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Journal of Environmental Management 248 (2019) 109283

Contents lists available at ScienceDirect

Journal of Environmental Management


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

Research article

Potentiality of sewage sludge-based organo-mineral fertilizer production in T


Poland considering nutrient value, heavy metal content and phytotoxicity
for rapeseed crops
Halyna Kominko*, Katarzyna Gorazda, Zbigniew Wzorek
Cracow University of Technology, Warszawska 24, Cracow 31-155, Poland

A R T I C LE I N FO A B S T R A C T

Keywords: Sewage sludge is a valuable source of nutrients and organic matter, which are beneficial for plant growth. The
Sewage sludge use of sewage sludge for agricultural purposes can be limited by the potential content of heavy metals and toxic
Organo-mineral fertilizers organic compounds that pose a threat to the environment. The characterisation of sewage sludges from 11 Polish
Nutrient recycling wastewater treatment plants (WWTPs) in terms of their fertilizing properties and heavy metal contents are
Secondary raw materials
presented in the study. Based on the chemical composition of sewage sludge from the WWTP in Żywiec, the
compositions of organo-mineral fertilizers dedicated for rapeseed crop was developed. Alternative raw materials
such as poultry litter ash and biomass ash were considered as components for fertilizer production. The pro-
duction process of organo-mineral fertilizers included mixing sewage sludge with poultry litter ash/biomass ash
and mineral fertilizers and granulation with mineral acids. The final products contained 24–34% of total NPK
and fulfilled the requirements regarding heavy metal content according to Polish legislation. Using sewage
sludge for fertilizer production is a promising solution for sewage sludge management, allowing the recycling of
82–140 tonnes of phosphorus (as P2O5) and 42–73 tonnes of nitrogen (N) annually in the WWTP in Żywiec.

1. Introduction (Angın and Yaganoglu, 2011) and enzymatic function (Siebielec et al.,
2018). Agricultural use of sewage sludge is framed by the Sludge Di-
Sewage sludge management is one of the most controversial issues rective (European Commission, 1986), which determines permissible
of modern wastewater treatment. Sewage sludge is rich in macro- concentrations of heavy metals in sewage sludge intended for soil ap-
nutrients and, more importantly, organic matter, and it can be suc- plications to prevent environmental pollution and to ensure safety for
cessfully used to improve soil fertility (Roig et al., 2012; Urbaniak et al., human health. Some member states (Austria, the Czech Republic, Fin-
2017) and to increase crop production (Latare et al., 2014; Sharma land, Netherlands, Slovenia, and Sweden) have established more
et al., 2017). However, there is public concern caused by the possible stringent limits for heavy metal content than those in the Directive.
presence of pathogenic microorganisms (Bibby and Peccia, 2013; Ye There is no uniform approach to monitoring organic pollutants in
and Zhang, 2011), toxic organic compounds (Aparicio et al., 2009; sewage sludge. Austria, the Czech Republic, Germany, Denmark, and
Clarke and Smith, 2011; Suciu et al., 2015), and heavy metals (Duan Sweden have also adopted maximum values for organic contaminants
et al., 2015; Hei et al., 2016; Tiruneh et al., 2014) in sewage sludge. (polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls
Therefore, dealing appropriately with sewage sludge in economically (PCBs), dioxins (PCDDs), di(2-ethylhexyl)phthalates (DEHPs), alkyl-
justified and environmentally acceptable ways is a matter of increasing benzene sulphonates (LASs), nonylphenol and nonylphenol ethoxylates
importance (Ren et al., 2017). (NPEs), etc.) in sewage sludge for agricultural use, while the UK, Ca-
Application of sewage sludge to soil has been practised worldwide nada, and the USA believe that there is no need to control organic
and much research has stated the positive influence of sewage sludge on pollutants because their concentrations are not high enough to pose
soil and crop production, including increasing the nutrient and organic threats to human health (Mininni et al., 2015). Attention is also paid to
matter content of soil (Suhadolc et al., 2010; Wang et al., 2008), im- pathogenic microorganisms in the legislations of Denmark, Finland,
proving soil structure and porosity, increasing cation exchange capacity Poland, and Luxemburg (Latare et al., 2014).

*
Corresponding author.
E-mail addresses: halynakominko@chemia.pk.edu.pl, halynakominko@chemia.pk.edu.pl (H. Kominko), gorazda@chemia.pk.edu.pl (K. Gorazda),
wzor@chemia.pk.edu.pl (Z. Wzorek).

https://doi.org/10.1016/j.jenvman.2019.109283
Received 25 February 2019; Received in revised form 14 July 2019; Accepted 15 July 2019
0301-4797/ © 2019 Elsevier Ltd. All rights reserved.
H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Sewage sludge use for agricultural purposes is important in the case (Werle, 2015). In the case of agricultural use of sewage sludge, a slight
of phosphorus recycling, which is known to be limited (Cordell et al., decrease is observed, which can be attributed to the growth in public
2009; Gorazda et al., 2017; van Dijk et al., 2016). Due to the scarcity of awareness of environmental issues and no social acceptance of this
phosphate rock and, consequently, the fluctuation in its price in recent disposal method (Smol et al., 2016). Moreover, some authors have
years (Mew, 2016), alternative sources of phosphorus, such as sewage highlighted that sewage sludge use in agriculture is seasonal and there
sludge, will gain increasing interest (Vogel et al., 2016). Furthermore, is no area in Poland for this purpose (Bauman-Kaszubska and Sikorski,
Europe has scant deposits of phosphate rock, primary in Finland, and 2011; Wolski et al., 2011).
depends strongly on its import (Reijnders, 2014). At the same time, A serious problem for sewage sludge management in Poland is
there is loss of phosphorus to the environment caused by the in- sewage sludge accumulation at WWTPs, which in 2016 accounted for
appropriate use of mineral fertilizers, which results in eutrophication 221.2 thousand tonnes of sewage sludge expressed as dry solids. After
and dead zones due to a lack of oxygen (Scholz et al., 2013). For this January 1, 2016, the landfilling of sewage sludge that has not been
reason, improvement in phosphorus management is of high priority. It processed properly is forbidden (Journal of Laws from 2015a, item
is estimated that approximately 60% of the phosphorus that goes to 1277). In the 2016 National Waste Management Plan (Polish Official
wastewater treatment plants is incorporated into sewage sludge. In a Journal, 2016), there is no strategy for the utilisation of sewage sludge
typical municipal WWTP with biological phosphorus removal and/or that was landfilled and accumulated at the WWTPs before. The ne-
precipitation, nearly 11% of phosphorus ends in primary sludge, and cessity to deal with sewage sludge according to waste hierarchy, which
28% and 50% in surplus sludge and sewage sludge after enhanced includes reducing sewage sludge production (use of effective stabilisa-
biological phosphorus removal and precipitation respectively (Cornel tion and dewatering processes), organic recycling (use for compost,
and Schaum, 2009). According to Yuan et al. (2012), phosphorus re- phosphorus recovery) and energy recovery is emphasised.
cycled from domestic waste streams satisfies 15–20% of the world de- Additionally, within the framework of the Water Directive (2000/
mand for phosphate rock and reduces, to some degree, dependence on 60/EC) and adopted policy of sustainable development, Poland has
mineral fertilizers. adopted a ‘Program of actions aimed at reducing water pollution with
However, sewage sludge disposal in agriculture can lead to an ac- nitrates from agricultural sources and prevention of further pollution’
cumulation of heavy metals and organic contaminations in soil as a (Journal of Laws from 2018, item 1339). The Program introduces
result of its long-term application (Bettiol and Ghini, 2011; Kirchmann changes in the field of nitrogen fertilisation, determines the permitted
et al., 2017; Yang et al., 2018). According to this, thermal treatment of date of use and dose of fertilizers that contain nitrogen, defines the
sewage sludge has become increasingly popular in some European storage conditions for organic fertilizers, and establishes rules for fer-
countries (Turunen et al., 2018). tilizer use at or near surface waters and areas with a large slope. The
Among the advantages of sewage sludge thermal utilisation, a sig- Program can affect sewage sludge management due to the fact that
nificant decrease in initial mass, decomposition of harmful compounds, sewage sludge is considered an organic fertilizer containing nitrogen
energy recovery (Pajak, 2013; Samolada and Zabaniotou, 2014), and a and can cause water pollution due to nitrogen compounds as a result of
final form of mineral ash that is beneficial for phosphorus recovery its application to soil.
(Atienza-Martínez et al., 2014; Donatello and Cheeseman, 2013) or as Intensive research and innovations in recent years have resulted in
an additive for construction materials (Smol et al., 2015), should be the creation of a wide spectrum of technologies for phosphorus re-
mentioned. Nevertheless, incineration leads to concentrations of heavy covery from sewage sludge (Withers et al., 2015). Most are based on
metals in ash that should be used in an appropriate way (Ottosen et al., precipitation/crystallisation processes from secondary treated effluent
2013) and it does not take into consideration the nutrient and fertilizing or aqueous phases resulting in struvite or different forms of calcium
potential of sewage sludge. In addition, thermal methods of sewage phosphate formation (Desmidt et al., 2015). Another possibility of
sludge disposal are not in line with waste hierarchy and circular phosphorus recovery is the wet-chemical or thermal treatment of
economy policy (Gharfalkar et al., 2015). It should also be pointed out sewage sludge and sewage sludge ash. The final product can be phos-
that incineration is energy intensive and a high-cost process, profitable phoric acid, white phosphorus, or a substitute for phosphate rocks in
only for large WWTPs (Świerczek et al., 2018). fertilizer production (Egle et al., 2015). However, such an approach
It is known that the quality of sewage sludge is dependent on the does not allow for the use of the organic matter contained in sewage
treatment technology, as well as on the share of industrial waste in the sludge. Additionally, the cost of phosphorus recovered from wastewater
total wastewater effluent (Eid et al., 2017). This parameter will be streams is generally higher than the market price of phosphate ore or
decisive in choosing the final sewage sludge disposal pathway. Methods fertilizers. Phosphorus recovery from the liquid phase and from sewage
for sewage sludge utilisation should be developed separately for each sludge through wet-chemical process costs USD6.72–11.2/kg phos-
WWTP to avoid detrimental environmental effects and the accumula- phorus and USD10.07–17.91/kg phosphorus, respectively (Ye et al.,
tion of contaminants in line with sustainable development (Cieślik 2017), and from triple superphosphate and phosphate ore the costs are
et al., 2015; Kacprzak et al., 2017). USD1.34–2.46/kg phosphorus and USD0.67–1.34/kg phosphorus
The production of municipal sludge in Poland in 2016 was 568.3 (Zhang et al., 2017). But when taking into account environmental
thousand tonnes of dry solids (d.s.), and the amount of sewage sludge benefits and profits from the fertilizers produced, these technologies
has increased 17% compared with 2005 (Central Statistical Office, can be economically viable (Mayer et al., 2016).
2017). The increasing production of sewage sludge is connected with This paper examines the nutrient and organic matter recycling in
modernisation of existing wastewater treatment plans to adopt new form of fertilizers based on sewage sludge. In this work, dried sewage
high-efficiency technologies, the expansion of the sewerage network, sludge from Polish WWTPs were analysed in terms of their fertilizing
and the construction of new wastewater treatment plants (Bień et al., properties and heavy metal content. The compositions of sewage
2011). The most popular method of sewage sludge disposal in 2016 was sludge-based fertilizers for rapeseed crop were developed and com-
agricultural use (20%); nearly 4% of sewage sludge was applied in land pared with mineral, organic and sewage sludge-based fertilizers avail-
reclamation, 6% in the cultivation of plants intended for compost able on the Polish market. The content of heavy metals obtained, in
production, 18% was thermally transformed, and 4% was landfilled particular that of Cd, was discussed.
(Central Statistical Office, 2017). It should be noted that the amount of
landfilled sewage sludge has decreased significantly (31% in 2005). The
reverse situation has occurred in the case of thermal methods of sewage
sludge treatment (1% in 2005 and 18% in 2016). Recent years have
brought dynamic growth in thermal methods for sewage sludge disposal

2
H. Kominko, et al.

Table 1
Characterisation of polish WWTPs.
Wastewater Treatment Location Population Municipal Industrial Sewage sludge treatment Sewage sludge Final disposal method
Plant equivalent (PE) sewage,% sewage,% methods amount,t ds/year

Nowy Targ N 49°28′51.875” 110 778 53.5 46.5 Thickening, dewatering on 1620 R3 Recycling/reclamation of organic substances which are not used as solvents
E 20°2′43.67” centrifuges, anaerobic (including composting and other biological transformation processes)
digestion, drying R12 Exchange of waste for submission to any of the operations numbered R 1 to R
11
Szczecin-Zdroje N 53°22′48.746” 114 852 72.9 27.1 Mesophilic anaerobic digestion, 1083 D10 Incineration on land (635 t ds/year)
E 14°37′11.702” dewatering, drying Using for growing plants intended for the production of compost (448 t ds/year)
Szczecin-Pomorzany N 53°25′0.12” 375 701 81.9 18.1 Mesophilic anaerobic digestion, 4226 R10 Land treatment resulting in benefit to agriculture or ecological improvement
E 14°34′59.879” dewatering, drying (181 t ds/year)
D10 Incineration on land (4045 t ds/year)
Gdynia - Dębogórze N 54°29′47.811” 431 461 91.1 8.9 Mesophilic anaerobic digestion, 7337 D10 Incineration on land
E 18°30′38.53” dewatering, drying, fluidal Using for growing plants intended for the production of compost
combustion
Częstochowa N 50°49′5.586” 256 624 87.8 12.2 Thickening, dewatering, 2966 D10 Incineration on land (2726 t ds/year)
E 19°9′49.707” anaerobic digestion, R3 + R5 Recycling/reclamation of organic substances which are not used as
dewatering, thermal drying solvents (including composting and other biological transformation

3
processes) + Recycling/reclamation of other inorganic materials (240 t ds/year)
Ruda Śląska- N 50°19′5.443” 36 577 95.5 4.5 Anaerobic digestion, 866 D10 Incineration on land
Orzegów E 18°53′14.254” dewatering, drying R3 Recycling/reclamation of organic substances which are not used as solvents
(including composting and other biological transformation processes)
Myszków N 50°34′50.53” 25 392 69.5 31.5 Aerobic simultaneous 882 R3 Recycling/reclamation of organic substances which are not used as solvents
E 19°18′7.029” stabilisation, dewatering, solar (including composting and other biological transformation processes)
drying
Rzeszów N 50°2′7.508” 222 881 94.3 5.7 Mesophilic anaerobic digestion, 4083 Temporary storage on the WWTP site (108 t ds/year)
E 22°0′38.655” dewatering, liming, drying Using for growing plants not intended for consumption and for the production of
feed (3094 t ds/year)
R3 Recycling/reclamation of organic substances which are not used as solvents
(including composting and other biological transformation processes) (881.3 t ds/
year)
Skarżysko-Kamienna N 51°6′17.425” 59 500 93.2 6.8 Anaerobic digestion, 554 Sedimentary lagoons, hydrophilic use of sludge (554 t ds/year)
E 20°51′21.364” dewatering, solar drying
(currently do not use)
Żywiec N 49°41′41.294” 193 927 51.6 48.4 Mesophilic anaerobic digestion, 1693 D10 Incineration on land (1539 t ds/year)
E 19°11′41.271” dewatering, drying Using for growing plants intended for the production of compost (155 t ds/year)
Kędzierzyn-Koźle N 50°21′0” 72 057 85.4 14.6 Anaerobic digestion, 1440 Using in agriculture (1319 t ds/year)
E 18°11′59.999” dewatering, drying D10 Incineration on land (50 t ds/year)
Temporary storage on the WWTP site (71 t ds/year)
Journal of Environmental Management 248 (2019) 109283
H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

2. Materials and methods producing more than 2 million tonnes of rape annually, which is 9% of
European rape production (Rosiak, 2014).
2.1. Materials used in the experiment The fertilizer production process was carried out in a laboratory disk
granulator. First attempts were aimed at selection of the amount of each
Dried sewage sludge was collected from 11 Polish WWTPs (in Nowy component and development of granulation parameters. Sewage sludge
Targ, Ruda Śląska, Częstochowa, Szczecin (2), Żywiec, Gdynia, was milled, mixed with poultry litter ash/biomass ash and mineral
Myszków, Skarżysko-Kamienna, Rzeszów, and Kędzierzyn-Koźle). The fertilizers, and loaded into the granulation disk. Dilute nitric/sulfuric
information about WWTPs, including population equivalent, waste- acids were added in portions to the granulator. The process was com-
water origin, sewage sludge treatment processes and final disposal pleted when whole mixture was granulated. The obtained granules
method of sewage sludge is presented in Table 1. All sewage sludge were dried at 70 ○C for 3 h.
underwent mechanical and biological treatment, then anaerobic di- In order to check the technology and the repeatability of results the
gestion and drying. WWTPs in Myszków, Rzeszów, and Skarżysko-Ka- process of fertilizer production was performed on a semi-technical
mienna have a solar dryer, whereas others are equipped with thermal scale. The disc granulator used in fertilizer production was equipped
dryers. with a liquid feeder and granule classifier. The granulation parameters
Dried sewage sludge were stored in covered storage site for 3–8 were follows: 1) diameter of granulation disk, 80 cm; 2) inclination
months depending on WWTP, except of sewage sludge from the WWTP angle, 35°; and 3) rotation, 60 rpm. The fertilizer production process
in Gdynia, where it is incinerated. The period of sample collection was was carried out as on the laboratory scale.
March-October 2013. The samples of dried sewage sludge were col-
lected representatively from sewage sludge storage. 2.3. Analytical procedures
Sewage sludge was used as a basis for production of organo-mineral
fertilizers. The low content of nutrients in sewage sludge in comparison The moisture content of analysed materials was determined by
with mineral fertilizers is one of the biggest drawbacks, which makes drying at 105 °C using a Mettler Toledo moisture analyser HG63. The
the effect of sewage sludge application visible after the use of large organic matter content of sewage sludge was determined by calcination
doses (Amann et al., 2018). Due to this fact, we considered the addition at 550 °C for 3 h according to the (Journal of Laws ,b, item 257).
of alternative sources of phosphorus and potassium in the form of The chemical composition of sewage sludge samples, poultry litter
poultry litter ash and biomass ash and mineral fertilizers in order to ash and biomass ash were determined by the use of atomic absorption
increase the nutrient content of organo-mineral fertilizers. spectroscopy (AAS) (AAnalyst 300, PerkinElmer) and inductively cou-
Poultry production is one of the biggest branches of the agri-food pled plasma optical emission spectrometry (ICP-OES) (Plasm 40,
industry, generating a significant amount of waste, which creates pro- PerkinElmer) after digestion in H2SO4 and aqua regia in the case of Ca
blems with its management. The alternative practice for poultry litter and Pb determination (Polish Committee of the Standardization, 2002;
disposal is incineration (Mierzwa-Hersztek et al., 2016). Poultry litter modified PN-91/, 1991). The fertilizer digestion was conducted in aqua
ash is a valuable source of phosphorus (9.1–15.3% P2O5) and potassium regia and the solutions analysed with the above-mentioned techniques.
(7.9–16.9% K2O) (Bauer et al., 2019; Billen et al., 2015) and be suc- The total phosphorus content, as well as its bioavailability, was de-
cessfully used as raw material in fertilizer production. The poultry litter termined using a spectrophotometric method according to EU (2003)
ash used in the experiment originated from an industrial incinerator and PN-88/C-, 87015. The determination of nitrogen content was per-
plant. Poultry litter was incinerated in a rotary kiln at 650–850 °C. formed using a 2400 CHN Elemental Analyser (PerkinElmer).
Biomass combustion is applied worldwide in bioenergy. Despite the All analysis was carried out twice for each sample. The results of
value of nutrients in biomass ash, landfilling still plays a key role in its analyses (including tables and figures) are given in % or mg/kg of dry
management, generating significant costs. The composition of biomass mass.
ash depends strongly on biomass type. For example, wood ash contains To examine the effects of sewage sludge-based fertilizers on the
2.3–13.4% P2O5 and 7.2–26.5% K2O (Insam and Knapp, 2011). Field early phase of rape germination, the Phytotoxkit test was used. The
studies have shown beneficial effects of biomass ash use for agriculture tests were performed in transparent polystyrene test plates filled with
purposes. However, because of the high alkalinity of ash (pH ≈ 12), reference soil, and reference soil mixed with 0.2 g of selected fertilizer.
direct application to the soil is not recommended (Brännvall et al., The rape seeds were incubated for 72 h at 25 °C and with no light ac-
2015). Therefore, ash can be recycled as a component of fertilizers in cess. The test was performed in triplicate.
line with a ‘zero-waste’ objective. Biomass ash for fertilizer production
in the experiment was prepared in the laboratory. Flax straw was in- 3. Results and discussion
cinerated in a muffle furnace for 3 h at 650 °C.
3.1. Material characteristics
2.2. Organo-mineral fertilizer production
3.1.1. Sewage sludge
Based on chemical characterisation of analysed sewage sludge The moisture content of analysed sewage sludge ranged from 4.79%
(especially heavy metal and nutrient content) sewage sludge from the in the case of sewage sludge from the WWTP in Częstochowa to 51.6%
WWTP in Żywiec was selected for organo-mineral fertilizer production. in that from the WWTP in Gdynia. The analysed sewage sludge con-
In spite of research, results of which showed the positive impact of sisted of 54.38–78.42% organic matter. The results of the study are
sewage sludge application on the growth of tomatoes (Waqas et al., presented in Table 2 and show significant differences in sewage sludge
2015), spinach (Kumar et al., 2016), barley (Pasqualone et al., 2017), composition. The phosphorus content (P2O5) of sewage sludge varied
corn (Grotto et al., 2015), and wheat (Koutroubas et al., 2014), sewage from 3.51% in the case of sewage sludge from the WWTP in Nowy Targ
sludge application to soil intended for crops to be consumed by humans to 8.96% in that from the WWTP in Gdynia. The nitrogen content ac-
or animals is prohibited (Journal of Laws, 2015b, item 257). For this counted for 4.01–6.80%. Typically, sewage sludge is poor in potassium
reason, we propose the compositions of organo-mineral fertilizers based (Grobelak et al., 2019), which was confirmed in this study. Sewage
on sewage sludge for rape crop. Rapeseed oil is used as a biocomponent sludge is a source of secondary nutrients and micro-nutrients, especially
of fuels such as diesel. As a consequence of a European Directive im- Ca, Mg, S, Fe and Mn.
plementation with regards to increasing the share of biocomponents in The considerable amount of nutrients in sewage sludge emphasises
fuels, growth in rape production has been observed (Küüt et al., 2017). the benefits of their agricultural use. Land application of sewage sludge
Poland is one of the biggest producers and exporters of rape in Europe, in Poland is regulated by (Journal of Laws from ,b, item 257). The

4
H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Table 2
Characterisation of sewage sludge from Polish WWTPs (numbers in bold indicate the highest value).
Primary nutrients Secondary nutrients Micronutrients

Moisture Organic N P2O5 K2O MgO CaO Na2O SO3 Fe Mo Mn Co B


content matter
% mg/kg
Nowy Targ 13.3 78.42 6.80 3.51 0.633 0.534 2.39 0.297 1.58 1.28 0.166 200 3.49 21.9
± 0.3 ± 0.04 ± 0.04 ± 0.02 ± 0.032 ± 0.02 ± 0.02 ± 0.015 ± 0.08 ± 0.02 ± 0.006 ± 10 ± 0.17 ± 1.1
Szczecin-Zdroje 8.37 67.09 4.01 7.44 0.240 0.985 6.06 0.118 4.51 2.88 2.26 227 5.65 79.6
± 0.23 ± 0.04 ± 0.12 ± 0.11 ± 0.012 ± 0.01 ± 0.06 ± 0.006 ± 0.23 ± 0.04 ± 0.11 ± 11 ± 0.28 ± 4.0
Szczecin 3.39 62.86 4.41 8.35 0.374 1.27 3.64 0.108 2.03 2.53 1.60 154 4.69 92.9
–Pomorzany ± 0.08 ± 0.18 ± 0.18 ± 0.08 ± 0.019 ± 0.03 ± 0.03 ± 0.005 ± 0.10 ± 0.08 ± 0.08 ±8 ± 0.23 ± 4.6
Gdynia- 51.6 65.04 4.75 8.96 0.323 1.00 2.17 0.143 2.87 1.70 3.33 252 5.35 8.64
Dębogórze ± 0.6 ± 0.04 ± 0.04 ± 0.03 ± 0.016 ± 0.01 ± 0.01 ± 0.007 ± 0.14 ± 0.21 ± 0.17 ± 13 ± 0.27 ± 0.43
Częstochowa 4.79 60.31 6.54 8.21 0.209 0.852 4.38 0.134 3.31 5.89 4.37 469 15.4 5.27
± 0.04 ± 0.10 ± 0.08 ± 0.18 ± 0.010 ± 0.01 ± 0.05 ± 0.007 ± 0.17 ± 0.21 ± 0.22 ± 23 ± 0.8 ± 0.26
Ruda Śląska- 20.8 72.05 6.23 7.67 1.13 0.885 1.65 0.207 1.73 2.58 0.957 559 20.7 9.15
Orzegów ± 0.1 ± 0.10 ± 0.04 ± 0.02 ± 0.06 ± 0.01 ± 0.01 ± 0.010 ± 0.09 ± 0.01 ± 0.048 ± 28 ± 1.0 ± 0.46
Myszków 7.75 75.77 6.54 5.35 1.07 1.24 1.69 0.139 0.0320 1.27 10.4 475 25.2 32.5
± 0.54 ± 0.18 ± 0.03 ± 0.10 ± 0.05 ± 0.02 ± 0.01 ± 0.007 ± 0.0016 ± 0.01 ± 0.5 ± 24 ± 1.3 ± 1.6
Rzeszów 11.2 56.87 4.57 7.23 1.02 1.50 3.78 0.242 2.82 1.23 2.36 242 16.3 2.66
± 0.1 ± 0.49 ± 0.04 ± 0.10 ± 0.05 ± 0.01 ± 0.02 ± 0.012 ± 0.14 ± 0.01 ± 0.12 ± 12 ± 0.8 ± 0.13
Skarżysko- 13.1 54.38 4.07 6.80 0.436 1.19 5.67 0.173 3.32 1.41 2.71 371 5.99 6.48
Kamienna ± 0.3 ± 0.10 ± 0.03 ± 0.05 ± 0.022 ± 0.01 ± 0.07 ± 0.009 ± 0.17 ± 0.31 ± 0.14 ± 19 ± 0.30 ± 0.32
Żywiec 6.51 55.42 4.44 7.24 0.345 0.651 3.19 0.154 2.45 6.99 12.6 535 29.7 18.43
± 0.10 ± 0.04 ± 0.04 ± 0.25 ± 0.017 ± 0.04 ± 0.02 ± 0.008 ± 0.12 ± 0.68 ± 0.6 ± 27 ± 1.5 ± 0.92
Kędzierzyn- 6.49 67.74 4.52 5.67 0.219 1.10 6.12 0.161 4.97 2.02 2.59 754 9.67 9.94
Koźle ± 0.13 ± 0.23 ± 0.05 ± 0.06 ± 0.011 ± 0.01 ± 0.04 ± 0.008 ± 0.25 ± 0.05 ± 0.13 ± 38 ± 0.48 ± 0.50
Mineral 3.5-31 10–20 10–28 0.1–2.7 4.9–24 1.1–20 0.1–0.2 0.02 0.2–0.7 0.01 0.2–1
fertilizersa

a
– composition of mineral NPK fertilizers available in the Polish market (n = 12).

Table 3
Heavy metal content in sewage sludge from Polish WWTPs.
Zn Cu Pb Cr Ni Cd Hg

mg/kg

Nowy Targ 521.4 38.61 12.14 139.1 23.05 7.85 0.083


± 25.7 ± 2.01 ± 0.10 ± 3.4 ± 1.03 ± 0.01 ± 0.004
Szczecin-Zdroje 1244 499.2 41.38 40.91 31.30 13.0 0.10
± 75 ± 5.9 ± 0.87 ± 2.00 ± 1.63 ± 0.4 ± 0.01
Szczecin –Pomorzany 906.8 190.8 33.78 32.35 37.82 14.7 0.11
± 58.3 ± 10.5 ± 0.59 ± 1.33 ± 1.45 ± 0.7 ± 0.01
Gdynia-Dębogórze 1116 223.8 41.95 45.68 41.00 13.1 3.1
± 42 ± 1.3 ± 1.32 ± 2.69 ± 1.78 ± 0.8 ± 0.2
Częstochowa 2110 271.0 96.8 302.5 136.2 15.6 1.1
± 56 ± 4.1 ± 1.5 ± 3.2 ± 0.7 ± 1.2 ± 0.1
Ruda Śląska- Orzegów 1153 66.60 64.49 53.89 41.84 14.9 7.2
± 54 ± 1.48 ± 0.12 ± 1.51 ± 1.96 ± 0.1 ± 0.4
Myszków 2157 37.24 168.0 58.33 39.28 13.7 0.46
± 53 ± 2.83 ± 0.4 ± 0.60 ± 2.59 ± 1.1 ± 0.02
Rzeszów 1119 200.9 44.34 90.97 63.66 14.4 7.2
± 60 ± 0.6 ± 1.20 ± 3.10 ± 1.33 ± 0.7 ± 0.4
Skarżysko-Kamienna 4504 325.8 97.53 246.8 65.57 11.6 2.6
± 24 ± 1.5 ± 2.78 ± 16.1 ± 2.54 ± 0.2 ± 0.1
Żywiec 936.4 193.3 29.84 66.05 90.10 1.88 2.3
± 12.8 ± 13.7 ± 0.12 ± 0.39 ± 2.15 ± 0.03 ± 0.1
Kędzierzyn-Koźle 3804 197.1 60.40 85.91 79.53 7.6 0.64
± 123 ± 6.08 ± 5.36 ± 2.04 ± 12.81 ± 1.0 ± 0.03
Permissible values for sewage sludge land application 1* 2500 1000 750 500 300 20 16
2* 3500 1200 1000 1000 400 25 20
3* 5000 2000 1500 2500 500 50 25
Permissible values for organic fertilizers 140 100 60 5 2

1* use of sewage sludge in agriculture or for land reclamation for agricultural purposes.
2* use of sewage sludge for land reclamation for non-agricultural purposes.
3* use of sewage sludge while adapting the land to specific needs resulting from waste management plans, spatial development plans or decisions on building and
land development conditions, for growing crops intended for the production of compost, or for growing plants not designated for consumption and feed production.

Directive sets permissible values for heavy metal content (Zn, Cu, Pb, set by the Directive except that from the WWTP in Kędzierzyn-Koźle, in
Ni, Cr, Cd and Hg) depending on the proposed sewage sludge use. The which the concentration of Zn was found to be higher (4504 mg/kg)
results of the study presented in Table 3 show that the heavy metal than the permissible value for sewage sludge intended for agricultural
content in the analysed sewage sludge did not exceed the limit values use (2500 mg/kg) and for reclamation (3500 mg/kg).

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Due to the fact that sewage sludge can be considered an organic metal load can be introduced to WWTPS from unidentified and dis-
fertilizer (Bai et al., 2017), the composition of sewage sludge was persed sources (European Commission, 2001). Therefore, there is a
compared with regulatory parameters set up by Polish Regulations re- need for deeper studies of dispersed heavy metal sources and analysis of
lating to organic fertilizers (Journal of Laws from 2008, No. 119, item the possible management of these sources in order to reduce con-
765). According to the Ordinance, organic fertilizers should contain no tamination load to wastewater.
less than 30% organic matter and, in the case of the declared content of In order to reduce the heavy metal content in sewage sludge, im-
N, P, or K or their sum, the content of each nutrient cannot be less than mobilisation techniques or removal technologies can be used. Heavy
the following: a) 0.3 mass/mass percent (% m/m) of total nitrogen, b) metal immobilisation can be achieved by mixing sewage sludge with
0.2% m/m of total phosphorus (expressed as P2O5), and c) 0.2% m/m of various substrates from the group of alkaline materials (lime, ash, hy-
total potassium (expressed as K2O). In addition, organic fertilizers droxyapatite), or clays (bentonite and limonite) or organic materials
should fulfil the requirements for heavy metal content (Cr, Pb, Cd, Ni (activated carbon, compost). This allows significant reduction in the
and Hg), which is important from an environmental point of view. mobility of heavy metals in sewage sludge and therefore decreases their
Sewage sludge from Polish WWTPs analysed in the study met the accumulation in soil after sewage sludge application (Penido et al.,
requirements in terms of organic matter and nutrient content. However, 2019; Tsadilas et al., 2014).
all sewage sludge contained at least one metal whose concentration Various technologies have been developed in recent years for re-
exceeded the limit value according to legislation (Table 3). moving heavy metals from sewage sludge. Chemical extraction by using
The content of Cr in sewage sludge varied from 32.4 to 303 mg/kg. mineral/organic acids or chelating reagents is the most commonly used
Eight sewage sludge samples had Cr concentrations below the max- method for the removal of heavy metals from sewage sludge with good
imum value (100 mg/kg), while sewage sludge from WWTPs in Nowy recovery rate (average 80–90%) (Suanon et al., 2016). However, it
Targ, Częstochowa, and Skarżysko-Kamienna were characterised by a requires high dosages of extraction agents, which lead to high operating
higher content of Cr than that allowed by the Ordinance. In the case of costs and operational difficulties (Deng et al., 2009). In addition, some
Pb, all samples, except that from the WWTP in Myszków, fulfilled the chelating reagents can pose secondary pollution problems through
requirement (140 mg/kg). The Ni content of sewage sludge from heavy metal leaching (Wu et al., 2015). Therefore, heavy metal removal
WWTPs in Nowy Targ, Szczecin-Zdroje, Szczecin-Pomorzany, Ruda by bioleaching has attracted increasing attention due to the low costs of
Śląska, Gdynia and Myszków was below 60 mg/kg. Other samples the method (80% cheaper than chemical extraction) (Gu et al., 2016),
contained higher concentrations of Ni than the maximum permitted the possibility of metal recovery from the leachate and improved de-
value. In the case of sewage sludge from the WWTP in Częstochowa, the watering properties of sewage sludge (Marchenko et al., 2018). The
concentration of Ni exceeded 127% of drawback of this removal method is the slow reaction kinetics. The
The concentration of Cd was found to be high in all analysed ma- recovery efficiency varies depending on the metal and can reach
terials, except in sewage sludge from the WWTP in Żywiec, whereas 34–100% Cu, 18–80% Cr, 18–69% Cd, 10–58% Pb, 58–99% Mn,
other samples contained 2–3 times higher concentrations of Cd than the 42–100% Ni, and 38–100% Zn (Gu et al., 2018). A better understanding
permissible value. The content of Hg was much higher than the max- of reactions taking place in biofilm as well as optimisation of process
imum concentration (2 mg/kg) in sewage sludge from WWTPs in parameters (pH, temperature, reaction time, mass transfer rate, etc.) are
Rzeszów (7.20 mg/kg), Ruda Śląska (7.15 mg/kg), and Gdynia needed to adapt bioleaching technology to heavy metal removal from
(3.07 mg/kg). Sewage sludge from WWTPs in Nowy Targ, Szczecin- sewage sludge on an industrial scale. Electrokinetic remediation, which
Zdroje, Szczecin-Pomorzany, Myszków, Częstochowa and Kędzierzyn- is based on transport of metal ions towards electrodes under an electric
Koźle fulfilled the requirement regarding Hg content in organic ferti- field is considered a promising technique for heavy metal removal from
lizers. The primary source of heavy metals in sewage sludge is industrial sewage sludge (Fu et al., 2017). This technology does not introduce
sewage, mainly from electroplating, the chemical industry, and the additional substrates into the system; however, the process requires a
metal processing industry (Fernandes et al., 2007). However, no strong great deal of energy (Shen et al., 2007). Emerging technologies for
correlation was observed between the share of industrial effluent in heavy metal removal from sewage sludge, such as supercritical water
wastewater and heavy metal content of sewage sludge analysed in the treatment (Qian et al., 2016), application of chitosan magnetite nano-
study. In WWTPs in Nowy Targ and Żywiec the share of industrial ef- particles (Bratina et al., 2016), and photocatalysis (Kabra et al., 2008)
fluent was the highest, at 46.5% and 48.4%, respectively. The ex- have been intensively studied.
ceeding of limit values of heavy metal content in sewage sludge from All the above-mentioned technologies give satisfactory results and
these WWTPs was not significant. An interesting finding is that sewage can be implemented in WWTPs. However, there are still some bottle-
sludge from WWTPs in Skarżysko-Kamienna, Częstochowa and necks, such as cost-effectiveness, simplicity and technical feasibility,
Rzeszów, where the share of industrial effluent was the lowest (6.8%, which should be improved to increase the attractiveness and accessi-
12.2%, 5.7%, respectively), contained three or four metals with con- bility of the technologies.
centrations above the permissible values for organic fertilizers. These A promising solution for sewage sludge management is its use as a
heavy metals can originate from runoff, corrosion processes and component in organo-mineral fertilizer production, which allows for
households, which are significant sources of heavy metals in sewage. nutrients and organic matter recycling. It should be highlighted that it
The study conducted by (Sörme and Lagerkvist, 2002) showed that the is not possible to prepare fertilizers from sewage sludge only, due to
large sources of Cu in the WWTP in Stockholm were tap water and problems with heavy metal content. The amount of sewage sludge in a
roofs. The large contributors of Zn in wastewater effluent were re- fertilizer composition should be selected based on the heavy metal
sidences (food, pipes, taps), galvanised goods and car washing, in the content of the sewage sludge. Special attention should be paid to Cd
case of Ni it was chemicals added to WWTPs and in the case of Hg it was content, due to its toxicity (Roberts, 2014). Such an approach provides
amalgams. It was concluded that sources of Cr, Cd and Pb were more a decrease in heavy metal content in the final product as a result of
poorly understood and difficult to track. The main sources of these dilution. Additionally, such fertilizers would have higher nutrient
metals were car washing and artists’ paint in the case of Cd. content in comparison to sewage sludge, which is associated with lower
Identification and quantification of key sources of heavy metals in doses.
effluents and their control are crucial for reducing heavy metal content
in sewage sludge and reducing contamination releases to the environ- 3.1.2. Alternative raw materials
ment through agricultural application. However, it should be noted that The characterisation of alternative raw materials is presented in
regulatory actions aimed at controlling heavy metal discharge can focus Table 4. The results of the study showed that poultry litter ash and
only on identified sources. It was reported that up to 30–60% of heavy biomass ash are rich sources of phosphorus and potassium. Their use as

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Table 4
Composition of alternative sources of P and K in organo-mineral fertilizers.
Poultry litter ash Biomass ash

P2O5 % 18.8 ± 0.3 12.1 ± 0.2


K2O 24.7 ± 0.8 19.9 ± 0.9
Ca 9.68 ± 0.47 2.98 ± 0.44
Mg 6.27 ± 0.03 0.261 ± 0.010
Fe 0.78 ± 0.10 0.33 ± 0.03
Zn mg/kg 2288 ± 29 7182 ± 0.9
Cu 694 ± 2 157 ± 4
Cr 122 ± 3 17.4 ± 0.01
Ni 110 ± 8 34.3 ± 2.5
Pb 19.1 ± 0.4 46.6 ± 1.7
Cd 5.27 ± 0.10 13.7 ± 1.3
Hg 0.24 ± 0.01 0.011 ± 0.001

Table 5
Sample names of organo-mineral fertilizers for rape crop.
Sewage sludge-based fertilizers for rape Sewage sludge-based fertilizers for
crop (R) with poultry litter ash (PA) rape crop (R) with biomass ash (BA)

N/P2O5/K2O = 11.2–13.2/4.0–5.6/13.2–17.6
R-PA1, R-PA2 R-BA1, R-BA2
N/P2O5/K2O = 7.4–9.9/3.0–4.8/9.9–13.2
R-PA3, R-PA4 R-BA3, R-BA4

components in fertilizer production is a sustainable disposal method.


Nevertheless, heavy metal content should be taken into account (see
Table 4).
The study showed, that poultry litter ash has high Zn, Cu, Cr and Ni
contents. Heavy metals in poultry litter originates from feed additives
used to promote animal growth (Sarvi et al., 2017) and depends on the
specifics of diet and farm size (Zhang et al., 2012). After combustion of
poultry litter the heavy metals are concentrated in the ash. Biomass ash
is generally characterised by low heavy metal content (Islam et al.,
2017), which was confirmed in this study. However, a very high con- Fig. 2. NPK composition of organo-mineral fertilizers for rape crop (red lines
centration of Zn was found in analysed biomass ash. In the literature the show the expected nutrient range: A) 11.2–13.2 (N) 4.0–5.6 (P2O5) 13.2–17.6
maximum concentration of Zn reported for some biomass ashes was (K2O); B) 7.4–9.9 (N) 3.0–4.8 (P2O5) 9.9–13.2 (K2O)). (For interpretation of the
16400 mg/kg (Vassilev et al., 2010). references to colour in this figure legend, the reader is referred to the Web
version of this article.)
3.2. Sewage sludge-based fertilizers for rape crop
component (sewage sludge, poultry litter ash, biomass ash, mineral
3.2.1. Composition of fertilizers fertilizers, acids) and the type of mineral fertilizer were selected so as to
According to the International Fertilizer Industry Association rape introduce such amounts of nutrients that would result in products with
uptakes nutrients (N/P2O5/K2O) in ratios of 2.8–3.3/1–1.4/3.3–4.4 the expected NPK contents and, at the same time, meet the require-
(International Fertilizer Industry Association, 1992). Based on this data, ments in terms of heavy metal content for organo-mineral fertilizers.
two types of organo-mineral fertilizers with different nutrient content Produced organo-mineral fertilizers contained 38–42% of sewage
were developed. Four organo-mineral fertilizers, two of which con- sludge. Such an amount allows for a reduction in the amount of heavy
tained poultry litter ash (R-PA1, R-PA2) and two biomass ash (R-BA1, metals in fertilizers and provides enough organic matter concentration
R-BA2) were produced with expected nutrient content (%) N/P2O5/ to comply with Polish requirements related to organo-mineral fertilizers
K2O = 11.2–13.2/4.0–5.6/13.2–17.6, and four fertilizers (two with (Journal of Laws from 2008, No. 119, item 765). The ash content in the
poultry litter ash – R-PA3, R-PA4 and two with biomass ash – R-BA3, R- obtained fertilizers was 9–12%. Different conventional fertilizers
BA4) with expected nutrient content (%) N/P2O5/K2O = 7.4–9.9/ (KNO3, K2SO4, NH4NO3, (NH4)2SO4, and diammonium phosphate
3.0–4.8/9.9–13.2 (Table 5). The appropriate amount of each (DAP)) were used for modification of the nutrient content of organo-

Fig. 1. Images of organo-mineral fertilizers for rape crop.

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Fig. 3. Different forms of phosphorus in sewage sludge-based fertilizers for rape crop.

mineral fertilizers. Images of the obtained organo-mineral fertilizers are value was between 21.9 and 28.7% total phosphorus content.
presented in Fig. 1. A low content of potentially plant-available phosphorus is con-
nected with the chemical state of phosphorus in sewage sludge and
poultry/litter biomass ashes, which are the main sources of phosphorus
3.2.2. Nutrient content
in innovative fertilizers for rape crop. From the literature data, it fol-
The moisture content in sewage sludge-based organo-mineral ferti-
lows that phosphorus in poultry litter ash is in the form of calcium
lizers ranged from 2.3 to 4.4%. The NPK contents of the final products
phosphates and apatite (Brod, 2018; Kaneko et al., 2014). In the case of
are presented in Fig. 2. With respect to nitrogen, all the organo-mineral
biomass ash, phosphorus occurs in apatite and potassium phosphate
fertilizers fulfilled the assumed concentration. In the case of phos-
salts (KNaCa2(PO4)2, KFe2(PO4)2, KFe2(PO4)2) (Bogush et al., 2018),
phorus, only the fertilizer R-BA2 had a 3% higher phosphorus content
which are characterised by low water solubility (Brod et al., 2016).
than expected. The phosphorus content in the other fertilizers was in
Phosphorus in sewage sludge is bonded in organic matter and also
line with expectations. The potassium concentration of the obtained
occurs in inorganic form. The composition of inorganic phosphorus
fertilizing products was close to that expected, except for fertilizer R-
depends on the chemicals used in the wastewater treatment process to
PA3, where that K2O content was 21% higher.
improve sludge dewatering and to enhance phosphorus removal
(Kahiluoto et al., 2015). Aluminium and ferric salts, which are widely
3.2.3. Phosphorus availability used, lead to a decrease in phosphorus availability in sewage sludge
The information of potentially plant-available phosphorus in ferti- (Mayer et al., 2016). However, after application of sewage sludge or
lizers enables assessment of their effectiveness and application rates. sewage sludge-based fertilizers, insoluble phosphorus can be trans-
The study has shown that sewage sludge-based fertilizers are generally formed into available forms as a result of organic matter mineralisation
characterised by low content of water-soluble phosphorus compounds and sorption–desorption processes taking place in the soil (Sapek,
(Fig. 3). In the case of fertilizers with the addition of poultry litter ash, 2014). Due to this, sewage sludge-based fertilizers can be considered
the content of water-soluble phosphorus was in the range of slow-release fertilizers, which reduce the risk of nutrient loss to the
8.03–19.6% total phosphorus content. Fertilizers containing biomass environment and consequently improve fertilizer efficiency.
ash, R-BA1 and R-BA2, had 12.1 and 14.6% water-soluble phosphorus,
respectively. The lowest content of water-soluble phosphorus was found
in R-BA3 and R-BA4 (2.47 and 2.70%, respectively). It can be con- 3.2.4. Heavy metal content
cluded that fertilizers containing poultry litter ash have higher water It is well known that fertilizers are a source of heavy metals in soil,
solubility of phosphorus compounds in comparison with those con- resulting in serious environmental damage. This fact becomes more
taining biomass ash. The higher content of water-soluble phosphorus in important in the case of fertilizers based on secondary raw materials,
fertilizers R-BA1 and R-BA2 can be attributed to the diammonium such as sewage sludge and poultry litter ash/biomass ash. The content
phosphate content in the fertilizers, which is characterised by good of heavy metals in all obtained fertilizing products did not excess per-
water solubility. There were no significant differences in the contents of missible concentrations set up by Polish legislation regarding organo-
ammonium citrate-soluble phosphorus in the obtained fertilizers. The mineral fertilizers (Table 6). Moreover, the Pb and Hg content in

Table 6
Concentrations of heavy metals in sewage sludge-based fertilizers for rape crop.
Cr Pb Ni Cd Hg

mg/kg

Sewage sludge-based fertilizers with poultry litter ash

R-PA1 47.9 ± 0.6 18.9 ± 0.0 56.3 ± 2.3 1.61 ± 0.07 0.377 ± 0.022
R-PA2 46.8 ± 1.2 17.9 ± 0.9 56.1 ± 0.9 1.35 ± 0.08 0.286 ± 0.062
R-PA3 55.6 ± 3.5 18.4 ± 1.5 56.1 ± 0.9 1.95 ± 0.12 0.750 ± 0.049
R-PA4 46.8 ± 0.5 14.8 ± 0.2 53.1 ± 1.1 2.12 ± 0.05 0.646 ± 0.069
Sewage sludge-based fertilizers with biomass ash
R-BA1 38.0 ± 0.8 19.6 ± 0.8 38.5 ± 0.9 2.68 ± 0.23 0.344 ± 0.010
R-BA2 36.1 ± 0.2 21.5 ± 0.4 44.4 ± 0.2 1.79 ± 0.03 0.588 ± 0.015
R-BA3 42.3 ± 0.3 15.2 ± 1.5 41.4 ± 0.1 3.34 ± 0.28 0.491 ± 0.025
R-BA4 49.4 ± 0.4 18.7 ± 0.4 45.0 ± 0.5 1.73 ± 0.03 0.578 ± 0.004
Organo-mineral fertilizer standards 100 140 60 5 2

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

sewage sludge-based fertilizers was relatively low, at 84–89% and


63–86%, respectively, lower than maximum permitted values. There
were no significant differences in heavy metal concentration between
fertilizers with the addition of poultry litter ash and those with biomass
ash addition, except for Ni, which was slightly higher in R-PA1–R-PA4
fertilizers.
The issue of heavy metal content in fertilizers has attracted in-
creasing attention. In March 2016, a regulation for CE fertilizers was
proposed to boost the use of organic and waste-based fertilizers
(European Commission, 2016). The proposal had two main objectives:
1) to create a market for fertilizers based on waste and by-products and
2) to harmonise cadmium limit for fertilizers in member states in order
to avoid cadmium accumulation in the soil. The commission proposed
to establish the limit for Cd to 60 mg/kg P2O5, and this value would be
Fig. 4. Inhibition of rape root and stalk growth in relation with the control
tightened to 40 mg/kg P2O5 after 12 years and to 20 mg/kg P2O5 after
sample.
15 years after adopting of the regulation. In organo-mineral fertilizers,
the proposal set a limit of up to 3 mg Cd/kg of fertilizer expressed as dry
solids in the case of fertilizers with a phosphorus content lower than 5% growth by 13–18%. In the case of fertilizers with biomass ash, the in-
P2O5. Requirements concerning Cd content for organo-mineral fertili- hibition was 26–29% compared to the control sample. At the same time,
zers containing more than 5% P2O5 should be the same as for mineral the stalk growth of rape was higher in all samples fertilised by sewage
fertilizers (European Commission, 2016). sludge-based fertilizers. The best results were obtained in the case of
From this point of view, sewage sludge-based fertilizers containing fertilizers with biomass addition, where rape stalks were 21% longer for
poultry litter ash (R-PA1–R-PA4) and biomass ash (R-BA4), which have fertilizer R-BA1 and 67% longer for fertilizer R-BA3 compared to the
less than 5% P2O5, meet the requirements of the proposal in regards to control sample. Similar results were obtained by Cybulska et al. (2018),
Cd content. In the case of R-BA3, the Cd concentration is higher than where the phytotoxicity effects of compost from poultry post-slaughter
the standard value (3.34 mg Cd/kg of fertilizer). R-BA1 and R-BA2 waste and commercial compost were examined. The authors suggest
(5.30 and 5.76% of P2O5) contain 51 and 31 mg Cd/kg P2O5, respec- that such results could be attributed to the organic matter and nutrient
tively, and fulfil the standard requirements of the proposed Directive. content of compost, which promoted better stalk growth of the tested
The impact of the new regulation on suppliers of phosphate rock, plants compared to the control sample.
fertilizer producers, and farmers is currently strongly contested. The
average Cd concentration in mineral fertilizers in the European Union is
3.2.6. Comparison with fertilizers available on the market
estimated to be 45 mg Cd/kg P2O5 (Cichy et al., 2014). The European
The granulation process for fertilizer R-PA2 was scaled up. The
Union suggests three main ways to obtain fertilizers with low Cd con-
obtained fertilizer product was characterised by a wide grain size range.
tent: 1) based on phosphate rock with low Cd content; 2) im-
However, the study has shown that there were no significant differences
plementation of decadmiation techniques, and 3) use of secondary raw
in nutrient content in each fraction (Table 7). The NPK concentration of
materials (Ridder et al., 2012).
the particular fractions was in line with the assumption. The granulated
The study by Fertilizer Europe showed that accepting new Cd limit
fertilizer met the standard requirements regarding heavy metal content.
of 60 mg would exclude 9% of fertilizers available on the market, 40 mg
A simplified analysis of raw material costs for sewage sludge-based
would exclude 32% and 20 mg would exclude 50% (Ulrich, 2019). In
fertilizer was made using the example of R-PA2. The costs of input
order to produce fertilizers that fulfil the new requirements, the Eur-
materials for the production of R-PA2 and of the input materials that
opean Union should consider increasing the supplies of low cadmium
could be used for the production of a blended fertilizer with the same
phosphate rocks, mainly from Russia, which has one of the largest de-
nutrient content as R-PA2 were calculated. The average prices of mi-
posits of phosphate ore with low cadmium content (Oosterhuis et al.,
neral fertilizers available from major global producers (‘Alibaba’) were
2000). This would result in the unavoidable dependence of the Eur-
used for calculation.
opean Union on one supplier, which can be associated with high fer-
Assuming that the indirect costs of fertilizer production in both
tilizer prices and political blackmail.
cases would be the same, production costs of sewage sludge-based
In the case of decadmiation technologies, it should be noted that
fertilizers would be 38–45% lower compared to traditional fertilizers
they exist but are not implemented on an industrial scale. It is estimated
with the same nutrient content (Table 8). This is due to the fact that
that investment costs of implementation of techniques to reduce Cd
fertilizer R-PA2 includes 50% waste, for which the producer does not
content will increase fertilizer prices by 5–10% (Ridder et al., 2012).
Furthermore, problems of the utilisation of waste with high Cd con-
Table 7
centrations will appear (Europe, 2014).
Composition of granulated organo-mineral fertilizer R-PA2.
The use of secondary raw materials for fertilizer production have
gained increasing attention as an element of sustainable nutrient Grain size 1–2 mm Grain size > 7 mm Mixed grains
management (Chojnacka et al., 2019). However, there are concerns
N % 11.6 ± 0.2 11.3 ± 0.1 11.5 ± 0.2
related mainly to contamination levels in waste fertilizing sources, their P2O5 5.63 ± 0.13 5.36 ± 0.11 5.17 ± 0.08
effectiveness and prices in comparison with conventional fertilizers K2O 17.3 ± 0.4 15.9 ± 0.4 16.2 ± 0.2
(Lupton, 2017). Regulatory and technical actions should be taken in Ca 2.02 ± 0.08 1.94 ± 0.05 1.91 ± 0.05
Mg 0.835 ± 0.004 0.787 ± 0.064 0.802 ± 0.021
order to improve the collection of waste, and to increase the safety and
Fe 2.32 ± 0.10 3.07 ± 0.06 2.13 ± 0.14
agronomic value of waste-based fertilizers. Zn mg/kg 624 ± 18 602 ± 11 566 ± 15
Cu 180 ± 8 175 ± 4 176 ± 3
3.2.5. Phytotoxicity Cr 56.9 ± 1.7 45.1 ± 1.2 57.5 ± 3.4
Four sewage sludge-based fertilizers were selected for phytotoxicity Pb 23.1 ± 0.2 22.5 ± 0.3 24.1 ± 2.0
Ni 58.5 ± 3.5 57.1 ± 0.8 58.2 ± 0.1
tests. The results of the tests are presented in Fig. 4.
Cd 1.62 ± 0.00 1.41 ± 0.10 1.61 ± 0.05
It should be noted that all fertilizers inhibited the root growth of Hg 0.712 ± 0.110 1.07 ± 0.41 –
rape. The fertilizers with poultry litter ash caused inhibition of root

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

Table 8
A simplified analysis of raw material costs used in sewage sludge-based fertilizer production.
Sewage sludge-based fertilizer Blended mineral fertilizer Blended mineral fertilizer II
R-PA2 I

N/P2O5/K2O = 11.5/5.2/16.2
Component Amount, kg Price, $ Component Amount, kg Price, $ Component Amount, kg Price, $
Sewage sludge 400 0 Single super-phosphate 289 64 NH4H2PO4 85 49
Poultry litter ash 100 0 KNO3 352 264 KNO3 352 264
KNO3 260 195 NH4NO3 188 56 (NH4)2SO4 256 49
NH4NO3 150 45
HNO3 (100%) 100 46
829 384 693 362
1000 286 1000 463 1000 522

bear the costs. Moreover, when the technology of sewage sludge-based order to show the importance of recycling nutrients and organic matter
fertilizers is implemented by an external firm, additional income would and to prove the safety of waste-based fertilizers is very important for
arise from the utilisation of sewage sludge from the WWTP, resulting in increasing public acceptance of such products (Mayer et al., 2016). The
decreased production costs. In Poland, the costs of sewage sludge uti- estimated prices of nutrients in fertilizer R-PA2 are higher than in fer-
lisation strongly fluctuate according to local conditions and are in the tilizer Polifoska 5 .
range 25–150 $/t of wet sewage sludge. Based on experimental data, it was calculated that it is possible to
The chemical composition of sewage sludge-based fertilizer R-PA2 produce 2716–4416 tonnes of organo-mineral fertilizers based on dried
was compared with mineral fertilizers dedicated for rape crop sewage sludge from WWTP in Żywiec. Moreover, such approach allows
(Polifoska 5, Lufobos pod rzepak), organic fertilizers (granulated cattle the recycling of 82–140 tonnes of phosphorus (P2O5) and 42–73 tonnes
manure, ecological granulated chicken manure) and sewage sludge- of nitrogen (N) annually. Additional economic benefits will result from
based fertilizers (OrCal, Oskar) available on the Polish market. The using poultry litter ash and biomass ash. It should be emphasised that
prices of nutrients in the compared fertilizers was calculated (Table 9). sewage sludge is a local, stable and cheap source of nutrients, which is
The total nutrient content of organo-mineral fertilizer R-PA2 is the very important in the case of the import dependency of Poland and the
same as that of mineral fertilizer Lubofos pod rzepak and 34% lower decreasing quality of phosphate rock.
than that of Polifoska 5. There are differences in the content of each Sewage sludge use for fertilizer production in order to recycle nu-
nutrient in the compared fertilizers. This can be attributed to the fact trients fits with the current European trend towards nutrient recycling
that such mineral fertilizers are also recommended for other crops and waste recovery. A number of technological concepts have been
(sugar beet, corn, potatoes), which have different nutritional require- created during recent years in Europe in this field, addressing mainly
ments (‘Polifoska 5’). It is worth pointing out that in the case of using bio-nutrients (Nutri2Cycle) and (RUN4LIFE) and organic carbon (SYS-
fertilizer R-PA2 there would be no need to use additional organic fer- TEMIC) as well as the recovery of bio-polymers, cellulose and bio-gas
tilizers, as besides its high NPK content the fertilizer contains organic production (SMART-Plant). The key objective of such projects is to
matter beneficial for plant growth, whereas the producers of mineral transform wastewater treatment plants into facilities where completely
fertilizers recommend soil fertilisation with manure before mineral new materials will be produced from waste streams. In some European
application. countries, nutrient recovery has become mandatory and a few gov-
Fertilizer R-PA2 has significantly higher total nutrient content in ernments have implemented political reforms related to phosphorus
comparison to organic fertilizers and fertilizers based on sewage sludge recovery in order to increase efficiency of nutrient use. In Switzerland,
produced in Poland (OrCal, Oskar), which will have an impact on fer- phosphorus recovery from sewage sludge, sewage sludge ash and meat
tilizer doses and the associated costs of transport and application. and bone meal is legally binding by ordinance (Ordinance on Avoid-
The prices of nutrients in mineral fertilizers are lower than in or- ance and Disposal of Waste). A new Sewage Sludge Ordinance Reg-
ganic fertilizers due to their high nutrient content. The fertilizer Oskar ulation entered into force in Germany in 2017, according to which
has the lowest nutrient prices, resulting from the low price of the fer- sewage treatment plants serving populations over 50,000 should re-
tilizer. The low price of waste-based fertilizers is common, due to the cover phosphorus from sewage sludge. Phosphorus should be recovered
lack of consumer confidence. Education and demonstration projects in from sewage sludge with a phosphorus content of not less than 2% of

Table 9
Comparison of produced organo-mineral fertilizer with mineral, organic and sewage sludge-based fertilizers available on the Polish market.
R-PA2 Polifoska 5 Lubofos pod rzepak Granulated cattle manure Granulated chicken manure (ecological) OrCala Oskarb

Moisture content % 3 >5 >5 10 10 na na


Organic matter ~20 0 0 ~65 ~65 ~20–40 ~50
N 11.5 5 3.5 2 4 4.7 3
P2O5 5.2 15 10 5 3 2.5 3
K2O 16.2 30 18.5 2 3 1.3 0.3
Total NPK content 32.9 50 32 9 10 8,5 6.3
CaO 2.7 na 2 na 9 25–36 na
MgO 1.3 2 2.5 1 1 na 16
Nitrogen price (N) $/kg 0.75c 0.67 0.80 1.52 3.79 1.39 0.01
Phosphorus price (P) 0.41c 0.37 0.44 0.83 2.07 0.76 0.05
Potassium price (K) 0.77c 0.69 0.82 1.56 3.89 1.42 0.10

na – data not available.


a
fertilizer produced by mixing sewage sludge with alkali agent.
b
fertilizer produced by treating sewage sludge with magnesite and sulfuric acid.
c
estimated only on the basis of raw materials costs.

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H. Kominko, et al. Journal of Environmental Management 248 (2019) 109283

sewage sludge, expressed as dry mass; in the case of a lower phosphorus salt-soils. Sci. Total Environ. 578, 47–55. https://doi.org/10.1016/j.scitotenv.2016.
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