9
Research Article Vertical Phosphorus Migration in a Biosolids-Amended Sandy Loam Soil in Laboratory Settings: Concentrations in Soils and Leachates Yulia Markunas, 1 Vadim Bostan, 1 Andrew Laursen, 1 Michael Payne, 2 and Lynda McCarthy 1 1 Department of Chemistry and Biology, Ryerson University, 350 Victoria Street, Toronto, ON, Canada M5B 2K3 2 Black Lake Environmental, 246 Black Lake Route, Perth, ON, Canada K7H 3C5 Correspondence should be addressed to Vadim Bostan; [email protected] Received 24 May 2016; Revised 5 October 2016; Accepted 16 October 2016 Academic Editor: Rafael Clemente Copyright © 2016 Yulia Markunas et al. is is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited. e impacts of biosolids land application on soil phosphorus and subsequent vertical migration to tile drainage were assessed in a laboratory setup. Soil, representing typical “nonresponse” Ontario soil as specified by Ontario Ministry of Agriculture, Food, and Rural Affairs (OMAFRA), was amended with anaerobically digested biosolids at a rate of 8 Mg ha −1 (dry weight). Over five months, these amended soil samples from two different depths were sequentially fractionated to determine various inorganic and organic phosphorus pools in order to evaluate phosphorus vertical migration within a soil profile. Soil leachate was analyzed for soluble reactive phosphorus. e results indicated that biosolids application did not significantly affect phosphorus concentrations in soil and did not cause phosphorus vertical migration. e concentrations of soluble reactive phosphorus also were not significantly affected by biosolids. 1. Introduction Even though the term biosolids, as it is understood now, only appeared at the end of 20th century, the concept of human waste application to agricultural lands has been known for thousands of years [1]. Agricultural land application is considered a viable way to recycle municipal biosolids. Biosolids are valued as a soil conditioner [1] and as a source of macro- and micronutrients and organic matter necessary for healthy crops [2, 3]. Even though municipalities, farmers, and the general public may benefit from the use of biosolids on agricultural lands, there are some environmental concerns related to this practice. One of these concerns is the relatively high level of total phosphorus in biosolids and its potential migration to surface- and groundwater from biosolids-amended lands [4] as its overabundance in surface water can lead to eutrophi- cation [5]. Many wastewater treatment plants (WWTPs) use alum or FeCl 3 in tertiary treatment to precipitate phosphorus, which becomes part of the biosolids material. Further, stabi- lization of raw sewage or biosolids by alkaline stabilization may result in some phosphorus precipitation as Ca 3 (PO 4 ) 2 . As a result the phosphorus may be in forms that are not biologically available, or in forms that retard migration from point of application [6]. erefore, total phosphorus in biosolids may not be relevant in considering the risk posed by phosphorus loss from fields to aquatic systems. Rather, to properly assess potential risk of biosolids-derived phosphorus to receiving waters, it may be more important to consider the various fractions of phosphorus in biosolids and their behaviour in soil (e.g., migration and transformation). Generally, phosphorus has the potential of being trans- ported to aquatic systems through three major pathways: surface runoff and erosion, subsurface flow, and tile drainage [4, 7]. To a smaller extent, it can also be transported by wind erosion and deposition [8]. Runoff and erosion are important pathways of soil phosphorus loss [9, 10], and the majority of studies on phosphorus loss from agricultural land Hindawi Publishing Corporation Applied and Environmental Soil Science Volume 2016, Article ID 3460939, 8 pages http://dx.doi.org/10.1155/2016/3460939

Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

  • Upload
    others

  • View
    0

  • Download
    0

Embed Size (px)

Citation preview

Page 1: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

Research ArticleVertical Phosphorus Migration in a Biosolids-AmendedSandy Loam Soil in Laboratory Settings: Concentrations inSoils and Leachates

Yulia Markunas,1 Vadim Bostan,1 Andrew Laursen,1 Michael Payne,2 and Lynda McCarthy1

1Department of Chemistry and Biology, Ryerson University, 350 Victoria Street, Toronto, ON, Canada M5B 2K32Black Lake Environmental, 246 Black Lake Route, Perth, ON, Canada K7H 3C5

Correspondence should be addressed to Vadim Bostan; [email protected]

Received 24 May 2016; Revised 5 October 2016; Accepted 16 October 2016

Academic Editor: Rafael Clemente

Copyright © 2016 Yulia Markunas et al.This is an open access article distributed under the Creative CommonsAttribution License,which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.

The impacts of biosolids land application on soil phosphorus and subsequent vertical migration to tile drainage were assessed in alaboratory setup. Soil, representing typical “nonresponse” Ontario soil as specified by Ontario Ministry of Agriculture, Food, andRural Affairs (OMAFRA), was amended with anaerobically digested biosolids at a rate of 8Mg ha−1 (dry weight). Over fivemonths,these amended soil samples from two different depths were sequentially fractionated to determine various inorganic and organicphosphorus pools in order to evaluate phosphorus vertical migration within a soil profile. Soil leachate was analyzed for solublereactive phosphorus. The results indicated that biosolids application did not significantly affect phosphorus concentrations in soiland did not cause phosphorus vertical migration. The concentrations of soluble reactive phosphorus also were not significantlyaffected by biosolids.

1. Introduction

Even though the term biosolids, as it is understood now, onlyappeared at the end of 20th century, the concept of humanwaste application to agricultural lands has been knownfor thousands of years [1]. Agricultural land applicationis considered a viable way to recycle municipal biosolids.Biosolids are valued as a soil conditioner [1] and as a sourceof macro- and micronutrients and organic matter necessaryfor healthy crops [2, 3].

Even though municipalities, farmers, and the generalpublic may benefit from the use of biosolids on agriculturallands, there are some environmental concerns related to thispractice. One of these concerns is the relatively high level oftotal phosphorus in biosolids and its potential migration tosurface- and groundwater from biosolids-amended lands [4]as its overabundance in surface water can lead to eutrophi-cation [5]. Many wastewater treatment plants (WWTPs) usealumor FeCl3 in tertiary treatment to precipitate phosphorus,

which becomes part of the biosolids material. Further, stabi-lization of raw sewage or biosolids by alkaline stabilizationmay result in some phosphorus precipitation as Ca3(PO4)2.As a result the phosphorus may be in forms that are notbiologically available, or in forms that retard migrationfrom point of application [6]. Therefore, total phosphorusin biosolids may not be relevant in considering the riskposed by phosphorus loss from fields to aquatic systems.Rather, to properly assess potential risk of biosolids-derivedphosphorus to receiving waters, it may be more important toconsider the various fractions of phosphorus in biosolids andtheir behaviour in soil (e.g., migration and transformation).

Generally, phosphorus has the potential of being trans-ported to aquatic systems through three major pathways:surface runoff and erosion, subsurface flow, and tile drainage[4, 7]. To a smaller extent, it can also be transported bywind erosion and deposition [8]. Runoff and erosion areimportant pathways of soil phosphorus loss [9, 10], and themajority of studies on phosphorus loss from agricultural land

Hindawi Publishing CorporationApplied and Environmental Soil ScienceVolume 2016, Article ID 3460939, 8 pageshttp://dx.doi.org/10.1155/2016/3460939

Page 2: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

2 Applied and Environmental Soil Science

are devoted to losses through runoff and erosion [11–16].Application of municipal biosolids, specifically, can increasetotal phosphorus (TP) in runoff from soil in laboratorymesocosms [17], although loss of P in runoff in agriculturalsoils may be dependent on the stabilization method used toproduce the biosolids [18–20]. These losses represent onlyhorizontal migration of phosphorus through surface runoff,while vertical migration of phosphorus through the soillayers can also contribute to the phosphorus escape fromagricultural lands [21]. It is especially significant in areas withlittle slope, areas with shallow groundwater, dry areas, or lessweathered soils and organic soils that have a low phosphorus-sorbing capacity [22, 23]. Vertical migration represents apotential route for phosphorus loss in agricultural areas, yetfew studies have considered vertical phosphorus migration,and none were found to have considered vertical migrationand evolution of the various phosphorus fractions relevant tobiosolids-amended soils.

The purpose of this study was to determine, in a labora-tory setting, how land application of biosolids might affectvarious phosphorus fractions in soil, time-related transfor-mations among fractions, and vertical loss of phosphorus toleachate.

2. Material and Methods

2.1. Experimental Setup. In order to study vertical P migra-tion, a series of soil columns were constructed in the labo-ratory [24]. Laboratory soil columns consisted of a series ofeight plastic columns (7 cm diameter, 60 cm height). Thesecolumns had rubber end-caps, and a plastic funnel (7 cmouter diameter) was inserted into each column with the stemof the funnel protruding through a hole in the end-cap. Thebottom 10 cm of the column (immediately above the funnel)was filled with river gravel to improve the drainage of theleachate percolating through the soil and to prevent soil fromescaping through the funnel. Above the gravel, each columnwas filled with 40 cm of sandy loam soil. The soil had a bulkdensity of 1.4with 3%organicmatter and a pHof 6.5 and has agoodwater drainage. It is commercially available from “CircleFarms” in BrantfordOntario and it was selected as it is a goodrepresentative for the farm soils in southern Ontario. Thefour randomly selected columns were amended with 3.65 gof anaerobically digested biosolids (dry weight), equivalentto a rate of 8Mg (dry weight) ha−1. This was achieved byadding 260mL of biosolids at 1.4% dry matter on top ofthe soil in each column selected for biosolids applicationand incorporated into the top 5 cm. Reference columns werewatered with the same volume of distilled water (260mL).The biosolids used in the current research were produced ata Southern Ontario wastewater treatment plant. The sewagetreatment process at this plant utilizes a conventional sec-ondary activated sludge process with chemical phosphorusremoval and anaerobic sludge digestion. Secondary treatmentinvolves phosphorus removal via precipitation with iron(in form of ferric chloride) followed by the addition ofsodium hypochlorite as a disinfectant to the treated water.Consequently, precipitated FePO3 becomes a constituent ofthe activated sludge and ultimately the biosolids. Anaerobic

digestion of the sludge occurs in airtight reactors over a two-week period. Biosolids produced at this wastewater treatmentplant are either used on agricultural land or dewatered andlandfilled. In Ontario, 8 Mg of biosolids (dry weight) per haof land per 5 years is the common application rate [25] andwas used in other similar studies [26].

2.2. Sampling. An initial set of soil samples (before biosolidsapplication) was collected for analysis of phosphorus frac-tions, including the Olsen sodium bicarbonate extractablephosphorus. Subsequent sample collections were performedwith decreasing periodicity: two weeks, one month, twomonths, three months, and five months after biosolidsapplication. The duration of the experiment approximateda growing season for southern Ontario. At each samplingperiod, approximately 2 g of soil samples was collected fromtwo different depths within the soil columns (3 cm from thetop and 35 cm from the top). Due to the 1.4 bulk densityof the soil, each soil sample had a volume of approximately3 cm3. The samples were collected by drilling holes in theplastic columns, extracting one soil aliquot per each column,at each of the two depths, and subsequently sealing the holeswith silicone glue.Water (approximately 200mL per column)was added to columns on a weekly basis. Leachate sampleswere collected with decreasing periodicity: 1 day, 2 weeks, 1.5months, 2 months, 3 months, and 5 months after biosolidsapplication. All sampling events happened next day afterwater was added to the columns [24].

2.3. Chemical Analysis. Biosolids, nonamended soils, andbiosolids-amended soils were analyzed (reagents and con-centrations are indicated after each of the forms) for variousinorganic (water-soluble, distilled water; loosely bound, 1MNH4Cl; metal-bound, 1M NaOH; and calcium-bound, 0.5MHCl) and organic (labile, 0.5M NaHCO3; moderately labile,1M HCl; and nonlabile, ash at 555∘C) phosphorus formsusing the sequential fractionation procedure. For the water-soluble phosphorus, 0.5 g of soil sample (dry weight) wasplaced into a 50mL Nalgene centrifuge tube and 25mL ofdistilled water was added. The supernatant was separatedfrom the solid residue by centrifugation, filtered through a0.22𝜇m filter (paper filter), and analyzed colorimetricallyusing the ascorbic acid, molybdate method. The residual soilwas kept for the next fractionations step, where persulfatedigestion for nonlabile phosphorus was replaced by strongacid digestion [27]. The leachate from the columns was ana-lyzed for soluble reactive phosphorus (SRP) according to theprocedure described byKovar and Pierzynski [27] which is anadaptation of the classical ascorbic acidmethod [28]. In addi-tion, the Olsen phosphorus soil test was determined using0.5M NaHCO3 according to the standard procedure [27].

2.4.Modeling P Concentrations. Based on the results of initialsoil and biosolids phosphorus analysis, a simple model wascreated to predict soil phosphorus increases after biosolidsapplication. The expected phosphorus concentrations (𝑐𝑓)were calculated for each form of phosphorus based uponthe initial concentration of each form in the soil (𝑐1), the

Page 3: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

Applied and Environmental Soil Science 3

concentration of each form in the biosolids (𝑐𝑏), the totalmass of soil (𝑀𝑠), and the quantity of biosolids added (𝑀𝑏)as follows.

𝑐𝑓 = 𝑐1 + 𝑐𝑏 ∗𝑀𝑏

𝑀𝑠. (1)

2.5. Statistical Analysis. A generalized linear mixed model(GLMM)was used to compare the quantities of various formsof phosphorus in biosolids-amended soil versus referencesoil, in surface soil versus bottom soil, and over time. More-over, a GLMM can model response data with non-Gaussiandistributions (e.g., exponential, lognormal) and can modela diversity of residuals correlation structures related to thelongitudinal variable (e.g., Gaussian, compound symmetry,linear, power, and exponential). General linear mixed modelANOVAs (PROC GLIMMIX, SAS 9.4, SAS Institute, Cary,NC, USA) were used to detect the primary effects of biosolidsapplication and location, as well as the interaction betweenthese factors and time, to determine if concentrations ofvarious forms of P followed different trajectories in responseto treatment (biosolids versus reference) or location (topversus bottom). Such models can be used to fit longitu-dinal models for data, regardless of whether the responseis linear with respect to the longitudinal variable (here,time). GLIMMIX models were run iteratively, with differentcombinations of specified covariance structure and responsevariable distributions. The final models were selected on thebasis of fit (based upon Akaike Information Criterion (AIC))and residuals distribution.

3. Results and Discussion

The results of the initial soil phosphorus analysis (Fig-ure 1(a)) revealed that the total phosphorus concentra-tion was 0.226mg/g of soil. This value is in range withother agriculture soils (0.050mg/g and up to 1.000mg/g)[29, 30]. Potentially readily available phosphorus fractionsrepresented by inorganic water-soluble and organic labilefractions were below the detection limit (BDL) of themethodwhich is 0.005mg/g. This may indicate a significant sorptioncapacity of the soil, although this was not explicitlymeasured.Inorganic loosely bound (0.055mg/g of soil) and organicmoderately labile fractions (0.022mg/g of soil), however,represent the major part of the bioavailable fractions. Theyconstituted more than 31% of the total phosphorus con-centration in initial soil. This pool of moderately availablephosphorus is almost double compared to other studies [31],reinforcing the idea that phosphorus sorption capacity ishigh for this soil. Relatively unavailable phosphorus fractions,such as inorganic calcium-bound (0.019mg/g of soil) andorganic nonlabile (0.049mg/g of soil) fractions, were alsominor.Their cumulative contribution to the total phosphorusconcentration in initial soil was approximately 13%. Theother 43% of the initial total phosphorus concentration inthe soil was represented by the metal-bound phosphorusfraction (0.115mg/g of soil), a fraction that is not directlyavailable for the plants but that can release bioavailablephosphorus under anoxic conditions. The Olsen phosphorus

NonlabileModerately labileLabile (BDL)Calcium-boundMetal-boundLoosely boundWater-soluble (BDL)

0

0.05

0.1

0.15

0.2

0.25

0.3

Cum

ulat

ive p

hosp

horu

s con

cent

ratio

n (m

g/g

of so

il)(a)

NonlabileModerately labileLabileCalcium-boundMetal-boundLoosely boundWater-soluble

0.00

1.00

2.00

3.00

4.00

5.00

6.00

Cum

ulat

ive p

hosp

horu

s con

cent

ratio

n (m

g/g

of b

ioso

lids)

(b)

Figure 1: Cumulative initial phosphorus fractions in soil (a) andbiosolids (b). Note different concentration scales between the twographs.

concentration (0.060mg/g) suggested that the soil used inthe experiment was relatively rich in phosphorus and wouldbe classified as a “no response” soil [32] meaning that thesoil is capable of producing high-yielding crops with littleor no additional phosphorus fertilizer. However, such soilmight increase the potential of phosphorus migration tosurrounding water bodies [33].

Biosolids analysis (Figure 1(b)) revealed that the totalphosphorus concentration (5.617mg/g of biosolids) inbiosolids was 21 times higher than the total phosphorusconcentration in initial soil. Individual phosphorus fractionswere also greatly exceeding those in initial soil.This indicatesthat these biosolids have the potential to fertilize the initialsoil. The distribution of the different phosphorus fractionscontributed to the total phosphorus concentration, however,was similar to the distribution observed for soil prior toamendment. Such a distribution was unexpected as theorganic fractions of phosphorus were expected to be larger(relative to total P) in the biosolids compared to the soil.An advanced level of mineralization of the biosolids mayexplain the relatively low organic phosphorus content. Thecumulative contribution of relatively unavailable phosphorusfractions, such as inorganic calcium-bound (0.454mg/g ofbiosolids) and organic nonlabile (0.550mg/g of biosolids)fractions, was 17%. The metal-bound phosphorus fraction(2.677mg/g of biosolids) represented the biggest phosphorus

Page 4: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

4 Applied and Environmental Soil Science

Beforeapplication

2 weeks 1 month 2 months 3 months 5 monthsWat

er-s

olub

le P

conc

entr

atio

n

0.000

0.005

0.010(m

g/g

of so

il)

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(a)

Beforeapplication

2 weeks 1 month 2 months 3 months 5 monthsLoos

ely b

ound

Pco

ncen

trat

ion

0.000.050.100.15

(mg/

g of

soil)

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(b)

Met

al-b

ound

Pco

ncen

trat

ion

0.000.020.040.060.080.100.120.14

(mg/

g of

soil)

Before 2 weeks 1 month 2 months 3 months 5 monthsapplication

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(c)

Calc

ium

-bou

nd P

conc

entr

atio

n

0.000.010.020.030.04

(mg/

g of

soil)

Before 2 weeks 1 month 2 months 3 months 5 monthsapplication

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(d)

Before application 1 month 2 months 3 months 5 monthsLabi

le o

rgan

ic P

conc

entr

atio

n

0.0000.0030.0060.009

(mg/

g of

soil)

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(e)

Beforeapplication

2 weeks 1 month 2 months 3 months 5 monthsMod

erat

ely la

bile

orga

nic P

co

ncen

trat

ion

0.000.020.040.060.08

(mg/

g of

soil)

top refbottom ref

top biosolidsbottom biosolids

(f)

Beforeapplication

2 weeks 1 month 2 months 3 months 5 monthsNon

labi

le o

rgan

ic P

conc

entr

atio

n

0.000.020.040.060.080.100.120.14

(mg/

g of

soil)

Top ref.Bottom ref.

Top biosolidsBottom biosolids

(g)

Figure 2: Phosphorus (P) fractions in soil measured in the reference and biosolids treated soil columns: a) inorganic water-soluble P, b)inorganic loosely bound P, c) inorganic metal-bound P, d) inorganic calcium-bound P, e) organic labile P, f) organic moderately labile P, andg) organic nonlabile P. The error bars represent standard deviation among replicate samples.

pool in biosolids and contributed 47% to the total phosphorusconcentration. High metal-bound phosphorus percentagein biosolids has already been reported by other studies[34, 35]. This is consistent with the wastewater treatmentprocedure for phosphorus removal. Readily available water-soluble (0.174mg/g of biosolids), inorganic loosely bound(0.201mg/g of biosolids), and organic labile (0.175mg/g ofbiosolids) fractions in biosolids represented minor poolsof phosphorus. Their cumulative contribution to the totalphosphorus concentration was 10%. The greatest differencebetween biosolids and the soil in the relative contributionto the total phosphorus was found for the moderately labileorganic fraction: 1.385mg/g of biosolids (25% of total phos-phorus) versus 0.022mg/g of soil (8% of total phosphorus).

This high value of moderately labile organic fraction wasexpected as it is relatively common in the biosolids [35].

The results of soil samples analysis after biosolids applica-tion are illustrated in Figure 2. When analyzing the statisticalsignificance of changes in phosphorus fractions concentra-tions, the family ofmixedmodels that consistently resulted inbest fit (based on AIC and residuals distribution) were thosethat fitted a log normal distribution in the response variables(P pools) and that modeled a compound symmetry residualscovariance structure. All reported statistical results are basedupon models of this form (Table 1).

As a general trend, concentrations of all P fractions variedover time (Table 1). The water-soluble (Figure 2(a)) and theorganic labile (Figure 2(e)) phosphorus fractions increased

Page 5: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

Applied and Environmental Soil Science 5

Table 1: Generalized linear mixed model (GLMM) results for various P pools.

Inorganic P Organic PWater-solubleP (AIC 48.3)

Loosely boundP (AIC 24.5)

Metal-boundP (AIC 42.2)

Calcium-boundP (AIC 118.5)

Labile P(AIC 27.7)

Moderately labile P(AIC 29.8)

Nonlabile P(AIC 32.4)

𝑝-valueTreatment (biosol. versusref.) 0.3213 0.8956 0.4507 0.7984 0.5585 0.6280 0.5083

Location (top versusbottom) 0.5762 0.7523 0.4934 0.5819 0.3401 0.5174 0.0551

Time <0.0001 <0.0001 <0.0001 0.0017 <0.0001 <0.0001 <0.0001Time × treatment 0.8539 0.8745 0.5661 0.5791 0.8268 0.9211 0.9942Time × location 0.0248 0.6792 0.8801 0.6515 0.7214 0.8461 0.2205

over time, showing some potential for long term phosphorusremobilisation. Although these increases were statisticallysignificant, the maximum amount by which these fractionsincreased remains very low at less than 0.005mg/g of soil(Figure 2(a)).

The loosely bound phosphorus concentrations were con-stant for the first two months and then increased by 50%at the three-month period (Figure 2(b)). As the increasein loosely bound phosphorus concentrations was observedfor both reference and biosolids-amended soils, it could beexplained in part by a 30% decrease in the metal-boundphosphorus fraction (Figure 2(c)) rather than by biosolidsapplication. The metal-bound phosphorus decreased overtime for both treatments in both top and bottom of the soilcolumn.The transformation of the metal-bound phosphorusto the loosely bound phosphorus could have occurred underanoxic conditions inside of the soil columns.

Over a five-month period, the concentration of calcium-bound phosphorus decreased by 35% (Figure 2(d)). Thecalcium-bound fraction constitutes mainly phosphates fromthe composition of hydroxyapatite mineral, which makes ita relatively stable fraction [27]. The reduction over time ofthe calcium-bound fraction is hard to explain, and furtherinvestigation may be required. In general, the hydroxyapatitephosphorus constitutes a fraction that leads to an overesti-mation of phosphorus impact on ecosystems in studies whereonly the total phosphorus is measured.The dissolution of thisform in soil is usually limited to a substantial drop in pH.Thesandy loam soil used in the present study has little bufferingcapacity and as a consequence, accumulation of organic acidsmay lead to some local dissolution of the hydroxyapatitefraction.The organicmoderately labile (Figure 2(f)) and non-labile (Figure 2(g)) phosphorus concentrations also increasedover the five-month period.No explanation for the changes inorganic moderately labile and organic nonlabile phosphorusconcentrations was found.

One of the main objectives of the present study wasto establish in a laboratory setting if biosolids may bringa significant contribution to different phosphorus fractionsin agricultural soils. Surprisingly, the chemical analysis ofthe pools of phosphorus fractions showed that no statisti-cally significant difference was induced by the application

of biosolids. No statistically significant difference betweenbiosolids-amended soils and reference soils was observedfor any phosphorus pool, nor did changes in phosphorusconcentrations over time differ between treatments (time ∗treatment effect).While some forms of phosphorus did showa time-related change, this was due to chemical and biologicalprocesses in the soil and not linked to the application ofbiosolids. Same trends were observed in both the treatedand the reference experimental columns. Therefore, it couldbe concluded that no measureable increase occurred inany phosphorus fraction as a result of biosolids application(Figure 2). Only water-soluble P differed over time betweenthe top and bottom (time ∗ location effect). While water-soluble P increased over time in both the top and the bottomof the soil column, the increase was greater in the top portionof the soil than in the deeper soil.

According to themodel (Table 2), an increase in almost allphosphorus fractions was expected in the top 5 cm of the soilcolumns immediately following biosolids application (67%increase for water-soluble, 4% increase for loosely boundphosphorus, 29% increase for metal-bound phosphorus,27% increase for calcium-bound phosphorus, 60% increasefor organic labile phosphorus, 77% increase for organicmoderately labile phosphorus, and 24% increase for organicnonlabile phosphorus). However, the expected increase inmost pools was near or below the nominal limit of detectionfor phosphorus analysis. When phosphorus enrichment tothe entire column was considered, the relative increasein each fraction was smaller still, with absolute increasesbelow the detection limit for all pools except metal-boundphosphorus. Therefore, this model predicted that applicationof biosolids with the moderately high total phosphorusconcentration, at recommended rates in Ontario, to a fertilesoil would result in no measureable increase in phosphoruspools for the integrated soil column, and only marginallydiscernable increases in the top 5 cm, where the material ismost concentrated.The interesting aspect of land applicationsof biosolids is that despite their relatively large phosphorusconcentrations of both bioavailable and unbioavailable formswhen compared to the soil concentrations, their impact onthe final concentrations in amended soils, due to limitsimposed on the application rates, is rather limited. Percentage

Page 6: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

6 Applied and Environmental Soil Science

Table 2: Quantitative phosphorus concentration increases expected in the entire length of the soil columns within 1 week from biosolidsapplication.

Inorganic fractions Organic fractions

Water-soluble P Loosely bound P Metal-bound P Calcium-boundP Labile P Moderately labile P Nonlabile

PExpected increasein P fractions (%)Top 5 cm 67.0 4.5 28.7 26.5 59.9 76.8 23.5

Expected increasein P fractions (%)Entire column 8.4 0.6 3.6 3.3 7.5 9.6 2.9

change calculations from biosolids concentrations, soil con-centrations, and application rates translate to relatively smallincreases in the nominal concentrations of the phosphorusforms in the soil. The detection limit allows accurate mea-surement of ≥0.1mg P/kg soil. The changes in concentrationare below this value, so soil phosphorus remained virtuallyunaffected after biosolids application.

The experimental design accounted for both temporalchanges and potential vertical migration of the phosphorusin the soil columns.The narrow diameter of the columns wasmeant to avoid lateral escapes of the phosphorus, limitingthe potential migration of the phosphorus fractions to thevertical direction. The data obtained from the upper layerand from a depth of 35 cm in the columns showed nodifference for any phosphorus fraction between the treatedand untreated soils. This suggests that the vertical transportof phosphorus remained insignificant for the duration of theexperiment, regardless of the phosphorus fraction consid-ered. As mentioned, changes in concentrations of P at thetop of the column were low to statistically insignificant. Thepossiblemigration of these nutrients towards the lower regionof the column did not occur in the case of this study. Soiladsorption and biological fixation are both mechanisms thatcould explain this lack of mobility.

The soil and biosolids used in this experiment repre-sented a kind of worst-case scenario, that is, phosphorus-rich anaerobically digested biosolids applied to soil that wasalso phosphorus-rich, providing conditions under which thephosphorus might be expected to migrate through the soiltowards the drainage system rather than being immobilized[33]. This was not observed. Accordingly, it is unlikely thatphosphorus vertical migration would be observed follow-ing application to more phosphorus-poor soils with higheradsorption capacity for phosphorus, or in soils receivingbiosolids produced by further processing such as alkalinestabilization or drying which may decrease phosphorusmobility.

In order to account for the phosphorus movement inthe soil columns, the laboratory-based experimental setupallowed the collection of water percolating down through thesoil. These leachate samples collected from both biosolids-amended and reference soil columns were analyzed forsoluble reactive phosphorus.

The concentrations of soluble reactive phosphorus inleachate samples collected from biosolids-amended soil

columns were noted to be very close to the concentrationsof soluble reactive phosphorus in leachate samples collectedfrom reference soil columns (Figure 3). No significant differ-ence was observed between samples (𝑡46 = 0.31, 𝑝 = 0.758).The absence of a significant difference in phosphorus concen-trations between leachate from biosolids-amended columnsand leachate from reference columns is in accord with thelack of statistical difference between the concentrations ofvarious forms of phosphorus in biosolids-amended columnsand reference columns (Figure 2). Within the five monthsof the research, leachate from both biosolids-amended soilcolumns and reference soil columns demonstrated phos-phorus concentrations around 0.039–0.054mg/L.These con-centrations were much smaller than the concentrations ofphosphorus measured in runoff from biosolids-amendedsoils [17, 20, 29, 36–38]. but still exceeded concentrationssuggested as optimal for limiting eutrophication potential(below 0.025mg/L in streams and 0.01mg/L in lakes) [39].Horizontal migration of P in runoff and erosion soon afterland application would seem to be a much more importantroute of potential loading to surface water than verticaltransport and groundwater transfers.

4. Conclusions

The results of the soil analysis revealed that concentrations ofseveral phosphorus fractions changed significantly over time.The water-soluble, the organic labile phosphorus, and theloosely bound phosphorus concentrations increased duringthe fivemonths of the experiment. However, this increase wasobserved for both reference and biosolids-amended soils andcan be linked to a decrease in the metal-bound phosphorusfraction which could have occurred under anoxic conditionsinside of the soil columns.

No statistically significant difference between biosolids-amended soils and reference soils was observed for any phos-phorus pool, nor did changes in phosphorus concentrationsover time differ between treatments (time∗treatment effect).Therefore, it can be concluded that no measureable increaseoccurred in any phosphorus fraction as a result of biosolidsapplication. Thus, phosphorus from the biosolids-amendedsurface does not measurably migrate through the soil pro-file towards underground tile drainage systems under theconditions simulated within the current research. This wasconfirmed by the lack of significant difference between

Page 7: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

Applied and Environmental Soil Science 7

1 da

y

2 w

eeks

1.5

mon

th

2 m

onth

s

3 m

onth

s

5 m

onth

s

From reference columnsFrom biosolids-amended columns

0.00

0.01

0.02

0.03

0.04

0.05

0.06

0.07C

once

ntra

tion

of P

(ppm

)

Figure 3: Concentrations of soluble reactive phosphorus in ana-lyzed leachate. The error bars represent standard deviation amongreplicate samples.

concentrations of soluble reactive phosphorus in the leachatefrom various columns.

The current study provided laboratory-based evidencethat anaerobically digested biosolids with phosphorus con-centration of 5.6mg/g of biosolids or below, when applied atthe rate of 8 dry tons (dry weight) ha−1 to sandy loam soilswith no or minimal slope, do not increase P leaching.

Additional Points

Core Ideas.Weexamined the impact of biosolids on soil phos-phorus fractions in vertical profiles. Concentrations of severalphosphorus fractions changed significantly over time.Mobilephosphorus fractions increased during the five months of theexperiment. No difference between biosolids-amended andreference soils was observed. In specific conditions, biosolidscan be applied without risk of increased P leaching.

Competing Interests

The authors declare that they have no competing interests.

Acknowledgments

This paper was possible due to the financial support providedby the Environmental Applied Science and Managementgraduate program from the Yeates School of Graduate Studies(YSGS) at Ryerson University.

References

[1] EPA, Land Application of Biosolids: Process Design Manual,Taylor & Francis, 1997.

[2] A. Atalay, C. Bronick, S. Pao et al., “Nutrient and microbialdynamics in biosolids amended soils following rainfall simula-tion,” Soil and Sediment Contamination, vol. 16, no. 2, pp. 209–219, 2007.

[3] A. L. Shober and J. T. Sims, “Phosphorus restrictions forland application of biosolids: current status and future trends,”Journal of Environmental Quality, vol. 32, no. 6, pp. 1955–1964,2003.

[4] O. Oenema andC.W. J. Roest, “Nitrogen and phosphorus lossesfrom agriculture into surface waters; the effects of policies andmeasures in the Netherlands,” Water Science and Technology,vol. 37, no. 3, pp. 19–30, 1998.

[5] T. C. Daniel, A. N. Sharpley, and J. L. Lemunyon, “Agriculturalphosphorus and eutrophication: a symposium overview,” Jour-nal of Environmental Quality, vol. 27, no. 2, pp. 251–257, 1998.

[6] B. Li andM.T. Brett, “The impact of alumbased advanced nutri-ent removal processes on phosphorus bioavailability,” WaterResearch, vol. 46, no. 3, pp. 837–844, 2012.

[7] V. Smil, “Phosphorus in the environment: natural flows andhuman interferences,” Annual Review of Energy and the Envi-ronment, vol. 25, pp. 53–88, 2000.

[8] K. A. Anderson and J. A. Downing, “Dry and wet atmosphericdeposition of nitrogen, phosphorus and silicon in an agricul-tural region,”Water, Air, and Soil Pollution, vol. 176, no. 1–4, pp.351–374, 2006.

[9] J. J. Hanway and J. M. Laflen, “Plant nutrient losses from tileoutlet terraces,” Journal of Environmental Quality, vol. 3, no. 4,pp. 351–356, 1974.

[10] G. W. Randall, T. K. Iragavarapu, and M. A. Schmitt, “Nutrientlosses in subsurface drainage water from dairymanure and ureaapplied for corn,” Journal of Environmental Quality, vol. 29, no.4, pp. 1244–1252, 2000.

[11] R. Gachter, J. M. Ngatiah, and C. Stamm, “Transport ofphosphate from soil to surface waters by preferential flow,”Environmental Science & Technology, vol. 32, no. 13, pp. 1865–1869, 1998.

[12] D. W. Lucero, D. C. Martens, J. R. McKenna, and D. E. Starner,“Accumulation and movement of phosphorus from poultrylitter application on a Starr clay loam,” Communications in SoilScience and Plant Analysis, vol. 26, no. 11-12, pp. 1709–1718, 1995.

[13] J. Magid, M. B. Jensen, T. Mueller, and H. C. B. Hansen,“Phosphate leaching responses from unperturbed, anaerobic,or cattle manured mesotrophic sandy loam soils,” Journal ofEnvironmental Quality, vol. 28, no. 6, pp. 1796–1803, 1999.

[14] K. C. Makris, J. H. Grove, and C. J. Matocha, “Colloid-mediated vertical phosphorus transport in a waste-amendedsoil,” Geoderma, vol. 136, no. 1-2, pp. 174–183, 2006.

[15] J. T. Sims, R. R. Simard, and B. C. Joern, “Phosphorus lossin agricultural drainage: historical perspective and currentresearch,” Journal of Environmental Quality, vol. 27, no. 2, pp.277–293, 1998.

[16] B. L. Turner and P. M. Haygarth, “Phosphorus forms andconcentrations in leachate under four grassland soil types,” SoilScience Society of America Journal, vol. 64, no. 3, pp. 1090–1099,2000.

[17] A. Hanief, D. Matiichine, A. E. Laursen, I. Vadim Bostan, andL. H. McCarthy, “Nitrogen and phosphorus loss potential frombiosolids-amended soils and biotic response in the receivingwater,” Journal of Environmental Quality, vol. 44, no. 4, pp. 1293–1303, 2015.

[18] H. A. Elliott, R. C. Brandt, and G. A. O’Connor, “Runoffphosphorus losses from surface-applied biosolids,” Journal ofEnvironmental Quality, vol. 34, no. 5, pp. 1632–1639, 2005.

[19] C. J. Penn and J. T. Sims, “Phosphorus forms in biosolids-amended soils and losses in runoff: effects of wastewater

Page 8: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

8 Applied and Environmental Soil Science

treatment process,” Journal of Environmental Quality, vol. 31, no.4, pp. 1349–1361, 2002.

[20] R. Quilbe, C. Serreau, S. Wicherek, C. Bernard, Y. Thomas,and J.-P. Oudinet, “Nutrient transfer by runoff from sewagesludge amended soil under simulated rainfall,” EnvironmentalMonitoring and Assessment, vol. 100, no. 1–3, pp. 177–190, 2005.

[21] N. C. Hansen, T. C. Daniel, A. N. Sharpley, and J. L. Lemunyon,“The fate and transport of phosphorus in agricultural systems,”Journal of Soil and Water Conservation, vol. 57, no. 6, pp. 408–417, 2002.

[22] W. G. Harris, R. D. Rhue, G. Kidder, R. B. Brown, and R.Littell, “Phosphorus retention as related tomorphology of sandycoastal plain soil materials,” Soil Science Society of AmericaJournal, vol. 60, no. 5, pp. 1513–1521, 1996.

[23] A. E. Hartemink, “Encyclopedia of soils in the environment (4volumes), D. Hillel, J.L. Hatfield, D.S. Powlson, C. Rosenzweig,K.M. Scow, M.J. Singer, D.L. Sparks (Eds.), 2005, ISBN 0-12-348530-4, Elsevier Academic Press, Amsterdam, Hardbound,2119 pp., US$1,095,” Encyclopedia of Soils in the Environment,vol. 132, no. 1-2, pp. 240–246, 2006.

[24] Y. Markunas, Vertical phosphorus migration in biosolids-amended soils: concentrations in soils and leachates [Ph.D.thesis], Ryerson University, Toronto, Canada, 2014.

[25] Ministry of Environment and Energy, Ministry of Agricul-ture, Food, and Rural Affairs, Guidelines for the Utilization ofBiosolids and Other Wastes on Agricultural Land, Ministry ofEnvironment and Energy, Ministry of Agriculture, Food andRural Affairs, Toronto, Canada, 1996.

[26] N. Gottschall, M. Edwards, E. Topp et al., “Nitrogen, phospho-rus, and bacteria tile and groundwater quality following directinjection of dewatered municipal biosolids into soil,” Journal ofEnvironmental Quality, vol. 38, no. 3, pp. 1066–1075, 2009.

[27] J. Kovar and G. Pierzynski, Methods of Phosphorus Analysis forSoils, Sediments, Residuals, and Waters, Virginia Tech Univer-sity, Blacksburg, Va, USA, 2nd edition, 2009.

[28] J. Murphy and J. P. Riley, “A modified single solution methodfor the determination of phosphate in natural waters,”AnalyticaChimica Acta, vol. 27, no. C, pp. 31–36, 1962.

[29] T. W. Andraski and L. G. Bundy, “Relationships betweenphosphorus levels in soil and in runoff from corn productionsystems,” Journal of Environmental Quality, vol. 32, no. 1, pp.310–316, 2003.

[30] J. Liu,H.Aronsson, L. Bergstrom, andA. Sharpley, “Phosphorusleaching from loamy sand and clay loam topsoils after applica-tion of pig slurry,” SpringerPlus, vol. 1, no. 1, article 53, pp. 1–10,2012.

[31] P. P. Motavalli and R. J. Miles, “Soil phosphorus fractions after111 years of animal manure and fertilizer applications,” Biologyand Fertility of Soils, vol. 36, no. 1, pp. 35–42, 2002.

[32] OMAFRA, Macro and Secondary Nutrients—Soil Diagnostics,Edited by Q. S. P. F. Ontario, Soil Diagnostics, Government ofOntario, 2009.

[33] J. Legg, Topsoil Report Ranges, Agri-Food Laboratories, Guelph,Canada, 2013.

[34] Z. He, H. Zhang, G. S. Toor et al., “Phosphorus distribution insequentially extracted fractions of biosolids, poultry litter, andgranulated products,” Soil Science, vol. 175, no. 4, pp. 154–161,2010.

[35] X.-L. Huang, Y. Chen, andM. Shenker, “Chemical fractionationof phosphorus in stabilized biosolids,” Journal of EnvironmentalQuality, vol. 37, no. 5, pp. 1949–1958, 2008.

[36] F. R. Cox and S. E. Hendricks, “Soil test phosphorus and claycontent effects on runoff water quality,” Journal of Environmen-tal Quality, vol. 29, no. 5, pp. 1582–1586, 2000.

[37] A. N. Sharpley, W. W. Troeger, and S. J. Smith, “Water quality:the measurement of bioavailable phosphorus in agriculturalrunoff,” Journal of Environmental Quality, vol. 20, no. 1, pp. 235–238, 1991.

[38] J.W.White, F. J. Coale, J. T. Sims, andA. L. Shober, “Phosphorusrunoff from waste water treatment biosolids and poultry litterapplied to agricultural soils,” Journal of Environmental Quality,vol. 39, no. 1, pp. 314–323, 2010.

[39] V. H. Smith, G. D. Tilman, and J. C. Nekola, “Eutrophication:impacts of excess nutrient inputs on freshwater, marine, andterrestrial ecosystems,” Environmental Pollution, vol. 100, no. 1–3, pp. 179–196, 1998.

Page 9: Research Article Vertical Phosphorus Migration in a Biosolids …downloads.hindawi.com/journals/aess/2016/3460939.pdf · 2019-07-30 · Research Article Vertical Phosphorus Migration

Submit your manuscripts athttp://www.hindawi.com

Forestry ResearchInternational Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Environmental and Public Health

Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

EcosystemsJournal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

MeteorologyAdvances in

EcologyInternational Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Marine BiologyJournal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Hindawi Publishing Corporationhttp://www.hindawi.com

Applied &EnvironmentalSoil Science

Volume 2014

Advances in

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Environmental Chemistry

Atmospheric SciencesInternational Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Waste ManagementJournal of

Hindawi Publishing Corporation http://www.hindawi.com Volume 2014

International Journal of

Geophysics

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Geological ResearchJournal of

EarthquakesJournal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

BiodiversityInternational Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

ScientificaHindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

OceanographyInternational Journal of

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

The Scientific World JournalHindawi Publishing Corporation http://www.hindawi.com Volume 2014

Journal of Computational Environmental SciencesHindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

Hindawi Publishing Corporationhttp://www.hindawi.com Volume 2014

ClimatologyJournal of