Journal of Cleaner Production 230 (2019) 1266e1275

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Journal of Cleaner Production

journal homepage: www.elsevier.com/locate/jclepro

Dairy industry derived wastewater treatment sludge: Generation, type

and characterization of nutrients and metals for agricultural reuse
S.M. Ashekuzzaman*, 1, Patrick Forrestal, Karl Richards, Owen Fenton
Teagasc, Environment Research Centre, Johnstown Castle, Co. Wexford, Ireland

a r t i c l e i n f o a b s t r a c t

Article history: Globally, the processing of milk and dairy products leads to huge volumes of dairy processing wastewater
Received 26 October 2018 treated sludge. Currently, there are knowledge gaps relating to the volumes generated and the nutrient
Received in revised form and metal contents of these sludges. This lack of knowledge prevents the dairy processing industry from
1 May 2019
making informed pre and post waste generation decisions. Using Ireland as a case study volumes
Accepted 3 May 2019
generated are estimated (2012e2017) and a two year seasonal database (2016e2018) across four sludge
Available online 9 May 2019
types (bio-chemically treated activated sludge; lime treated dissolved air flotation processing sludge; a
combined treatment sludge and anaerobically digested sludge) utilising samples from nine dairy pro-
Keywords:
Dairy food industry
cessing plants was created. Results show that dairy processing sludge increased by 39% in the period up
Dairy processing sludge to 126,718 tonnes (wet weight). Database results showed that nutrient contents did not vary seasonally
Nutrients but varied significantly across sludge type and processing plants. The median values (g kg
1 dry weight)
Metals for N:P:K for the four sludge types were N: 57.2, 19.5, 46 and 70.4, P: 36.8, 65.9, 20 and 14.6, and K: 7.2,
Recycling 3.9, 2.9 and 6.1, respectively. Heavy metal concentrations across all samples were significantly lower than
Agriculture those regulated by the European Union for controlling metals accumulation in agricultural land due to
sludge recycling. The characterization profile presented in this paper serves as a national and interna-
tional reference database for future investigations that focus on the valorisation of dairy processing
sludge.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction (40
8,240 mg L
1), chemical oxygen demand (COD)

The European dairy industry is the largest milk producer in the
world accounting for approximately 160 million tonnes of milk
(22% of the world's total milk production) and this industry plays a
vital role in the agri-food sector of the European Union (EU)
(European Dairy Association, 2018). For the same reason dairy food
processing companies combined produce one of the main sources
of industrial effluent in Europe (Carvalho et al., 2013). These
wastewaters consist of fractions of milk (~2% of total milk pro-
cessed) or converted products, acidic or alkaline compounds, de-
tergents and sanitizing agents, mainly from cleaning and washing
operations (Kushwaha et al., 2011). Such wastewaters have a high
polluting potential as they are typically characterised by high
concentrations of biological oxygen demand (BOD)
* Corresponding author.
E-mail address: sm.ashekuzzaman@teagasc.ie (S.M. Ashekuzzaman).
1
Present Address of corresponding author: Teagasc, Environment Research
Centre, Johnstown Castle, Wexford, Y35 TC97, Ireland.
(430
18,045 mg L
1), nutrients (total nitrogen, TN: 14e830 mg L
1,
total phosphorus, TP: 9e280 mg L
1) and suspended solids (SS)
(24e4500 mg L
1) (Erkan et al., 2018; Andrade et al., 2015).
Therefore before discharge, dairy wastewaters must be treated at
source to meet licensed discharge limits resulting in the generation
of large amounts of settled solid-liquid fractions known as “dairy
processing wastewater treatment sludge (DPWTS)” (dry matter
typically 10e25%). Currently, there is lack of data in the scientific
literature on the composition of this waste stream which is a barrier
to optimize its valorisation process and sustainable management.
In order to meet the discharge effluent quality, the dairy processing
sector needs to achieve BOD: 16 mg L
1, COD: 125 mg L
1, SS:
30 mg L
1, TN: 5e25 mg L
1, TP: 2e5 mg L
1 and total ammonia
(NH4eN): 10 mg L
1 in the treated effluents (Gil-Pulido et al., 2018;
Ryan and Walsh, 2016).
In Ireland, the dairy industry is one of the significant contribu-
tors to the Irish agri-food exports accounting about 30%, which was
estimated to generate V4.02 billion in 2017 (Bord Bia, 2017e2018).
Due to the abolition of European milk quotas in 2015, milk

https://doi.org/10.1016/j.jclepro.2019.05.025
0959-6526/© 2019 Elsevier Ltd. All rights reserved.
 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275
production in the Irish dairy sector has already reached to about
98% (~7.2 billion litres in 2017) of the predicted increase by 2020
outlined in the national Food Harvest 2020 vision compared to the
average of reference years 2007e2009 (CSO, 2018a; Finnegan et al.,
2017b; DAFF, 2011). This means there will be an added challenge to
treat inevitably increased dairy wastewaters and tackling more
DPWTS generation in a sustainable manner. Currently, Ireland is
one of the top 10 largest producers of cow's milk in EU-28 coun-
tries, representing about 5% share of milk production in Europe
(Eurostat, 2019). Globally, an increasing consumption (2.5% per
annum) of dairy products creates the challenge of industrial sym-
biosis for operational performance and resource efficiency in terms
of less energy use, water re-use and waste minimization
(Enterprise Ireland, 2011).
Wastewater treatment processes in the dairy processing sector
mainly consist of the dissolved air floatation (DAF) technique to
remove fats, oils and greases, and traditional aerobic secondary
treatment such as bio-towers, activated sludge aeration to remove
organic material and suspended solids (Ryan and Walsh, 2016;
Kushwaha et al., 2011; Britz et al., 2006). The removal of phos-
phorus is predominantly conducted in the tertiary treatment phase
involving the use of costly chemicals such as ferric sulphate or
aluminium chloride. The use of such conventional biological and
chemical processes for wastewater treatment cause high sludge
generation and disposal problem (sludge disposal could cost up to
50% of the operation cost) (Chen et al., 2017; Fraga et al., 2017). The
DPWTS that are generated can be mainly categorised into two
types: (1) bio-chemically treated activated sludge (light to dark
brown colour) and (2) lime treated DAF sludge (light grey colour)
based on the typical dairy wastewater treatment process (Fig. 1). In
addition, a few processors use a combination of aerobic, anaerobic
or anoxic processes with advanced set up of sequencing batch re-
actors (SBRs), membrane bioreactors (MBRs) and anaerobic di-
gesters (AD) (Ryan and Walsh, 2016).
Currently, the disposal pathways of DPWTS in Ireland include
land spreading (63%) as an organic fertiliser to agricultural grass-
land, composting (13.6%) and removal by licensed contractors
(23.4%) (Ryan and Walsh, 2016). Agricultural land spreading is also
a common practice across Europe including United Kingdom,
Denmark, France, Luxemburg, Portugal, Spain and Poland, and is
regulated to comply with the waste management and nutrient
application regulations like “EU Good Agricultural Practice for the
Protection of Waters” (the Nitrates Regulations (S.I. No. 31 of 2014),)
and “Waste Management (Use of Sewage Sludge in Agriculture)
Regulations” (S.I. No. 148 of 1998). Although the benefit of dairy
processing sludge for soil fertility had been found positive in some
previous studies (Lopez-Mosquera et al., 2002, 2000), there is very
limited or hardly any comprehensive data available on the volume
Fig. 1. Flow chart of a typical dairy wastewater (WW) treatment process, sludge
generation and photographic examples of sludge samples. AC ¼ Bio-chemically treated
activated sludge; DAF ¼ Lime treated dissolved air floatation processing sludge; CM ¼
Combined treated (using both AC and DAF process) sludge; AD ¼ Anaerobically
digested sludge.
1267
and characterization of such waste stream produced world-wide.
For example, the quantification of DPWTS generation in Ireland
with seasonal physicochemical composition is rarely available in
the existing literature. The information on the concentrations of
major nutrients such as nitrogen (N), phosphorus (P) and potas-
sium (K) is required to realize and optimize the fertiliser value of
DPWTS. One of the major challenges of using organic wastes in
agroecosystems is the uncertain fertiliser efficiency and soil
nutrient cycles (Bernal, 2017). For example, the fertiliser replace-
ment value (FRV) in terms of crop nutrient availability of dairy in-
dustry sludge is presently unknown. As a first step, it is very
important to know the nutrient composition of DPWTS. Moreover,
the concepts of Circular Economy (EC, 2014) and Bioeconomy
Strategy (EC, 2012) in Europe have put new challenges of devel-
oping sustainable and integrated circular system to utilise waste
residues towards the production of food, energy, and bio-based
products (Bernal, 2017). This means a comprehensive character-
ization of dairy industry derived sludge waste is vital to open new
opportunities for technological solution and valorisation process.
The main purpose of the present study was to quantify the pro-
duction of DPWTS and to develop a seasonal characterization of the
dominant dairy processing waste streams in Ireland. This paper is
providing a first time comprehensive characterization profile of
dairy industry generated wastewater treatment sludge.
2. Materials and methods
2.1. Estimation of DPWTS generation in Ireland
The perspective of Ireland was taken as a case study and an
initial step to estimate and predict the generation of dairy pro-
cessing sludge and this can be similarly followed across other EU
countries. Firstly, sludge generation was estimated from the avail-
able data in the Environmental Protection Agency (EPA) of Ireland.
The annual environmental report (AER) published between 2012
and 2017 by the EPA of Ireland was used to extract available sludge
quantity data for the licensed Irish dairy processors. The AER re-
ports were obtained from the EPA website at the “Industrial
Emissions Directive (IED)/Integrated Pollution Control (IPC)”
licenses application documents. The annual DPWTS generation was
estimated from the registered sludge quantity in AER reports for 21
dairy processing facilities covering 11 major dairy processing
companies (Kerry Group, Arrabawn Co-op, Carbery Foods, Tipper-
ary Co-op, Lakeland Dairies, Dairygold, Glanbia, Aurivo, Town of
Monaghan, Wyeth Nutritions, and Abbott Ireland) in Ireland. The
sludge data was considered corresponding to the specific code
“020502 (i.e. sludges from on-site effluent treatment)” as recom-
mended in the “European Waste Catalogue and Hazardous Waste
List” (EPA, 2002) for wastes from the dairy products industry.
Secondly, sludge generation was predicted from the data avail-
able in the Central Statistics Office in Ireland (CSO, 2018a), Irish EPA
(EPA, 2018) and scientific literature (Finnegan et al., 2017a; Ryan
and Walsh, 2016; Shete and Shinkar, 2013; Danalewich et al.,
1998), respectively, pertaining to raw milk, sludge and waste-
water (Table S1). From the reported literature, the average waste-
water generation in the dairy industry was calculated to be
2.71 ± 0.9 (n ¼ 6) litter of wastewater per litter of raw milk pro-
cessing (wastewater to raw milk (WRM)) and this was used to
calculate the annual wastewater produced (WP, equation (1)) cor-
responding to the raw milk (RM) processing in Ireland. The AER
based estimated sludge (EPA, 2018) was used to calculate the sludge
to raw milk processing ratio (ESRM, equation (2)) between the
years 2012e2017. The average of ESRM and WRM was used to
calculate the sludge to wastewater ratio (SW, equation (3)). Then,
predicted sludge (PS) was calculated using equation (4).
1268 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275

WP ¼ WRM  RM (1) supplementary section shows typical milk processing volume in

ES
ESRM ¼
RM
Average of ESRM
SW ¼
Average of WRM
PS ¼ SW  WP
Where, WP is wastewater produced in L, WRM is wastewater to raw
milk ration (m3 m
3), RM is raw milk processing volume (L), ESRM
is estimated sludge to raw milk ration (kg m
3), ES is estimated
sludge (tonne), SW is sludge to wastewater ration (kg m
3) and PS
is predicted sludge (tonne, wet weight).
2.2. Sample collection, preparation and analysis
The dairy sludge samples were collected seasonally from nine
dairy processing wastewater treatment facilities of six of the major
dairy companies in Ireland which includes a total of 63 samples.
These samples were categorised into four types depending on the
wastewater treatment process and sludge disposal management,
such as: (1) bio-chemically treated activated sludge (“AC”), (2) lime
treated dissolved air flotation processing sludge (“DAF”), (3) com-
bined treated (using both AC and DAF process) sludge (“CM”), and
(4) anaerobically digested sludge (“AD”). The sludge sample cate-
gory, source (presented with numerical numbers like AC1-7, DAF1-
3, CM1-2, and AD1 across sludge type for different processing sites)
and sampling period is presented in Table 1. In general, this sam-
pling matrix can be considered as the most representative to pre-
sent the main dairy processing sludge type across dairy companies
in Ireland, where majority (~90%) of the processing facilities
commonly use traditional aerobic techniques involving activated
sludge and bio-towers, and some use a combination of aerobic,
anaerobic or anoxic processes with advanced set up of sequencing
batch reactors (SBRs), membrane bioreactors (MBRs) and anaerobic
digesters (AD) (Ryan and Walsh, 2016). The sampling months were
grouped into two major seasonal categories in relation to the vol-
ume of milk received for processing, where April to September
(generally summer months) and October to March (generally
winter months) represent high and low milk processing volume,
respectively, in the Irish dairy processing Industry. Fig. S1 in the
Ireland.
Seasonal sludge samples were collected from 2016 to 2018 from
(2)
selected dairy wastewater treatment facilities to assess the physi-
cochemical composition across sludge type and source (Table 1).
The samples (about 2 kg) were collected in plastic containers with
(3)
screw top lids and transferred to the laboratory for analysis. The
samples were stored in the cold room at 4  C and homogenized by a
(4) mechanical mixer within 1e2 days of collection. Some homoge-
neous sub-samples were separated for immediate analysis of dry
matter (DM), organic matter (OM) and pH. Then, enough sub-
samples (200e400 g) were transferred into petri dishes for
freezing (
20  C) and subsequently, freeze dried using ScanVac
(CoolSafe 55e9 Pro) freeze dryer at
55  C for 24e48 h. The freeze
dried samples were pulverized in a mixer mill (Retsch MM200)
with a vibrational frequency of 25 Hz for 1 min. The resulting
powder samples were stored in the falcon tubes at room temper-
ature for analysis of nutrients, trace metals and other elemental
composition.
The DM and OM were determined using standard gravimetric
method 2540 G (APHA, 2005), where a sample aliquot of 15e20 g of
fresh sludge was dried for about 20 h at 105  C in an oven followed
by ignition of the dried residue at 550  C in a muffle furnace for 1 h.
Sludge pH was determined in a 1:2.5 (w/v) ratio of fresh sludge to
deionised water solution (making up to 25 ml) by Jenway 3510 pH
meter after 1 h of mixing at 20 rpm by an end-to-end shaker. The
concentrations of nutrients (phosphorus (P), potassium (K), mag-
nesium (Mg), sulphur (S), sodium (Na), and calcium (Ca)), and
metals (arsenic (As), cadmium (Cd), chromium (Cr), copper (Cu),
nickel (Ni), lead (Pb), zinc (Zn), aluminium (Al), iron (Fe), cobalt
(Co), molybdenum (Mo) and manganese (Mn)) were determined by
an Agilent 5100 synchronous vertical dual view inductively coupled
plasma optical emission spectrometer (Agilent 5100 ICP-OES)
following the microwave-assisted acid digestion of freeze dried
powder samples (USEPA, 1996). Also, freeze dried samples were
analysed for total carbon (TC) and total nitrogen (N) by high tem-
perature combustion method using LECO TruSpec CN analyser.
2.3. Data analyses
The results of all analytical parameters (i.e. continuous vari-
ables) were statistically analysed involving analysis of variance
(ANOVA), pairwise significance test (statistically significant when
p < 0.05), correlation coefficients and principal component analysis

Table 1
DPWTS sampling matrix.

Sample type Source Sampling period e montha/year Seasonal categoryb

2016 2017 2018 ApreSep OcteMar

AC AC-1 Mar, Oct Feb (n ¼ 2), May, Aug e 2 4

AC-2 Mar, Nov Mar, May, Jul Feb 2 4
AC-3 e May, Jul, Oct Feb 2 2
AC-4 Mar, Jul, Oct Feb, May, Jul e 3 3
AC-5 Aug, Oct Mar, May, Aug e 3 2
AC-6 Aug, Oct Mar, May, Aug Feb 3 3
AC-7 Nov Mar, May, Aug e 2 2
DAF DAF-1 Mar, Oct Mar, May, Aug Feb 2 4
DAF-2 Mar, Nov Jan, May, Aug e 2 3
DAF-3 Aug Mar, May, Aug, Oct Mar 3 3
CM CM-1 e Nov Feb, Apr 1 2
CM-2 e Nov Feb, Apr 1 2
AD AD-1 e Oct Feb, May 1 2

AC ¼ Bio-chemically treated activated sludge; DAF ¼ Lime treated dissolved air floatation processing sludge; CM ¼ Combined treated (using both AC and DAF process) sludge;
AD ¼ Anaerobically digested sludge.
a
Months presented with the respective first 3 letters.
b
ApreSep ¼ high milk processing season (n ¼ 27 samples) and OcteMar ¼ low milk processing season (n ¼ 36 samples).
 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275
(PCA) across the four DPWTS sample categories to assess the het-
erogeneity of these variables and to provide an insight into
elemental clustering. The samples were collected category wise
from different sources (herein, different dairy processors) at
different seasonal months that covered two major seasons of milk
processing volume (sampling matrix in Table 1). Significant differ-
ences in the physicochemical parameters across the sample cate-
gories were assessed by one-way analysis of variance (ANOVA) and
Kruskal-Wallis test, respectively, for normal and non-normal data.
The Shapiro-Wilk test was used to assess the distribution of data
under each sample category. Tukey's HSD (for normal distributions)
and Mann-Whitney (for non-normal data) tests were performed to
identify the pairwise significant differences with adjustment to p-
values (Bonferonni Correction). Correlation analysis (Pearson's
product-moment correlation for normal distributions and Spear-
man's rank order correlation for non-normal data) of Ca and Al to N,
P, K, DM, OM and TC across sample categories was performed to
identify the association of these parameters due to the use of
dominant chemicals (e.g. Ca, Al) in the dairy processing plant's
wastewater treatment process.
3. Results and discussion
3.1. Trend of DPWTS generation in Ireland
The quantity of dairy industry generated sludge in Ireland was
estimated and predicted as shown in Fig. 2. Based on the estimation
from the AER available in the Irish EPA website, approximately
108,783 tonnes (wet weight) of DPWTS were generated in Ireland
in 2017, which was 25.5% more compared to 2012. It can be
assumed that increasing raw milk processing will increase the
quantity of dairy processing wastewater (wastewater to raw milk
ration ¼ 2.71 m3 m
3), which will likely to increase the sludge
generation. The abolition of European milk quotas in 2015 opened
the opportunity for the Irish dairy sector to increase more raw milk
processing in the recent years compared to the reference years
2007e2009 (Finnegan et al., 2017b). For example, an increasing
trend in raw milk processing by creameries and pasteurisers can be
seen in Fig. 2 from 2012 to 2017, revealing about 38.8% more in 2017
compared to 2012. Similarly, dairy processing wastewater was
increased up to 38.8% in 2017 compared to 2012 (Fig. 2).
It was observed that AER based estimated sludge quantity did
not increase consistently after 2015 with a decrease in year 2016
and 2017, respectively. This was unlikely due to the fact that both
Fig. 2. Annual raw milk processing, generation of dairy processing wastewater and sludge (wet weight reported) in the Irish dairy processing industry. The values of bar (rep-
resenting raw milk and wastewater) and line (sludge) diagrams are respectively assigned to the left and right vertical axis.
1269
milk processing and wastewater volume consistently increased in
those years. However, the calculation of sludge quantity prediction
showed a steady increasing trend between the year 2012 and 2017.
Based on the calculation, the predicted sludge quantity in 2016 and
2017 was 116,043 and 126,718 tonnes (wet weight), respectively,
which are reasonably higher compared to the AER based estima-
tion. Although it is reasonable to expect an increasing trend in
relation to what was observed in the milk processing volume
(Fig. 2), the lack of timely update and availability of the AER of some
dairy processors in the EPA website (as observed) might be a reason
for such discrepancy. Based on these results, it can be arguably
expect that the sludge quantity will increase over the coming years
with respect to more raw milk to be processed by the Irish dairy
industry as per Food Harvest 2020 and Food Wise 2025 strategy
(DAFF, 2011; DAFM, 2015).
3.2. Physicochemical composition
The results of DM, OM, pH, and concentrations of major crop
nutrients (N, P, K) and elements (Ca, Na, Mg, S, C) that were
determined in the collected DPWTS samples are presented in
Table 2. The statistical significance test showed that DPWTS sam-
ples were very different in terms of highly variable concentrations
of different parameters across four sludge categories as well as
within each treatment type irrespective of sources (except AD
sludge). Sludge type (i.e. AC, DAF, CM and AD) was observed to be a
major factor for statistically different N, P and K concentrations
across type (Table S3), where statistically significant variation
observed for N: between the pair AC
DAF, DAF
CM, DAF-AD and
CM
AD; for P: AC
DAF, DAF
CM and DAF
AD; and for K: AC
DAF
and AC
CM, respectively (Table S3). The results indicated that most
of the measured parameters were more statistically different
within AC and DAF sludge types than those in CM sludge. For
example, all the measured parameters between CM-1 and CM-2
were not statistically different, except Mg concentrations. In
respect to sludge category, the median DM value was much higher
in DAF followed by CM, AC and AD sludge. In contrary, the median
OM content in DAF sludge was the lowest among the sludge cate-
gories. This could be related to the use and dosing of chemicals
during wastewater treatment process, because higher dosing of
chemicals like Fe, Al or Ca based coagulants can lead to more
inorganic based compounds remaining in the sludge. For example,
Fe (112 g kg
1 DM) and Ca (78 g kg
1 DM) concentrations in AC-1
sludge were found to be much higher than those in most of the
1270 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275

Table 2
Dry matter, organic matter, pH and major nutrient content of DPWTS across different plants (values are presented as mean ± standard deviation of n seasonal samples).

Plant DM OM pH Total N Total P Total K Total Mg Total S Total Na Total Ca Total C

% of wt. % of DM g kg
1 g kg
1 g kg
1 g kg
1 g kg
1 g kg
1 g kg
1 % of DM

Bio-chemically treated activated sludge “AC”

AC-1 (n ¼ 6) a20.1 ± 2.5 a52.1 ± 8.5 a,b,c
7.3 ± 0.4 a45.6 ± 12.9 a,c40.7 ± 4.2 a,c,d,e9.2 ± 4.1 a2.9 ± 0.5 a
3.4 ± 0.3 a
3.8 ± 0.6 a,c
78.1 ± 50.4 a25.2 ± 4.6
AC-2 (n ¼ 6) b,d12.3 ± 1.9 b,c,d68.7 ± 6.2 a,b,c
7.3 ± 0.3 b66.1 ± 7.2 a,c39.2 ± 3.9 c,d10.8 ± 2.8 b,c4.5 ± 1.1 b,c,e6.1 ± 0.8 b,d5.1 ± 0.3 a45.2 ± 15.9 b,c,d32.0 ± 2.2
AC-3 (n ¼ 4) b,c13.6 ± 1.0 a,b60.1 ± 3.9 a,b,c
7.1 ± 0.2 a,b53.7 ± 8.7 a49.8 ± 4.8 d
14.1 ± 3.0 c
5.1 ± 1.0 c,d,e
6.0 ± 0.8 c,e7.4 ± 1.5 a
54.5 ± 6.5 a,b
25.9 ± 4.2
AC-4 (n ¼ 6) b,d11.7 ± 2.0 c,d75.3 ± 4.5 a,b
7.0 ± 0.4 a,b57.5 ± 4.8 b22.6 ± 6.2 a,e
5.7 ± 1.3 a,b
3.0 ± 1.6 d5.3 ± 0.9 d,e
5.7 ± 1.9 a45.4 ± 14.9 c,d37.7 ± 4.0
AC-5 (n ¼ 5) b,c14.3 ± 2.0 d73.7 ± 3.5 a,b
6.7 ± 0.4 b,c62.9 ± 6.9 b,c31.8 ± 5.6 e4.3 ± 0.6 d
1.9 ± 0.3 a,d
4.2 ± 0.9 e9.1 ± 1.8 b
17.2 ± 2.4 d,e
34.8 ± 5.2
AC-6 (n ¼ 6) d10.9 ± 0.9 a,b60.5 ± 3.9 a,b,c
7.2 ± 0.1 a46.6 ± 3.5 a,c38.6 ± 13.9 a,c8.3 ± 2.8 a,b,d
3.0 ± 1.2 d,e5.5 ± 1.4 a,b,d4.9 ± 1.0 a43.7 ± 14.1 a,b26.1 ± 2.5
AC-7 (n ¼ 4) c15.3 ± 1.1 a,b
58.2 ± 3.1 c
7.8 ± 0.3 a,b
55.8 ± 5.0 a,b35.6 ± 2.4 b2.9 ± 0.9 e
6.2 ± 0.8 a
3.5 ± 0.5 c,e,f
7.2 ± 1.1 c78.5 ± 5.3 a,b,e
28.5 ± 0.8
Medianx 13.3 62.9 7.3 57.2 36.8 7.2 3.2 4.8 5.3 44.8 29.4
Lime treated DAF sludge “DAF”
DAF-1 (n ¼ 6) a28.7 ± 4.1 a55.8 ± 7.8 a,c
6.8 ± 0.8 a
9.6 ± 3.3 a
13.1 ± 4.7 a
0.8 ± 0.3 a
7.4 ± 4.6 a
0.9 ± 0.2 a
4.0 ± 1.6 a
116.6 ± 39.3 a47.8 ± 10.3
DAF-2 (n ¼ 5) b21.6 ± 2.4 a51.0 ± 6.5 a
6.4 ± 0.6 b
39.5 ± 6.9 b
76.1 ± 17.4 b5.4 ± 1.7 a
4.5 ± 1.6 b,c
2.4 ± 0.5 a
3.8 ± 1.7 a
160.4 ± 44.1 b24.9 ± 3.4
DAF-3 (n ¼ 6) a,b25.8 ± 4.0 b24.2 ± 2.8 b
7.7 ± 0.2 c
20.3 ± 2.1 b,c
84.1 ± 21.3 b,c4.7 ± 1.0 a
3.7 ± 0.7 c
2.5 ± 0.5 a
3.0 ± 0.5 b
220.3 ± 31.1 c11.4 ± 1.3
Mediany 25.9 46.9 7.2 19.5 65.9 3.9 4.3 2.1 3.5 152.9 24.3
Combined treated sludge “CM”
CM-1 (n ¼ 3) a15.6 ± 3.0 a74.6 ± 1.3 a
6.7 ± 0.1 a
50.5 ± 7.9 a
23.8 ± 2.7 a
2.9 ± 0.7 a
1.2 ± 0.1 a
6.7 ± 1.4 a
5.9 ± 2.3 a
20.6 ± 7.2 a
41.8 ± 1.3
CM-2 (n ¼ 3) a18.3 ± 4.3 a58.7 ± 22.6 a
9.7 ± 3.2 a
41.7 ± 8.4 a
15.1 ± 4.9 a
3.6 ± 1.5 b
1.7 ± 0.2 a
7.9 ± 0.5 a
3.0 ± 0.9 a
28.5 ± 17.2 a
37.4 ± 11.6
Medianz 16.1 73.9 6.8 46.0 20.0 2.9 1.4 7.6 3.6 21.0 42.2
Anaerobically digested sludge “AD”
AD-1 (n ¼ 3) 3.5 ± 1.1 72.5 ± 1.3 7.5 ± 0.1 70.4 ± 1.2 14.6 ± 1.2 6.1 ± 1.1 1.9 ± 0.1 5.3 ± 0.7 19.9 ± 3.0 59.7 ± 12.0 35.6 ± 1.2

Statistical significance within treatments is indicated by different superscript letter, for non-significance: same or common superscript letter is present.
x
Median value of 37 different activated sludge samples.
y
Median value of 17 different DAF sludge samples.
z
Median value of 6 different combined treated sludge samples.

other processors' AC sludge resulting lowest OM (Table 2, Table 3).
Likewise, DAF-3 sludge contained higher Ca concentration
(220 g kg
1 DM) in comparison to other processors’ DAF Ca con-
centration range (117e160 g kg
1 DM), resulting lower OM content
(Table 2). Typically, the DM content in biosolids (stabilised organic
material derived from chemical, thermal or biological treatment of
sewage sludge (Peyton et al., 2016)) and industrial biowaste were
reported to be 24e87 and 8e41% of wet weight, respectively, and
OM in those were 28e80 and 16e96% of DM, respectively (Peyton
et al., 2016; Rigby and Smith, 2014). The range of DM and OM
observed in this study indicates a heterogeneous nature of dairy
industry derived sludge stream. The comparisons with sewage
sludge and biowaste indicate that the DM concentrations in DPWTS
are in the low range of sewage sludge. The median pH range of the
AC, DAF, CM and AD sludge samples (n ¼ 63) was observed to be 6.8
to 7.6.
The N concentration was highest in the AD sludge and lowest in
the DAF sludge, which was opposite for P concentration. The nature
of DAF wastewater treatment process with lime addition could be
the reason of lower N and higher P in DAF sludge in comparison to
other types. The use of lime causes the pH of wastewater to be in
the alkaline range, which is favourable to convert NHþ
4 to NH3 and

Table 3
Concentration (mg kg
1 DM) of trace elements in DPWTS (values are presented as mean ± standard deviation of n seasonal samples across different plants). *Values are
presented in g kg
1 DM for Al and Fe.

Plant Cr Cu Ni Pb Zn Al* Fe* Co Mo Mn

Bio-chemically treated mixed sludge “AC”

a,c a,c a a a a a a a a
1 (n ¼ 6) 12.0 ± 4.6 8.7 ± 5.5 13.9 ± 5.1 6.0 ± 2.3 132.5 ± 35.7 0.8 ± 0.9 111.9 ± 37.3 11.1 ± 3.9 0.5 ± 0.2 216 ± 69.3
a b a b a b,c b,f b,f b a,e
2 (n ¼ 6) 14.7 ± 2.6 26.4 ± 7.9 8.8 ± 1.9 2.8 ± 0.8 155 ± 36.0 24.8 ± 14.7 2.8 ± 1.0 1.6 ± 0.5 5.4 ± 1.4 180 ± 92.3
a,b a b,c b,c c,d c,e,g c,d,e c b,c,d
3 (n ¼ 4) 9.1 ± 0.9 13.3 ± 0.8 4.0 ± 0.6 <2.0 65.9 ± 5.8 33.6 ± 6.2 0.7 ± 0.3 0.5 ± 0.2 3.9 ± 0.6 40.4 ± 24.6
a,b a c b c a,c d d d,f c
4 (n ¼ 6) 9.4 ± 0.8 14.8 ± 3.0 4.0 ± 0.4 2.2 ± 0.3 64.1 ± 9.1 15.7 ± 7.3 1.4 ± 0.2 0.8 ± 0.1 2.3 ± 0.3 43.9 ± 8.9
b c d c,d b,d e,g c,e e c,d
5 (n ¼ 5) 5.4 ± 2.0 7.1 ± 1.0 1.6 ± 0.8 <2.0 51.3 ± 21.4 41.3 ± 8.5 0.7 ± 0.2 0.4 ± 0.1 1.3 ± 0.3 30.1 ± 22.9
b,c a,c c,e b,c,e e f d,f f e
6 (n ¼ 6) 8.8 ± 3.8 11.8 ± 6.8 4.7 ± 2.3 <2.0 66.7 ± 33.4 57.8 ± 17.9 2.3 ± 0.9 1.0 ± 0.5 2.6 ± 0.6 91.5 ± 45.8
a,c a,c a,c a,b b,c,f g g,e g d,f
7 (n ¼ 4) 13.3 ± 4.2 10.2 ± 5.1 6.4 ± 3.1 <2.0 119 ± 41.2 34.0 ± 2.2 0.6 ± 0.3 0.3 ± 0.1 2.1 ± 0.2 19.9 ± 8.7
Medianx 9.8 12.6 4.6 < 2.0 75.2 27.7 1.5 0.8 2.2 55.1
Lime treated DAF sludge “DAF”
a a a a a a a a a
1 (n ¼ 6) 8.1 ± 3.9 7.2 ± 1.7 4.6 ± 2.9 2.2 ± 0.3 102.8 ± 47.1 1.3 ± 0.9 1.0 ± 0.2 0.4 ± 0.1 0.5 ± 0.2 22.7 ± 10.4
b b a a b b b a a
2 (n ¼ 5) 3.7 ± 0.7 1.5 ± 0.3 2.6 ± 1.9 <2.0 70.5 ± 50.7 0.4 ± 0.1 0.3 ± 0.1 0.2 ± 0.1 0.4 ± 0.1 25.9 ± 10.4
a a a b b,c c a b a
6 (n ¼ 6) 7.2 ± 2.3 5.6 ± 3.7 10.0 ± 7.9 <2.0 29.7 ± 15.6 0.6 ± 0.2 2.6 ± 0.8 0.3 ± 0.1 2.2 ± 1.7 44.5 ± 27.6
Mediany 5.4 5.3 4.0 < 2.0 54.7 0.6 1.1 0.3 0.5 28.2
Combined treated sludge “CM”
a a a a a a a a a
LBB (n ¼ 3) 12.3 ± 6.4 14.9 ± 2.3 4.1 ± 3.4 <2.0 100 ± 43.3 50.3 ± 4.0 0.9 ± 0.2 0.4 ± 0.1 1.5 ± 0.4 25 ± 1.8
a a a a b a a b b
LLE (n ¼ 3) 8.9 ± 2.2 31.2 ± 15.5 10.5 ± 4.5 <2.0 164 ± 96.7 23.7 ± 4.3 5.2 ± 2.8 1.5 ± 0.7 2.5 ± 0.4 188 ± 57
z
Median 8.8 17.3 7.9 < 2.0 109.8 37.2 1.8 0.7 2.1 80.7
Anaerobically digested sludge “AD”
3 (n ¼ 3) 13.4 ± 3.5 38.2 ± 6.7 9.3 ± 2.4 6.3 ± 2.9 217 ± 46 1.5 ± 0.5 0.7 ± 0.1 0.9 ± 0.2 18.4 ± 3.6 28.2 ± 6.8

Concentrations of As and Cd were below <1.5 and < 0.15 mg kg
1 DM, respectively; Statistical significance within treatments is indicated by different superscript letter, for
non-significance: same or common superscript letter is present.
x
Median value of 37 different activated sludge samples.
y
Median value of 17 different DAF sludge samples.
z
Median value of 6 different combined treated sludge samples.
 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275
subsequently, releasing NH3 to the atmosphere (Libhaber and
Orozco-Jaramillo, 2012). On the other hand, higher concentrations
of Ca and P in DAF sludge indicate that lime use predominantly
caused CaeP precipitation (Ashekuzzaman et al., 2017). The higher
concentration of N in AD sludge suggests that anaerobic degrada-
tion of organic matter released more nitrogenous compounds
during wastewater treatment. For example, the hydrolysis and
acidogenesis steps of AD process generally converts the macro-
molecular compounds (proteins, lipids, and polysaccarides) into a
more simpler molecules (volatile fatty acids, ammonia, carbon di-
oxide, hydrogen sulphide, and other byproducts) (Ashekuzzaman,
2010). For K concentrations, the order was observed to be
AC > AD > DAF > CM. The median of N and P concentrations in
DPWTS samples were found to be much higher than those
observed in cattle slurry (Table 4). This means that N and P contents
of DPWTS would be a better strength of this waste for fertiliser
value when comparing with cattle slurry fertiliser. The concentra-
tions of K in DPWTS were generally lower than those in biowaste
and cattle slurry. The vast majority of K consumed by cattle and
dairy cows is released in the urine which is collected together with
the manure (Saunders, 1982). But little of the K ingested remains in
the milk, giving a relatively low concentration in the sludge after
dairy wastewater treatment. The presence of vegetable wastes (rich
in K) in the biowaste may be responsible for its high K concentra-
tion (Rigby and Smith, 2014).
The median values of other macronutrients (Mg, S, Na and Ca)
were statistically different between sludge types. The median
concentration of total C (TC) was observed to be highest in CM
sludge followed by AD, AC and DAF sludge. The lime dosing in the
treatment of DAF based wastewater could be related to the lowest
TC content of DAF sludge. The reason for low TC at the high lime
dose is likely the fact that lime is an inorganic compound, thus its
addition simply reduces the proportion of TC by increasing the
inorganic fraction.
The measured concentrations of heavy metals and arsenic in the
collected DPWTS samples are presented in Table 3. The median
values (mg kg
1 dry matter) of metals, which are currently under
EU regulatory guideline, across AC, DAF, CM and AD sludge types
showed that Cr, Cu, Ni, Pb and Zn had their highest values for AD
sludge and that of these were lowest for DAF sludge. The overall
median values of these metals for the DPWTS (n ¼ 63 seasonal
samples from 9 processing plants) were Cd: <0.15, Cr: 9.2, Cu: 11.5,
Ni: 4.8, Pb: <2.0 and Zn: 76.8 mg kg
1 dry matter (Table 5). These
values are significantly lower than those recommended in the
global standards of compost quality for heavy metals limits (Mohee
and Soobhany, 2014). For example, the EU regulation on the limits
of heavy metals for acceptable biowaste derived compost quality is
Cd: 0.7, Cr: 70, Cu: 70, Pb: 45, Ni: 25 and Zn: 200 mg kg
1 dry
matter (European Commission, 2008). Moreover, the maximum
Table 4
Typical ranges and median of dry matter, organic matter, pH and major nutrient content of DPWTS in comparison to other commonly used organic fertiliser.
a
Representing the range of 63 samples covering source, treatment and seasonal variability measured in this study.
b
Values are presented as median of 63 seasonal samples.
c
Peyton et al. (2016).
d
Rigby and Smith (2014).
e
Average values used from Teagasc Greenbook (2016).
1271
measured values of heavy metals (Cd, Cu, Ni, Pb, Zn) were found to
be very low in the present study when compared to the EU upper
limit thresholds in soil and sludge associated heavy metal con-
centrations (Table 5). The heavy metal concentrations measured in
this study were also fairly in the lower range when compared to
those typically seen in farmyard manure and biosolids for agricul-
tural land application (Table 3, Table 5). This indicates that heavy
metal concentrations will not be a limiting factor for estimating
legal application rate of dairy processing sludge for agricultural
recycling.
In general, P is considered to be the limiting factor to estimate a
legal application rate (usually 40 kg-P ha
1 for pasture establish-
ment at a low Morgan's P Index soil (e.g. P Index 2 equivalent to
Morgan's P of 3.1e5.0 mg L
1, where Morgan's P indicates plant-
available P in soil)) when applying biosolids and cattle slurry as
organic fertiliser (Ashekuzzaman et al., 2018). Considering this P
application rate of up to 40 kg-P ha
1 year
1, the estimated quantity
of dairy sludge to be applied to land would be approximately 1
tonne DM ha
1 year
1 that can be associated with heavy metal
concentrations of Cr: 0.003e0.02, Cu: 0.001e0.05, Ni:
0.0007e0.022, Pb: ~0.009 and Zn: 0.016e0.274 kg ha
1 year
1,
respectively (assuming median value of P from Table 4 and heavy
metal concentrations range from Table 5). This ingestion of heavy
metals to soil from dairy sludge land spreading is very low when
compared to the limit of average annual rate of addition of metal
such as Cr: 3.5, Cu: 7.5, Ni: 3.0, Pb: 4.0 and Zn: 7.5 kg ha
1 year
1
over a 10-year period as recommended in the “Codes of Good
Practice for the Use of Biosolids in Agriculture” (Fehily Timoney
Company, 1999; Lucid et al., 2013). Also, such metal concentra-
tions are not likely to be harmful for grassland pasture comparing
the values of phytotoxic concentrations in ryegrass (Table 5). In a
relevant study using dairy processing sludge (as nutrient source)
for grassland fertilisation over a period of 4 years, Lopez-Mosquera
et al. (2000) observed that heavy metal contents (Hg, Pb, Cd, Cu, Zn,
Ni and Cr) in both soil and grass tissue did not exceed the EU leg-
islative limits, however, their findings of a number of significant
metal-metal correlations in sludge and sludge-applied soil sug-
gested that long-term land application of sludge might be a
possible source of metal transfer to soil.
The presence of Al and Fe was also measured in DPWTS samples
with higher concentrations observed in the AC and CM sludge in
comparison to DAF and AD sludge (Table 3). The main source of Al
and Fe in AC and CM sludge was associated with the use of
chemicals such as Al or Fe based salts for reducing nutrients
(mainly P) from wastewaters and their concentrations varied
widely across different processing plants within AC and CM type.
Worldwide, chemical and combined biological
chemical treat-
ment by using Al and/or Fe salts for effective P removal from
sewage wastewater is the most common treatment method
1272 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275

Table 5
Concentration (mg kg
1 dry weight) range and mean of trace elements in DPWTS, comparison with other organic fertiliser, European Union (EU) regularity upper limit values
in soil and sludge for agricultural land application, and phytotoxic concentrations in ryegrass.

Plant Cd Cr Cu Ni Pb Zn

Rangea <0.15e0.4 3.2e19.6 1e47.9 0.7e22.3 <2e9.6 16e274

Medianb <0.15 9.2 11.5 4.8 <2.0 76.8
Cattle slurryc <0.2 1 3.9 0.44 <0.25 14
Farm Manured 0.1e0.8 1e55 2e172 2e30 1e27 15e566
Biosolidsc,e 0.4e13 8e51 112e756 12e140 11e791 219e1273
DPSf 0.11 16 59 11 10.1 290
EU limit-soilg 3 e 140 75 300 300
EU limit-sludgeg 40 e 1750 400 1200 4000
Phytotoxicityh >100 >100 >20 >80 e >400
a
Representing the ranges of 63 samples covering source, treatment and seasonal variability measured in this study.
b
Values are presented as median of 63 seasonal samples.
c
Peyton et al. (2016).
d
Lopez-Mosquera et al. (2000).
e
Biosolids are treated sewage sludge, values adapted from Peyton et al. (2016) and Healy et al. (2016b).
f
Dairy processing sludge (DPS) data adapted from Lopez-Mosquera et al. (2000).
g
Limit values taken from EU Directive 86/278/EEC (EEC, 1986).
h
Phytotoxicity of metals in ryegrass adapted from Healy et al. (2016a).

(Øgaard and Brod, 2016). The median of Al was more dominant

than that of Fe in both AC and CM sludge types, which indicates the
wider use of Al salts across processing plants. This means Al is likely
to be transferred to soil when DPWTS of AC and CM types are
applied to agricultural land, which may pose perceived threats to
soil quality and agronomic yield. However, two long term incuba-
tion studies (Brennan et al., 2014; O'Flynn et al., 2018) have already
shown that chemically amended dairy slurry and pig slurry (with
alum and ferric chloride) were beneficial in terms of their capacity
to sequester dissolved reactive P and did not negatively affect plant
available P. In another long-term study Moore et al. (1998) inves-
tigated the effect of alum added poultry litter on the reduction of
ammonia volatilization and P runoff losses, where they observed a
positive outcome (ammonia volatilization and P runoff reduced by
97 and 75%, respectively) with no increase of Al availability in soils,
Al runoff, or Al uptake by plants. Al is a strongly hydrolysing metal
and is hardly soluble at pH > 5.5 (ranged from 6.0 to 8.0) (Canadian
Environmental Protection Act (CEPA), 1999).

3.3. Spatial and temporal variation of DPWTS

The PCA results as presented in Fig. 3 showed that the clustering

of data points in the sample locations was different across sludge
type based on their composition of DM, OM and nutrients (e.g. N, P,
K, Mg, S, Na, Ca and TC). Principle component (PC) 1 and 2
accounted for 68% of the variation in the overall dataset. Along the
PC 2 axis, most of the data points of DAF sludge varied in the same
direction, whilst those of AC and AD sludge varied together and
separately. The PC 1 axis separated sample locations between DAF
and AC, and DAF and AD sludge, respectively, which contained
higher or lower values of the analysed parameters. Similarly, ma-
jority of the data points of AC and CM sludge varied in the opposite
direction and separately along the PC 1 axis with the sample
location separated by the PC 2 axis. Thus, these results revealed a
clear distinction among the dominant sludge streams, where strong
association was also observed between some parameters. For
example, Ca and P were significantly associated with the DAF
sludge. The AC and AD sludge samples had higher association with
N, K, Na and S, whilst CM sludge with OM and TC, respectively. The
correlation of Ca and Al to N, P, K, DM, OM and TC across sample
type was analysed to identify the association of these parameters
due to the use of dominant chemicals (i.e. Ca, Al) in the dairy
processing plant's wastewater treatment process.
It was observed that Ca is one of the dominant elements across
Fig. 3. Principal component analysis DPWTS samples based on the 630 datasets of 63
samples by 10 parameters (DM, OM, N, P, K, Mg, S, Na, Ca and TC).
sludge categories and sources with higher Ca concentration prev-
alence in DAF sludge followed by Al in particular being the domi-
nant element in AC and CM sludge, respectively (Table 2, Table 3). It
was found that Ca content in AC sludge had strong significant as-
sociation with DM, OM and TC, respectively, where Ca
DM was
positively correlated (r ¼ 0.379, p < 0.05), and Ca
OM (r ¼
0.619,
p < 0.0001) and Ca
TC (r ¼
0.366, p < 0.05) were inversely
correlated, respectively. Similarly, Ca in DAF sludge was observed to
be inversely correlated with OM (r ¼
0.770, p < 0.001) and TC
(r ¼
0.866, p < 0.0001). This means higher concentration of Ca in
sludge was associated with lower organic matter and total C con-
tent, which was also reflected in PCA analysis due to opposite
localisation of OM and TC with respect to Ca (Fig. 3). The Ca content
in DAF sludge was positively correlated with the P content with
strong significance (r ¼ 0.831, p < 0.0001). This means addition of
lime in DAF based dairy wastewater treatment process was a sig-
nificant factor in having the highest P content in DAF sludge among
other sludge categories in this study. The use of lime to precipitate P
 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275
or to stabilise sludge is also common during the sewage treatment
process and in this respect a number of studies reported different
results on the plant availability of sludge P (Øgaard and Brod, 2016;
Shu et al., 2016; Kahiluoto et al., 2015; Shober et al., 2006). For
example, Shu et al. (2016) conducted a long-term study to examine
the effect of lime treated biosolids on the dynamics and bioavail-
ability of biosolids P in acidic soils, where they observed an increase
in Mehlich 3 P (M3P), water extractable P (WEP), and the P satu-
ration index (PSI) for application rate between 14 and 42 Mg ha
1
year
1. The effect of Al and Fe on the P fertilisation using 11 sewage
sludges (these were varied widely in amounts and ratios of Al and/
or Fe salts to capture P from wastewater) was assessed in a pot
experiment with ryegrass and a nutrient-limiting sand-peat soil
mixture by Øgaard and Brod (2016). They found that the P avail-
ability from these sludges in terms of mineral fertiliser equivalent
(MEF) was low in comparison to mineral fertiliser due to consid-
erably high (Fe þ Al)/P ratio (between 2.8 and 13.0). The liming of
those Al and/or Fe rich sludge in the same study was observed to be
beneficial to increase the P availability of Al-/Fe-bound P with
better MEF performance for higher FeeP precipitated sludge, which
was caused by higher solubility of FeeP than AleP with increasing
pH. An increase in pH by liming of sludge liberates P release from
Al/Fe-bound P in sludge and subsequently, increases both labile P
(NaHCO3 extractable P) and stable CaeP (HCl extractable P). Some
studies reported the low solubility of CaeP (mainly hydroxyapatite)
when Al/Fe precipitated sludge was post-treated by lime addition
(Kahiluoto et al., 2015; Shober et al., 2006).
Interestingly, no significant correlation was observed between Ca
and P, and Al and P in AC sludge, while the concentrations of both Ca
and Al were generally dominant in AC sludge. Instead, a significant
polynomial regression (y ¼
11.469  2 þ 33.78x þ 19.97,
R2 ¼ 0.8824, p ¼ 0.0403, y ¼ P concentration and x ¼ Ca/Al ratio
(weight basis)) was observed between Ca/Al ration and P concen-
tration in AC sludge. This regression indicates that the dosing of both
Ca and Al based chemicals during wastewater treatment process
should be at an optimal ratio for efficient P removal. In the CM sludge
with the prevalence of Al, a positive significant correlation was
observed between Al and P (r ¼ 0.844, p < 0.05). There was no sig-
nificant association observed in N or K with the dominant presence
of Ca and/or Al across sludge categories in the present study. These
results support the main purpose (i.e. removal of P and suspended
solids) of chemical dosing in wastewater treatment process and
therefore, providing a passive information on the possible associa-
tion of the selected parameters in sludge as a result of chemical use.
Also, the variation of N, P and K was statistically significant
between the sources (i.e. across dairy processing plants) for AC and
Table 6
An estimation of fertiliser equivalence value (FEV) of DPWTS (with median values) compared to other common organic materials.
Organic materials
DM OM
% of wt. % of DM
DPWTS - AC 9.4e25 43e80
DPWTS - DAF 18e32 20e66
DPWTS - CM 13.2e23 37e82
DPWTS - AD 2.2e4.4 71e74
Cattle slurrya 6.3 64.9
Biosolidsb 42.5 60.0
Biowastesc 29.2 60.0
a
Average values used from Teagasc Greenbook (2016).
b
Average values used from Peyton et al. (2016).
c
Average values used from Rigby and Smith (2014).
d
FEV is calculated based on average national price of calcium ammonium nitrate (CAN) (271 V ton
1), compound 10-10-20 (408 V ton
1) and muriate of potash (388 V
ton ) inorganic fertilisers for the year between January 2015 to May 2018 (41 months), which provide the unit price of N (0.99 V kg
1), P (1.55 V kg
1) and K (0.78 V kg
1)

1
(source: CSO (2018b)). Total FEV (V ton
1) ¼ (Total N  unit price þ Total P  unit price þ Total K  unit price) (kg ton
1  V kg
1).
1273
DAF sludge type. However, there was no statistically significant
variation observed for these major crop nutrients between seasonal
samples, where samples were assigned to two major seasons based
on the milk processing volume: 1) AprileSeptember ¼ high milk
processing season and 2) OctobereMarch ¼ low milk processing
season. This could be an indication that the concentrations of N, P
and K in the sludge samples were not significantly associated with
the wastewater volume; rather these concentrations were expected
to be strongly associated with the wastewater treatment process.
The evidence of significant correlation between Ca and P, Al and P in
DAF and CM sludge, respectively and significant regression be-
tween Ca/Al ration and P in AC sludge demonstrates such indication
in the present study.
3.4. Implication and research perspective
Valuable nutrients such as N, P and K are recycled back to soil
through land spreading of organic fertilisers which has an equiva-
lent mineral fertiliser replacement value. If the predicted sludge
generation (i.e. 126,718 tonnes (wet weight)) across the Irish dairy
industry in 2017 and the median of DM, N, P and K from Table 4 are
taken into consideration, the total quantity of N, P and K in DPWTS
is 905, 664 and 96 tonnes, respectively. Herein, the fertiliser
equivalent value (FEV) for the Irish dairy processing sludge has
been estimated from the total nutrient concentration (N, P, K;
Table 6). This provides a theoretical estimation of the total FEV of
AC, DAF, CM and AD sludge in comparison to that of other organic
fertilisers (Table 6). The plant-available FEV (67 and 27 V ton
1DM,
respectively) of cattle slurry and biosolids were only 72 and 38.6%,
respectively, of the theoretically estimated total FEV (Teagasc
Greenbook, 2016; Sullivan et al., 2015). The crop available fraction
of N and P were observed to vary widely across different organic
residue based fertilisers when applied to land (Sullivan et al., 2015;
Rigby and Smith, 2014; Lalor et al., 2011). Hence, future research
needs to be conducted to assess the fertiliser efficiency and soil
nutrient cycles using DPWTS in agronomic trials.
An expansion of this database throughout the EU dairy sector
would be beneficial to optimize the value of this waste stream by
developing effective technology on resource recovery. For example,
P recovery from DAF based sludge can be an interesting option to
consider due to its high total P (~6% of DM) and Ca (~17% of DM)
content. There is growing demand to recover and recycle P from
secondary resources like waste stream in order to achieve sus-
tainable global food security (Huang et al., 2017), a priority for the
future development agenda 2030 of the United Nations (UNDP,
2016). In this context, P recovery technologies are particularly
Total nutrient Total FEVd
N P K
kg ton
1 DM V ton
1
31e74 17e61 1.7e18 58
182 (119)
3.7e49 5e122 0.5e8 12
243 (124)
32e59 9.6e27 2.1e5.2 48
104 (79)
69e72 13.6e16 4.8e6.7 93
100 (96)
38.1 7.9 55.6 93
41.7 17.4 2.2 70
27.0 9.4 6.9 46
1274 S.M. Ashekuzzaman et al. / Journal of Cleaner Production 230 (2019) 1266e1275
focused on utilising alternative sources such as manure, sewage, or
wastewater. For example, struvite (magnesium ammonium phos-
phate, MgNH4PO4 6H2O), a P recovery product from wastewater,
has gained interest as a low soluble slow release P fertiliser with
full-scale operation of struvite production (e.g. Ostara struvite-
crystallisation processes Pearl, AirPrex and NuReSys) available in
Europe (Hukari et al., 2016). The technical recovery of P from
municipal wastewaters is approximately 2000 tonnes/year in
Europe (Hukari et al., 2016). The dairy industry in Europe is the
largest source of industrial food wastewater with high concentra-
tions of nutrients (total nitrogen, TN: 14e830 mg L
1, total phos-
phorus, TP: 9e280 mg L
1) and one of the main sources of N and P-
rich industrial effluent (Erkan et al., 2018; Carvalho et al., 2013). The
recovery of P as struvite precipitation from anaerobically treated
dairy wastewater effluent was found effective with 88.4% and 79.3%
of NHþ 3

4 and PO4 respectively being captured in struvite formation,
where the final product consisted of 3.30% N, 11.13% P, 8.64% Mg and
0.73% K (Uysal and Kuru, 2015). Due to high organic matter content
to influent P (e.g. COD: P influent ~37e40) ratio (Mulkerrins et al.,
2004), dairy wastewaters are particularly suitable for anaerobic
digestion based P removal and recovery as struvite from digestates
and/or treated effluent. Further research is required to investigate
the suitable pathway of P removal and recovery systems from dairy
wastewaters including the optimization of struvite precipitation
chemistry. In addition, P from partially to fully dried dairy sludges
can be recovered by chemical leaching, (hydro)thermal treatment,
composting, and mono-incineration for application as fertiliser
(Bradford-Hartke et al., 2015). In the recent years, a number of
studies looked into the transformation of P in the thermally treated
solid biowastes/sewage sludge and animal manures to assess its
availability for fertilisation (Huang et al., 2015, 2017, 2018), which
suggests that P speciation and availability are highly dependent on
treatment techniques and conditions that are adjustable to
enhance P recovery and recycling from different biowastes. Dairy
industry derived sludge could be an interesting feeding material
due to its high N and P content to develop novel bio-based fertiliser
through innovative scientific research. Therefore, it is important to
identify alternative treatment and disposal options of DPWTS,
which would add value to the supply chain of dairy production
process.
4. Conclusions
Globally the processing of milk and dairy products is significant
with a large volume of heterogeneous dairy processing sludge
produced. Very little is known about the content of this dairy
processing wastewater treated sludge. Herein a seasonal database
was created segmented into four sludge types (bio-chemically
treated activated sludge; lime treated dissolved air floatation pro-
cessing sludge; a combined treatment sludge and anaerobically
digested sludge). Results showed that median N, P and K concen-
trations did not vary seasonally but differed significantly across
sludge type and processing plant source. Ca and Al were deter-
mined to be the externally added dominant elements across sludge
types due to the current wastewater treatment practice across
different processors. In terms of N, P and K content of four sludge
types, AC and CM sludge were observed to have a better balance of
these (N: P: K (% dry weight) ¼ 4.6e5.7: 2e3.7: 0.3e0.7), while DAF
and AD sludge were particularly rich in P and N respectively. In
addition, dairy sludges were found to contain several micro-
nutrients required by plants including Cu, Fe, Mn and Zn. Metal
concentrations across the entire archive were significantly lower
than the EU guidelines. The nutrient and other physicochemical
characterization of this study would serve as a national and inter-
national reference database for future investigation on the
valorisation process of dairy processing sludge. For agricultural re-
use as bio-based alternative fertiliser this archive will play a vital
role to assess agronomic benefit and facilitating nutrient recycling
opportunity. Such an archive should be expanded longer term
across global dairy processing plant networks to inform pre and
post sludge generation management.
Acknowledgement
This work has received funding from Enterprise Ireland and the
Dairy Industry Partners in Ireland under Dairy Processing Tech-
nology Centre (DPTC) programme. Grant Agreement Number
TC2014 0016. We would like to thank DPTC associated dairy in-
dustry partners - Kerry Group, Arrabawn Co-op, Carbery Foods,
Tipperary Co-op, Lakeland Dairies, Dairygold, Glanbia and Aurivo
for supplying seasonal sludge samples.
Appendix A. Supplementary data
Supplementary data to this article can be found online at
https://doi.org/10.1016/j.jclepro.2019.05.025.
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