 cm height) and a perforated plate on both ends. The dewatered sludge was leached from the bottom up by a continuous flow of the acetic acid solution (pH = 2.88) using a peristaltic pump. A flowing rate of 5 mL h−1, commonly used in literature, was adopted here; and a rate of 10 mL h−1 was also applied for a comparison.
The leachate was sampled at different liquid-to-solid ratios (L/S, mL g−1). L represents the volume of the acetic acid solution passed through the column, in mL; and S represents the mass of the sludge sample in the column, in g. Heavy metals in the leachate were analyzed. The extraction percentage of each heavy metal is the mass ratio of heavy metal leached out to the total mass of heavy metal in the original sludge sample.
Specimens | LL (wt%) | PL (wt%) | PI (wt%) | OMC (wt%) | MDD (g cm−3) | Coefficient of permeability (cm s−1) |
---|---|---|---|---|---|---|
Clay | 40.6 | 20.0 | 20.6 | 12.4 | 1.890 | 3.31 × 10−8 |
RS-I | 69.7 | 58.1 | 11.6 | 37.5 | 1.581 | 6.45 × 10−8 |
RS-PAM | 69.3 | 59.8 | 9.5 | 36.9 | 1.561 | 6.71 × 10−8 |
Fe–Lime-I | 64.7 | 40.9 | 23.8 | 25.5 | 1.421 | 5.90 × 10−7 |
Fenton–RM-I | 68.5 | 33.1 | 35.4 | 23.0 | 1.435 | 7.20 × 10−6 |
In addition, RS-I showed a high OMC of 37.5 wt% and an MDD of 1.581 g cm−3. While for both deep-dewatered sludge cakes, the values of OMC and MDD decreased considerably. It implied that deep-dewatered sludge cakes have lower water-absorption capacity, when compared with RS and RS-PAM.
It can also be seen from Table 3 that the deep-dewatered sludge cakes had higher permeability coefficient values (>10−7 cm s−1) than that of RS (6.45 × 10−8 cm s−1). These results validate the roles of skeleton builders in the conditioning stage that increased the porosity of dewatered sludge. No existing Chinese standards define acceptable parameters with regards to the permeability coefficient of landfill cover. In USA, the permeability coefficients of lime-stabilized sludge as landfill cover range from 1 × 10−3 to 10−6 cm s−1.29 In general, the permeability coefficient values of the deep-dewatered sludge and the RS are less than the reported permeability coefficient values of lime-stabilized sludge. Both deep-dewatered sludge cakes had a permeability coefficient value (between 10−6 and 10−8 cm s−1), which is smaller to the reported permeability coefficient of the lime-stabilized sludge.
Fig. 5 SEM images of (a) RS-I, and the (b) dewatered sludge cakes of Fe–Lime-I, (c) Fenton–RM-I; and (d) the XRD patterns of these samples. |
The dewatered sludge cake of Fe–Lime-I consists of smaller particulates and it is more porous with an irregular shape (Fig. 5(b)). It indicates that the raw sludge with a high organic content and poor dewaterability can be improved with skeleton builders to generate a porous, but relatively incompressible structure. The XRD pattern indicates the Fe–Lime-I consists mainly of quartz, calcium hydroxide and calcite.
Some irregularly shaped crystals embedded among the sludge particles were found in Fenton–RM-I (Fig. 5(c)). This dewatered sludge cake appears to be more porous. The XRD patterns indicate that it consists mainly of quartz, mica, gypsum, cancrinite, and gibbsite.
Fig. 6 Concentrations of heavy metal in the leachates from the TCLP tests: (a) RS-I, and Fe–Lime-I; (b) RS-II, and Fenton–RM-II. |
As shown in Fig. 6(a) and (b), leached concentrations of Cu, Zn and Pb from the two dewatered sludge cakes of Fe–Lime-I are significantly lower than those of the RS-I; while Cr concentration in the dewatered sludge of Fenton–RM-II are the highest among all of RS and dewatered sludge specimens (Fig. 6(b)). The higher concentrations of Cr might come from the red mud which was added as the conditioner. In general, the sludge cake from the Fe–Lime system has a good retention for heavy metals.
Typical acceptable TCLP concentrations of heavy metals effluent discharge standards of municipal solid waste landfills are 40, 100, 0.25, 0.15 and 4.5 mg L−1 of Cu, Zn, Pb, Cd, and Cr (GB16889-2008), respectively.30 The results show that Pb in Fe–Lime-I exceeded the acceptable limit, while the retention capability of Fenton–RM-II on Pb and Cd needs to be improved. In order to facilitate technology adaptability, two improvements could be used to promote the solidification effects of the dewatered sludge cakes. Firstly, during the conditioning and dewatering process, a little more dosage of conditioner (lime or cement) could be added to further improve the dewatering effects and the heavy metal solidification behavior. Besides, to avoid the risk of heavy metal release in the landfill process, small amount of cement could be mixed with the dewatered sludge cakes to strengthen the heavy metal solidification effects, given the good cooperation of alkali cement and red mud.
The results of this CLT study indicate that the deep-dewatered sludge cakes conditioned with skeleton builders are relative stable for a long period of time, with regards to heavy metal leaching, when they are used as daily or final landfill cover.
In summary, the skeleton builders introduced in the conditioning stage during deep-dewatering process improve the geotechnical properties and heavy metal leaching characteristics of the dewatered sludge cakes which make them appropriate for re-use as landfill cover materials.
CLT | Column leaching test |
DS | Dry solid |
DSS | Direct shear strength |
LL | Liquid limit |
L/S | Liquid-to-solid ratio |
MDD | Maximum dry density |
OMC | Optimum moisture content |
PAM | Polyacrylamide |
PI | Plasticity index |
PL | Plastic limit |
RM | Red mud |
RS | Raw sludge |
SEM | Scanning electron microscopy |
TCLP | Toxicity characteristic leaching procedure |
TSS | Total suspended solids |
UCS | Unconfined compressive strength |
VSS | Volatile suspended solids |
WWTP | Wastewater treatment plant |
XRD | X-ray diffraction |
Footnote |
† Electronic supplementary information (ESI) available. See DOI: 10.1039/c6ra26480h |
This journal is © The Royal Society of Chemistry 2017 |