Ameliorating some quality properties of an erosion-prone soil using biochar produced from dairy wastewater sludge

Catena 171 (2018) 193–198

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Ameliorating some quality properties of an erosion-prone soil using biochar produced from dairy wastewater sludge

T

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Seyed Hamidreza Sadeghia, , Mohammad Hossein Ghavimi Panaha, Habibollah Younesib, Hossein Kheirfamc a

Department of Watershed Management Engineering, Faculty of Natural Resources, Tarbiat Modares University, Iran Department of Environment Science, Faculty of Natural Resources, Tarbiat Modares University, Iran c Department of Environmental Science, Urmia Lake Research Institute, Urmia University, Urmia, Iran b

A R T I C LE I N FO

A B S T R A C T

Keywords: Environmental pollutions Land degradation Soil improvement Soil quality Waste management

Land degradation due to decline in soil quality and wastewater pollution is a major challenge for ecosystems sustainability, worldwide. Hence, utilizing adaptable and multi-objective strategies is essential to address environmental challenges. To this end, we produced a biochar from air-dried dairy wastewater sludge (i.e., Kalleh Dairy Company, Iran) through pyrolysis process at 300–350 °C which led to reduction in initial heavy metals contents. The produced biochar was then used to improve the soil quality of a highly degradable soil. Some important nutrients and heavy metals of dairy wastewater and produced biochar were measured by acid digestion/ICP-MS. We then spread two rates of the biochar (400 and 800 g m−2) over the surface of the small-scale boxes (0.5 × 0.5 × 0.5-m) filled by an erosion-prone soil collected from the Chalus Watershed, Northern Iran, and left for 30 days. The carbon (C), nitrogen (N) and organic matter (OM) content, and also carbon/nitrogen (C/N) ratio of treated soil were measured to assess effect of the produced biochar on soil quality improvement. The results showed that some contents of the measured heavy metals (i.e., Pb, Ni, Al, Cr, Mn, Fe and Zn) in the produced biochar significantly (p < 0.01) reduced compared to those of the raw dairy wastewater. Additionally, application of two dosages of 400 and 800 g m−2 of biochar to the study soil increased C, N, OM and C/N of the soil at tunes of 2.67–5.5; 2–3 and 2.67–5.5 times, and 22–61%, respectively, in comparison with untreated soils (control). By and large, converting the wastewater as an environmental pollution source to biochar and using it as an eco-friendly soil amendment is a multi-objective and adaptive approach for the ecosystem management.

1. Introduction Land degradation and soil and environmental pollutions are one of the most serious ecological and economic problems in the world (Rasul, 2014). Soil quality decline particularly from hill-slopes is known as a type of land degradation, which threatens human health and wellbeing (Kheirfam et al., 2017a). Therefore, various techniques have been used to reduce land and soil quality degradation from hill-slopes (e.g., Sadeghi et al., 2015, 2016a; Mamedov et al., 2016; Kheirfam et al., 2017a) striving for environmentally friendly, economically efficient, and practically doable measures. In this regard, many amendments like sawdust and wood ash, municipal wastes, gypsum, lime (Khan and Khan, 2016; Sadeghi et al., 2016a); animal and crop manures, organic composts, crop and food industry remnants (Sadeghi et al., 2015; Gholami et al., 2016; Mamedov et al., 2016) have been applied to

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conserve and improve soil quality. Improvement of soil properties using native environmentally based amendments has long been a desired way to improve soil quality. In recent years, biochar has been used for various purposes viz. carbon sequestration with the aim of soil fertility improvement (Glaser et al., 2002; Lehmann and Rondon, 2006; Haider et al., 2017), reduction in greenhouse gas emissions and climate change mitigation (Lehmann and Rondon, 2006; Woolf et al., 2010; Rasul et al., 2016), recapturing excess nutrients from wastewaters (Ghezzehei et al., 2014), controlling runoff and soil loss (Jien and Wang, 2013; Hseu et al., 2014; Hazbavi and Sadeghi, 2016; Sadeghi et al., 2016a), increasing plant growth and yield (Rasul et al., 2017), sorption of heavy metals (Xu et al., 2013; Ghezzehei et al., 2014; Inyang et al., 2015) and even improving soil aggregate characteristics (Li et al., 2017). Although, temperature, residence time, heating rate, and feedstock particle size in pyrolysis

Corresponding author. E-mail addresses: [email protected] (S.H. Sadeghi), [email protected] (H. Younesi), [email protected] (H. Kheirfam).

https://doi.org/10.1016/j.catena.2018.07.018 Received 24 January 2018; Received in revised form 15 June 2018; Accepted 16 July 2018 0341-8162/ © 2018 Elsevier B.V. All rights reserved.

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2.2. Heavy metals and nutrient analyses

process potentially affect the quality and quantity characteristics of the produced biochar and thus its interactions with the environment of its application (Yuan et al., 2015). According to the literature, biochar has been produced from different materials including woodchip (Lai et al., 2013), oak wood (Mukherjee et al., 2014), poultry litter (Brantley et al., 2016), bamboo and rice straw (Liu et al., 2016); vinasse (Sadeghi et al., 2016a), sewage sludge (Yuan et al., 2016), wastewater sludge (Yue et al., 2017a) and cow manure (Yue et al., 2017b) at different conditions. The results showed that biochar application improved soil physical and chemical (Hass et al., 2012; Nelissen et al., 2015) and biological (Mitchell et al., 2015) properties, water holding capacity (Cao et al., 2014), as well as soil fertility, nutrient and plant productivity (Major et al., 2010; Vaughn et al., 2013). Nonetheless, the studies focused on impacts of biochar produced from industry sludge on soil characteristics and particularly pollutants and insanitary absorption are still lacked. Since dairy industries sludge hugely produced, characterized by high concentrations of heavy metals, nitrogen (N), phosphorous (P), and other elements (Ghezzehei et al., 2014) and resulted in environment pollution (Arvanitoyannis and Giakoundis, 2006; Massah and Mirbagheri, 2012; Mohebi-Fard, 2015), it is fair to apply it in original or modified type for useful goals. Towards the increasing amount of urban wastes, application of different wastes as soil amendments therefore was considered as one of the effective methods in order to manage large amounts of wastes potentially produced worldwide to fulfill human needs (e.g. Hazbavi and Sadeghi, 2016; Sadeghi et al., 2016a). Finding sustainable and economic methods for disposing different wastes and by-products is increasingly becoming a major environmental challenge throughout the globe. Biochar technical intervention has increased potential for adaptation in areas where large agricultural and urban wastes are available (Sadeghi et al., 2016a; Haider et al., 2017). But, the possibility of biochar production from dairy wastewaters as a major source of environmental pollution threatening the water and soil resources has not been considered or documented yet. The present study was therefore planned to (1) produce biochar from air-dried dairy wastewaters of the Kalleh Company, Amol City, Mazandaran Province, Iran, (2) measure and assess the content of heavy metals in raw material and produced biochar in comparison with the standards given by the United States Environmental Protection Agency (U.S. EPA), and (3) appraise the effect of produced biochar on improving the nutrient contents of a highly degradable soil under laboratorial circumstances.

In order to assess the potential of pyrolysis process in changeability of heavy metals and nutrient contents compared to dairy wastewaters, 11 heavy metals viz. lead (Pb), nickel (Ni), aluminum (Al), cobalt (Co), cadmium (Cd), arsenic (As), chromium (Cr), copper (Cu), manganese (Mn), iron (Fe) and zinc (Zn) with higher concentrations than other metals, as well as content of carbon (C), nitrogen (N), phosphorus (P), potassium (K) and C/N ratio were measured in both raw dairy wastewater and produced biochar samples. To this end, we used the acid digestion method (Uras et al., 2012). Afterwards, the Whatman No. 2 paper was used to filter solutions. Finally, the inductively coupled plasma optical emission spectrophotometry (ICP/OES) was used to detect element concentrations. Summary of the backgrounds and standards for determining the measured heavy metals and other elements have been given in Table 1. The international standards given in “Code of Federal 40CFR Regulations” protocols (U.S. EPA, 1977, 1979, 1992) were used as basis for the comparative analyses. 2.3. Experimental setup A Silty-Loam-Clay (40% clay, 44% silt and 16% of sand) soil from the Chalus Watershed, Mazandaran Province, Northern Iran was used for the study. Soil bulk density, pH, electrical conductivity (EC), organic matter and total nitrogen were 1.16 g cm−3, 7.55, 0.21 dS m−1, 0.57% and 0.09%, respectively. The study soil was air-dried and sized using a 4-mm sieve (Sadeghi et al., 2014, 2016a, 2016b, 2017; Kheirfam et al., 2017a, 2017b). Three layers of mineral pumice grains with different sizes and a total thickness of 28 cm were used as a filter layer and placed at the bottom of the boxes to simulate natural conditions and decreasing boxes weights (Sadeghi et al., 2014, 2016a and b; Kheirfam et al., 2017a). An approximately 0.075 m3 of soil was packed in the 0.5 × 0.5 × 0.5-m boxes for each experiment. Unlike conditions governing agricultural lands, no tillage was applied to the experimental plots because of necessity of imitating governing conditions on soil origin. To overcome the disturbance made in soil conditions through collecting and transferring process from study area into the experiment boxes, the soil surface was levelled and compacted manually by a hand roller until natural conditions of hill-slopes of the soil origin was achieved in viewpoint of bulk density. The experimental boxes consisted of control and treated with 400 and 800 g m−2 of biochar were set in three replications (Fig. 2). The produced biochar with the help of a small sieve was evenly spread over the surface of the study boxes (Hazbavi and Sadeghi, 2016; Sadeghi et al., 2016a, 2016b). However, in sloping soils, biochar may be lost through wind (Peng et al., 2016). To resolve this, before treating, we moisten the soil surface to increase the adhesion of biochar and soil particles together. To simulate natural condition, the boxes were placed at the outside of the lab on 25% slope (according to the study area slope) for a 30-days period for complete settlement of the soil. The period was arbitrarily selected based on apparent features of the soil conditions which it was supposed to be similar to real conditions and pointed by Galvez et al. (2012), Chintala et al. (2014) and Berihun et al. (2017) as a suitable period for effective influence of biochar on soil properties.

2. Materials and method 2.1. Biochar production To produce biochar, 20 kg of fresh dairy wastewater was provided through sampling from 50 points of the waste tanks of the Kalleh Dairy Company, Amol City, Mazandaran Province, Iran. The wastewater samples were air-dried for three days under natural condition at the Rainfall and Soil Erosion Simulation Laboratory, International Campus of Tarbiat Modares University, Noor, Iran. The air-dried samples were thoroughly mixed together and then pyrolyzed in a vertical kiln (Sadeghi et al., 2016a) at 300–350 °C for 3 h residence time. The produced biochar samples were allowed to cool down up to the laboratory temperature (Sadeghi et al., 2016a; Zornoza et al., 2016). The produced biochar was ultimately crushed and subsequently passed through a 2mm sieve (Butnan et al., 2015), and hence, it was thoroughly mixed to obtain a fine granular product allowing better uniform mixing (Butnan et al., 2015). The obtained biochar was directly used in subsequent experiments. All different steps of biochar production have been depicted in Fig. 1.

2.4. Some soil quality properties analyses The soil carbon (C), nitrogen (N), organic matter (OM), and C/N ratio were also considered as accessible soil quality indicators (Kheirfam et al., 2017a; Valle and Carrasco, 2018). 2.5. Statistical analyses The Shapiroe-Wilk and the Levine's tests were used to test normality 194

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Fig. 1. General view of (a) air-dried dairy wastewaters, (b) produced and sieved biochar and (c) used kiln (Sadeghi et al., 2016a).

3. Results and discussion

Table 1 Background of used measurement methods for determination of heavy metals, carbon (C), phosphorus (P), nitrogen (N), and potassium (K) in dairy wastewaters and produced biochar samples. No.

Element

Determination method

Reference

1

Heavy metals

2

Carbon

Extraction with a solution of DTPA Walkley-Black

3 4 5

Phosphorus Nitrogen Potassium

Olsen method Kjeldahl method Flame photometer method

(Lindsay and Norvell, 1978) (Nelson and Sommers, 1996) (Olsen et al., 1954) (Bremner, 1996) (Varley, 1966)

3.1. Heavy metals contents in wastewater and biochar As per procedures explained before, all heavy metals were measured in raw wastewater and produced biochar. The results have been summarized in Fig. 3. According to Fig. 3, heavy metals of Pb, Ni, Al, Cr, Mn, Fe and Zn in dairy wastewater were observed in very high levels indicating a possible contamination of surface and ground waters as a result of leaching. Concentrations of Pb, Ni, Al, Cr, Mn, Fe and Zn in the raw dairy wastewater were respectively found to be 106, 12, 153, 23, 18.83, 608 and 40.25% more than standard levels proposed by the U.S. EPA. Therefore, it is necessary to protect ecosystems from absorbing harmful and dangerous dairy wastewater, especially those intended for direct food production. Literature showed that the long-term wastewater irrigation or solid waste disposal has resulted in the heavy metal contamination in both soil and groundwater (Liang et al., 2014). Removal of heavy metal ions from wastewaters is therefore essential before they reach the

and homogeneity of variances of the data, respectively. Significant differences in data among treatments analyzed using a one-way analysis of variance (ANOVA), followed by the Turkey's Honestly Significant Difference (HSD) test at the 95% confidence level. The IBM SPSS 19 software package was used for the analyses.

Fig. 2. General view of (a) control box (without biochar), (b) 400 g m−2 of biochar, and (c) 800 g m−2 of biochar on soil box. 195

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a

a

Dairy Wastewater

140

Biochar

U.S. EPA

b Concentration (mg kg -1)

120 100 a

80

a 60

a

a

a

b

a

40 20

b

c

b b

b

b b b

b b

a

a

b

b c

a b

c

c

b

c

c

c

Cd

Ar

0 *Cr

*Co

**Mn

***Fe

**Zn

*Pb *Ni Heavy Metal

**Al

**Cu

Fig. 3. Comparison of measured heavy metals in the air-dried dairy wastewater and biochar based on U.S. EPA standards. (*, ** and ***, indicated that the values divided by 10, 100 and 1000, respectively).

450

a a

Dairy wastewater

400

Biochar

Table 3 Results of ANOVA on effect of biochar application on the soil carbon (C) and nitrogen (N) in the study treatments.

U.S. EPA

350

Value

300

a

b

Property

Variation sources

df

Mean square

F-value

p-Value

C

Between groups Within groups Total Between groups Within groups Total

2 6 8 2 6 8

7.63 0.11

68.75

0.00

0.055 0.001

47.77

0.00

250

200

N

150 100 a

50

b

b a

c

a

a b

b c a

12

C/N (ratio)

10

0 C (g/kg)

N (g/kg)

P (g/kg) K (g/kg) Nutrient / Variable

8

Fig. 4. Comparison of the fertilizers elements in air-dried dairy wastewater and biochar based on U.S. EPA standards.

a Control

400 g of biochar on 1 square meter of soil

a

0 (control)

400

800

1 2 3 Average Standard deviation Coefficient of variation (%) 1 2 3 Average Standard deviation Coefficient of variation (%) 1 2 3 Average Standard deviation Coefficient of variation (%)

2

c

c C (%)

N (%)

OM (%)

C/N

0.50 0.66 0.57 0.58 0.08 13.79 1.9 2.1 2.4 2.13 0.25 11.74 3.2 3.9 4.2 3.77 0.15 13.53

0.07 0.09 0.11 0.09 0.02 22.00 0.23 0.29 0.28 0.27 0.03 11.79 0.31 0.36 0.40 0.36 0.05 13.89

0.86 1.1352 0.9804 0.99 0.13 13.9 3.268 3.612 4.128 3.67 0.43 11.79 5.57 6.79 7.32 6.47 0.88 13.62

7.14 7.33 5.18 6.55 1.19 18.17 8.26 7.24 8.57 8.02 0.70 8.73 10.32 10.83 10.50 10.55 0.26 2.41

b

b

0

Soil quality indicators C (%)

b

800 g of biochar on 1 square meter of soil

Table 2 Measured soil quality indicators (carbon, C; nitrogen, N; organic matter, OM; carbon-nitrogen, C/N) under different treatments. Plot no. and statistical criteria

c

6 4

Biochar (g m−2)

a

b

a

c

N (%) OM (%) Soil quality indicators

C/N ratio

Fig. 5. Comparison of carbon (C), nitrogen (N), organic matter (OM), carbonnitrogen ratio (C/N) in the study treatments.

that these heavy metals enter the human food chain through soil or water (Friesl et al., 2006) and lead to irreparable consequences (Liu et al., 2013). The results are in line with Zhang et al. (2010), Agrafioti et al. (2013) and Kim et al. (2015) who noted that the biochar created organic ligands complexes with heavy metals due to its physical structure and reduced the mobility of the metals in the soil. Additionally, in consistent with the results of the present research, Shinogi et al. (2003) reported that biochar produced from sewage sludge in Japan did not show harmful levels of heavy metals. For the same reasons, the direct application of dairy wastewaters is not recommended as soil amendment for soil and water conservation. The ANOVA results showed that the effect of pyrolysis and biochar production on reducing heavy metals was significant (p < 0.01). Our results further showed that the concentration of all the study heavy metals from biochar were 1.34 to 30.24 and 0.04 to 161.5 times lower than those from raw dairy wastewater and the U.S. EPA standards, respectively (Fig. 3). In confirmation, Kumar et al. (2011), Komkiene

environment as recently notified by Patra et al. (2016). Although, concentrations of Co, Cd, Ar and Cu were found less than those reported by the U.S. EPA. Though these may even cause toxic contamination due to high emission of the dairy wastewater from industries. It is verified 196

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quality properties of C, N, OM, and C/N ratio were significantly improved in the study poor soil. By and large, we found that converting eco-destructive industrial based wastewater to eco-friendly and costeffective by-products like bio-fertilizers could be drawn a perspective of multi-objectives bio-techniques for ecosystem clean up and restoration. However, extending similar studies with different temporal and spatial scales and under various circumstances of rainfall intensities, slope steepnesses, elapse times between biochar application and rainfall occurrence, more dosages of application and other soil types are needed to gain comprehensive information. Further studies also are required to investigate the possibility of using sewage sludge in different locations as its level of contamination may be quite variable at different locations and times. Over the course of time, it may be then possible to develop the necessary prerequisite to get access to hygiene sewage for biochar production. Further studies are required on application, quantification of impact, environmental perspective, feasibility of production and economics of producing biochar from different raw materials to allow drawing proper conclusion.

and Baltrenaite (2016) and, Patra et al. (2016) demonstrated high surface area and pore volume of biochar had a greater affinity for heavy metals because metallic ions could be physically absorbed onto the char surface and retained within the pores. In addition, Nartey and Zhao (2014) noted that biochar is a promising alternative to remedy the soils contaminated with heavy metals and organic compounds through adsorption and immobilization due to its large surface area, charged surface, and functional groups. Overall, the bioavailability of heavy metals and organic compounds decreased when biochar was amended into soils. The adsorptions of Cu, Cd, Pb, and Ni onto biochar prepared from anaerobically digested biomass were also investigated by Inyang et al. (2012). It was found that the biochar demonstrated a better ability to remove Ni and Cd. 3.2. Nutrients elements Besides heavy metal contents, important nutrient elements viz. C, N, P, K and C/N were measured whose results have been carted in Fig. 4. As seen in Fig. 4, contents of C, N, P and K, and also C/N ratio in dairy wastewater were 28.5, 3.89, 29.33 and 2.7%, and 7.33, respectively. According to the U.S. EPA standards, the higher amounts of P and N could disrupt plant growth (Chen et al., 2013). Whereas, the biochar production significantly decreased the N, P and K (p < 0.01) and increased the C and C/N (p < 0.05). In this regards, Ghezzehei et al. (2014) suggested a potential of biochar for recovering essential nutrients from dairy wastewater and improving soil fertility if the enriched biochar is returned to the soil.

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3.3. Soil quality indicators In this section, effects of biochar application with rates of 400 and 800 g m−2 successfully applied by Sadeghi et al. (2016a) for biochar produced from vinasse were investigated in triplicate on soil quality indicators at box scale. The rates were considered below levels of 12 to 32 ha−1 proposed for agricultural lands (Laghari et al., 2015) subjected to tillage operation and mixed with an upper soil layer. The results of statistical analyses have been shown in Tables 2 and 3, and Fig. 5. The results showed that application of 400 and 800 g m−2 of biochar significantly improved (p < 0.01) the C (and/or OM) and N content of the treated soils by 2.67 and 5.5; and 2 and 3 times respectively in compared than control (Table 3 and Fig. 5). Additionally, C/N ratio were respectively improved at tune of 22 and 61%, due to 400 and 800 g m−2 of biochar application compared to those of untreated soils (Table 3 and Fig. 5). The similar results were reported by Laird et al. (2010) showed that the biochar addition to a typical Midwestern agricultural soil was an effective management option for reducing nutrient leaching in agricultural production. In addition, Foereid (2015) noted that application of biochar to extract and concentrate the nutrients could eliminate current difficulties associated with the storage of high volume of the waste liquids, and also eliminate environmental concerns related to spreading the high volume of liquid fertilizers on soil. It has been well documented in the previous researches (e.g., Glaser et al., 2002; Major et al., 2010; Yao et al., 2012) that the biochar produced from different wastes increased soil fertility and crop productivity by reducing the leaching of nutrients or even supplying nutrients to the plants. 4. Conclusion In this study, we assessed the reducibility of heavy metals of airdried dairy wastewaters through producing biochar as well as improvability of some quality properties of an erosion-prone soil due to application of produced biochar as a nutrient source amendment. Our measurements showed that the heavy metals contents in the dairy wastewaters significantly decreased resulted from pyrolysis (biochar) led to produce a safe and nutrient-rich soil amendment. So that the 197

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