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Bioresource Technology 291 (2019) 121857

Contents lists available at ScienceDirect

Bioresource Technology
journal homepage: www.elsevier.com/locate/biortech

Filling in sewage sludge biodrying gaps: Greenhouse gases, volatile organic T


compounds and odour emissions
Daniel Gonzáleza,b, Nagore Guerrac, Joan Colónc, David Gabrielb, Sergio Ponsác,
Antoni Sáncheza,

a
Composting Research Group (GICOM) Dept. of Chemical, Biological and Environmental Engineering, Universitat Autònoma de Barcelona, 08193-Bellaterra, Barcelona,
Spain
b
Group of Biological Treatment of Liquid and Gaseous Effluents (GENOCOV) Dept. of Chemical, Biological and Environmental Engineering, Universitat Autònoma de
Barcelona, 08193-Bellaterra, Barcelona, Spain
c
BETA Technology Centre: “U Science Tech”, University of Vic-Central University of Catalonia, 08500 Vic, Barcelona, Spain

GRAPHICAL ABSTRACT

ARTICLE INFO ABSTRACT

Keywords: In the present work, a complete study of the sewage sludge (SS) biodrying technology was conducted at bench-
Sewage sludge scale, aiming at assessing its performance and providing a valuable insight into the different gaseous emission
Biodrying patterns found for greenhouse gases (GHG) and odorant pollutants. As process key parameters, temperature,
Gaseous emission specific airflow, dynamic respiration index, final moisture content and Lower Calorific Value (LCV) were
Greenhouse gases (GHG)
evaluated. At the end of the biodrying, a product with a 35.9% moisture content and a LCV of
Odour
7.1 MJ·kg−1product was obtained. GHGs emission factor was 28.22 kgCO2eq per Mg of initial mass of dry matter
in the SS (DM0-SS). During the biodrying process, maximum odour concentration measured was 3043 ou·m−3
and the estimated odour emission factor of the biological treatment was 3.10E + 07 ou per Mg DM0-SS. Finally,
VOCs were completely identified and quantified. The most abundant VOCs found in the biodrying gaseous
emissions were terpenes, sulphur-compounds and ketones.

1. Introduction processes are used to manage SS produced, such as land application,


thermal processing, composting or anaerobic digestion, aiming at re-
The large amount of sewage sludge (SS) production is becoming a ducing its volume and quantity as well as stabilizing it. In fact, com-
worldwide environmental problem. Nowadays, different treatment posting, which is one of the most applied SS stabilization approaches, is


Corresponding author.
E-mail address: antoni.sanchez@uab.cat (A. Sánchez).

https://doi.org/10.1016/j.biortech.2019.121857
Received 3 June 2019; Received in revised form 16 July 2019; Accepted 20 July 2019
Available online 23 July 2019
0960-8524/ © 2019 Elsevier Ltd. All rights reserved.
D. González, et al. Bioresource Technology 291 (2019) 121857

considered as an environmental friendly technology. Nevertheless, screening on the diversity of VOC families found in the gaseous emis-
there are some limitations when applying SS or the compost obtained sions from the biodrying of SS, which can be valuable information in
from SS on soil due to the possible presence of heavy metals or other further environmental assessment studies.
emergent contaminants (European Commission, 2014). Regarding that,
and taking into account the limited land resources, thermal processes
2. Materials and methods
have risen as an attractive sludge treatment option in many countries.
However, due to the high water content present in SS, a pre-drying step
2.1. Characteristics of feedstock
is required prior to incineration. Between the existing alternatives for
SS drying, biodrying is catching attention of researchers in the last years
SS was obtained from the wastewater treatment plant of Navàs,
(Huiliñir and Villegas, 2015; Villegas and Huiliñir, 2014; Zhao et al.,
Barcelona, which treats 1500 m3·d−1 of domestic wastewater.
2011). The objective of SS biodrying process, which is based on the
Diatomaceous earth (DE), which was used as a high-energy content co-
mechanisms of a composting process, is to remove water from biowaste
substrate to enhance metabolic activity and to adjust moisture content
with high moisture content and to reduce the volume and the biological
(Johnson, 1997), was obtained from the organic fraction of Municipal
activity of the solid matrix to obtain a product with a considerable
Solid Waste (MSW) biomethanization plant of Can Barba in Terrassa,
Lower Calorific Value (LCV) and low moisture content that can be used
Barcelona. Finally, pruning waste (PW), used as bulking agent, was
as a biomass fuel (Adani et al., 2002). To this aim, both the metabolic
obtained from the composting plant of Manresa, Barcelona. The mix-
heat generated during the aerobic degradation of the easily biode-
ture was prepared manually with an industrial mixer, and the used
gradable organic matter as well as forced aeration are used (Frei et al.,
mixing ratio of the three feedstocks (SS:DE:PW) was 1:0.25:3 on a vo-
2004). In this sense, and compared with composting, higher aeration
lume basis and 1:0.15:0.48 on weight basis, which is a typical mixing
rates are used during biodrying to enhance water removal (Cai et al.,
ratio used during SS composting (González et al., 2019a; Maulini-Duran
2013; Yuan et al., 2016).
et al., 2013). As aforementioned, the addition of a 10–15% of DE
Different studies have been conducted to find operating strategies to
(weight basis) has been reported to enhance the metabolic activity of
optimize the SS biodrying process in terms of aeration and initial
the mixture in different treatment processes (Pognani et al., 2012).
moisture content, as they are the key parameters to achieve an optimum
Table 1 shows the physical-chemical characteristics of each material
SS biodrying performance. For example, Cai et al. (2013) studied the
and mixture.
influence of aeration on water removal reporting higher evaporation
rates at higher aeration rates during the thermophilic phase of the SS
biodrying process. Moreover, Huiliñir and Villegas (2015) worked on 2.2. Experimental set-up and process operation
the simultaneous effect of the aeration and the initial moisture of the
material on the water evaporation. They reported that higher material Fig. 1 shows a scheme of the biodrying pilot plant. A cylindrical
temperature is achieved when initial moisture content is around 68% bioreactor with an operative volume of 100 L was used to carry out the
and that, under these conditions, higher aeration rates enhance water SS biodrying process. The reactor was filled with 41.4 kg of the mixture
evaporation. However, critical aspects such as gaseous emissions and its with a density of 414 kg·m−3. The dimensions of reactor were 0.85 m
associated environmental impacts have not been systematically studied high and had a diameter of 0.50 m. The internal and external walls of
yet as it has been done with SS composting. Greenhouse gases (GHG) the reactor were made of stainless steel. A thermal isolation layer of
and odorant compounds characterization have been widely reported for polyurethane foam (2 cm) was used to avoid heat losses and to maintain
SS composting at bench-scale (Maulini-Duran et al., 2013; Rincón et al., near-to-adiabatic conditions. A perforated plate was fixed at the bottom
2019), whereas few studies have been conducted in full-scale facilities of the reactor to support the material and to facilitate aeration, working
(González et al., 2019a; Shen et al., 2012). Nonetheless, few informa- as a diffusor. The biodrying reactor was opened but covered with a
tion about gaseous emissions from bench-scale SS biodrying can be straw cover to prevent heat loss and vapour condensation on the mix-
found in literature (Kim et al., 2018; Wei et al., 2016), but with no ture. Temperature of the material was measured with a temperature
concluding or profitable information in terms of environmental impact probe (PT-100, Iserntech S.A., Spain) introduced into the reactor, with
of the technology. In this sense, gaseous emissions assessment studies sensors located at the top, middle and bottom of each one. An air
must be carried out to fill existing knowledge gaps and to help im- compressor (Dixair DNX 2050, Worthington Creyssensac, Spain) and
proving the performance of such biological treatment technology. digital mass flow controllers (D-6311-DR, Bronkhorst High-Tech B. V.,
Emission factors referred to specific pollutants are a useful tool for Ruurlo, Netherlands) were used for continuous aeration. During bio-
environmental impact assessment and facilitate the estimation of the drying, the aeration flowrate was regulated based on the temperature of
overall emission rate of a treatment process based on a specific activity the material using a feedback control loop. The control software
index, which should represent the process evaluated (Capelli et al., adapted the aeration level depending on different temperature ranges
2009). The US Environmental Protection Agency defined the emission referred to the temperature in the middle of the reactor (< 35 °C;
factor of a specific pollutant as the relation between the quantity of the 35–45 °C; 45–55 °C; 55–70 °C; > 70 °C), increasing the airflow rate
pollutant emitted to the atmosphere with an activity associated with the
release of the pollutant, such as the mass of waste to be treated, the Table 1
emitting surface or time units (United States Environmental Protection Physical-chemical properties of the feedstocks and mixture used during the
Agency (USEPA), 1995). Analogously, in the last years this tool has biodrying process.
been referenced for the assessment of odour impact from different Physicochemical SS PW DE Biodrying
treatment processes and facilities, namely Odour Emission Factor (OEF) properties mixture
(Capelli et al., 2014; Sironi et al., 2006).
Moisture (%) 83.5 ± 0.1 18.0 ± 0.0 3.9 ± 0.0 54.6 ± 0.1
To the authors’ knowledge, this is the first bench-scale work where a Organic matter (%) 68.9 ± 0.2 88.7 ± 0.0 35.2 ± 0.1 85.2 ± 0.0
systematic study of the gaseous emissions generated during the bio- C/N ratio 9.1 31.6 1321.6 13.6
drying process of conventional SS is conducted. Due to the lack of this pH 6.7 8.2 6.2 –
scientific information and its importance for further development of the Electrical conductivity 2.5 1.7 1.2 –
(mS/cm)
biodrying technology, the aim of this work was to study the SS bio-
DRI24h (g O2·h−1·kg−1 7.3 ± 0.9 – – 6.3 ± 1.7
drying process performance and, specially, to acquire knowledge about VS)
the GHGs and odorant gaseous emission patterns related to this treat-
ment. Emission factors for specific pollutants are provided, as well as a SS: sewage sludge; PW: pruning waste; DE: diatomaceous earth.

2
D. González, et al. Bioresource Technology 291 (2019) 121857

Fig. 1. Scheme of the biodrying system and the external industrial mixer used during the experiment (TT represents the temperature measure; FC represents the mass
flow controller; O2T represents the O2 measure).

when the material temperature increased (2, 6, 10, 14 and 20 L·min−1, the injector temperature was 120 °C, the detector temperature was
corresponding to 0.12, 0.36, 0.60, 0.84 and 1.20 L·min−1·kg−1 of initial 345 °C and the oven, which worked isothermally, was set at 60 °C. The
total VS of mixture). In this case, the middle temperature was used to injection volume used for each sample was 500 µL and the total time of
regulate airflow because both the bottom and the top temperatures of analysis was 4 and 6 min for CH4 and N2O, respectively.
the reactor can be influenced by the temperature of the inlet airflow or Odour concentration analysis were performed using a SM-100 por-
due to the loss of volume of the material along the biodrying process, table field olfactometer provided by Scentroid (IDES Canada, Inc.,
respectively. To follow the evolution of the process in terms of biode- Whitchurch-Stouffville, ON, Canada), as explained in González et al.
gradation, the oxygen content of the outlet gas of the reactor was (2019b). All gaseous samples were analysed three times by the same
monitored using an O2 sensor (O2 A1, Alphasense, UK) located after a panellist in a closed, well-ventilated room the same day of sampling.
condensation trap to prevent sensors damage. The biodrying process Total volatile organic compounds (tVOCs), NH3 and H2S concentration
lasted 13 days and the material was mixed manually every day during of the outlet gases of the reactor were measured daily in situ with a
the thermophilic phase and every two days during the mesophilic stage. MultiRAE Lite portable analyser (RAE Systems, San José, CA, USA),
Water and VS loss during the biodrying process was monitored through equipped with a 10.6 eV PID lamp for tVOCs measurement and two
weight loss using a scale (Gram Precision k3-k3i, Gram Group, Spain). electrochemical sensors for NH3 and H2S measurement, respectively.
Arduino UNO was used for data acquisition and LabView 2017® was tVOCs detection ranged from 0 to 1000 ppmveq isobutylene with
used for data analysis and airflow control. 1 ppmveq isobutylene increments, NH3 detection ranged from 0 to
100 ppmv with 1 ppmv increments and H2S detection ranged from 0 to
2.3. Gas sampling and analysis methodologies 100 ppmv with 1 ppmv increments. During each analysis, the portable
analyser was placed inside a closed recipient with inlet and outlet ports
A semi-spherical stainless steel flux chamber (0.443 m of base dia- and the outlet gases of the reactor were passed through it until a steady
meter, 0.154 m2 of base area and 0.045 m3 of volume) provided by value was read on the analyser. Since the biodrying process was held in
Scentroid (IDES Canada Inc., Whitchurch-Stouffville, ON, Canada) was an open reactor, a suction pump was used to redirect part of the outlet
used daily to perform emissions sampling (González et al., 2019b). gases from the surface of the material to the hermetic recipient where
Nalophan® bags were used to store gas samples, which were flushed the portable analyser was placed. The gases were measured just before
twice before obtaining the final gaseous sample for analysis. All gas the water trap installed to protect the rest of the measurement devices
samples were always obtained before mixing of the material. from the gaseous flow moisture.
CH4 and N2O analysis were performed using an Agilent 6890 N Gas To perform the VOCs characterization, two different gaseous sam-
Chromatograph (GC) (Agilent Technologies, Inc., Santa Clara, CA, ples of 1 L each were pumped through sorbent tubes packed with two
USA), equipped with a flame ionization detector (FID) and an electron different hydrophobic sorbents (Tenax® TA and Carbograph™ 1TD,
capture detector (ECD) for CH4 and N2O detection, respectively. The Markes International, Inc., Gold River, CA, USA) by means of a manual
column used for the analysis was a HP-PLOT Q semi-capillary column sampling pump (Markes International, Inc.). The gaseous samples were
(30 m × 0.53 mm × 40.0 µm, Agilent Technologies, Inc.) with N2 as obtained the 3rd and the 12th day of running, coincident with the
carrier gas at 2 psi pressure, and a post-column particle trap (2 m, n° thermophilic and the mesophilic phases of the biodrying process. First,
5181–3352, Agilent Technologies, Inc.). For CH4 analysis, the injector a UNITY-2 Thermal Desorber (TD) (Markes International, Inc.) was
temperature was 240 °C, the detector temperature was 250 °C and the used to desorb the gaseous samples retained in the sorbent tubes. Then,
oven, which worked isothermally, was set at 60 °C. For N2O analysis, an Agilent 7820 GC coupled to an Agilent 5975 Mass Spectrometer

3
D. González, et al. Bioresource Technology 291 (2019) 121857

(MS) (Agilent Technologies, Inc.) was used to analyse and characterize 3. Results and discussion
the different VOCs present in the gas samples (González et al., 2019b).
Both samples were analysed the same day that they were obtained in 3.1. Biodrying performance
order to preserve the stability of VOCs in sorbent tubes (Ribes et al.,
2007). Fig. 2a shows the performance of the biodrying reactor while a
summary of the process parameters evaluated during the treatment is
2.4. Estimation of the gaseous emission factors presented in Table 2. In Fig. 2a, the evolution of the temperature in the
middle of the solid matrix, the specific airflow, the decrease of moisture
The emission factor was calculated based on the measured con-
centration of a specific pollutant, the aeration flow through the reactor
at time of each sampling event and normalised by the initial mass of dry
matter in the SS (DM0-SS) introduced in the reactor. Firstly, daily
emission rates of each pollutant were calculated (Eq. (1)).
ERi = Ci F (1)

where ERi is the emission rate of the target pollutant (mg pollu-
tant·d−1); Ci is the concentration of the target pollutant (mg pollu-
tant·m−3); F is the aeration flow through the reactor during sampling
(m3·d−1).
Then, the emission rates of a target pollutant obtained for each
sampling day were represented versus process time, thus the area below
the curve obtained corresponds to the emitted total mass of the pollu-
tant throughout the process studied. Finally, the emitted total mass of a
target pollutant was divided by the initial mass of DM0-SS introduced in
the reactor to obtain the emission factor (Eq. (2)).
mi
EFi =
I (2)

where EFi is the emission factor of the target pollutant (mg pollu-
tant·kg−1 DM0-SS); mi is the total emitted mass of the target pollutant
during the process (mg pollutant); I is the initial mass of DM0-SS treated
as specific activity index (kg DM0-SS).

2.5. Analytical methods for solid samples

Moisture content, dry matter, organic matter content, N-Kjeldhal,


C/N ratio, pH and electrical conductivity were determined according to
the standard procedures (US Dept. of Agriculture and US Composting
Council, 2001; Water Environment Federation, 1995). To evaluate the
final biological stability of the treated material, the Dynamic Respira-
tion Index in the 24 h of maximum biological activity (DRI24h) and the
cumulative oxygen consumption in 4 days (AT4) were used. These in-
dices provide information about the biological stability of an organic
solid sample, and are expressed in g O2·h−1·kg−1 VS and g O2·kg−1 VS,
respectively. The determination of the DRI24h and the AT4 was per-
formed using a dynamic respirometer (Ponsá et al., 2010) as explained
in González et al. (2019a).
The determination of the Higher Calorific Value (HCV) was done by
means of a bomb calorimeter (1341 Plain Jacket Calorimeter – 1108
Oxygen Combustion Vessel, Parr, IL, USA), according to manufacturer’s
instructions and following the methodology proposed at the DIN
51900-3:2005 (German Institute for Standardisation, 2003). The Lower
Calorific Value (LCV) was calculated from HCV according to Eq. (3), Fig. 2. (a) Performance of the biodrying process. In black dots, the evolution of
taking into account the moisture content of the final product and its the temperature of the material in the middle of the reactor (°C); in white dots,
estimated hydrogen content (Koppejan and van Loo, 2008). the evolution of the moisture content of the solid mixture (%); solid line, the
specific airflow introduced in the reactor (L·min−1·kg−1 VS0), black arrows
MC MC H MC represent the mixing pattern. (b) CH4 and N2O emission rate profile during the
LCV = HCV 1 2.444 2.444 8.936 1
100 100 100 100 biodrying process. In black dots, the temperature of the material in the middle
(3) of the reactor (°C); in white squares, the inlet specific airflow rate
(L·min−1·kg−1 VS0); in blue squares, the evolution of the CH4 emission rate (mg
where LCV is the Lower Calorific Value of the biomass fuel (MJ·kg−1 CH4·d−1); in green triangles, the evolution of the N2O emission rate (mg
product); HCV is the Higher Calorific Value of the biomass fuel N2O·d−1). (c) Odour emission rate (OER) profile during the biodrying process.
(MJ·kg−1 DM); MC is the moisture content of the biomass fuel (%); H is In black dots, the temperature of the material in the middle of the reactor (°C);
the estimated hydrogen content of the biomass fuel (%), which was in white squares, the inlet specific airflow rate (L·min−1·kg−1 VS0); in cyan
considered to be a 5% (Choi et al., 2014); 2.444 is the enthalpy dif- squares, the evolution of the odour emission rate (OER, ou·d−1). (For inter-
ference between liquid water at 25 °C and gaseous phase; 8.936 is the pretation of the references to colour in this figure legend, the reader is referred
molecular weight ratio between both molecules (mH2O·m−1H2). to the web version of this article.)

4
D. González, et al. Bioresource Technology 291 (2019) 121857

Table 2 –increasing a 65.1% compared to the initial LCV–, which is known to be


Summary of the process parameters evaluated during the biodrying process. sufficient for self-sustaining combustion (Hao et al., 2018).
Parameter Biodrying Units
3.2. Greenhouse gases emissions
Air supplied Total air volume 1.4E + 05 L
Average air supply 0.46 L·min−1·kg−1 VS0
GHGs emissions from SS composting processes have been widely
2.54 L·min−1·kg−1 VSSS
Total evaporated water 13.3 kg H2O
reported in the past years due to their potential impact to global
Calorific value HCV Initial 15.1 ± 0.1 MJ·kg−1 TS warming (Pan et al., 2018; Yuan et al., 2016). However, an information
Final 13.6 ± 0.2 gap exists about GHGs emission generated during the biodrying of SS. It
LCV Initial 4.3 ± 0.1 MJ·kg−1 product has to be mentioned that during this study, only GHGs emissions re-
Final 7.1 ± 0.1
ferred to the biological process have been accounted, and CO2 has not
Biological stability DRI24h Initial 6.3 ± 1.7 g O2·h−1·kg−1 VS
Final 3.5 ± 0.1 been taken into account due to its biogenic origin. Fig. 2b shows the
AT4 Initial 403.6 ± 43.8 g O2·kg−1 VS daily emission rates of CH4 and N2O from the biodrying processes, al-
Final 175.1 ± 18.9 together with the temperature profile of the material and the specific
airflow supplied to the reactor. At first sight, two different emission
HCV: higher calorific value; LCV: Lower Calorific Value.
patterns were found for CH4 and N2O. In general, the CH4 emission
pattern followed the temperature profile of the material, presenting its
content and the mixing pattern are represented for the whole process
emission peak when maximum temperature and maximum aeration
time. As expected, two temperature stages were encountered, a ther-
occurred. On the other hand, N2O showed a high emission peak the first
mophilic stage (> 41 °C) and a mesophilic stage (≤41 °C). Temperature
sampling day due to the stripping effect of the remaining N2O present in
increased rapidly during the first 48 h to the maximum values regis-
the SS, which rapidly decrease to lower values. However, an increase of
tered (51.0 °C).
the N2O emission was observed when the temperature of the material
The key parameters to explain the biodrying process are tempera-
was below 40 °C, suggesting that an increase in the SS biodrying process
ture, specific airflow and moisture content of the solid material, which
time would have a negative effect in terms of GHG emissions.
are shown in Fig. 2a for the whole process time. Similar to a typical SS
Generally, CH4 is formed by methanogens under anaerobic condi-
composting process, material temperature reached its peak on day 2.
tions. Anaerobic spots can be created around the reactor by the oxygen
Then, temperature was maintained around 40 °C until day 7. There-
demand at this temperature range due to the rapid degradation of or-
after, the temperature progressively decreased to a final value of 30 °C,
ganic matter during thermophilic phase (Yuan et al., 2016). As ob-
as previously observed in this kind of biological treatment (Huiliñir and
served in Fig. 2b, the peak of CH4 emission coincided with that of
Villegas, 2015). Specific airflow, referred to the total VS in the initial
temperature, and then CH4 emission decreased as temperature de-
mixture (VS0) or to the initial VS in the SS (VSSS), depended on the
creased into the mesophilic range. Maximum and minimum CH4 con-
temperature in the middle of the biodrying reactor. Its average value
centration measured during the SS biodrying process were 8.16 ppmv
during the whole process was 0.46 L·min−1·kg−1 VS0 (2.54
and 1.07 ppmv, respectively.
L·min−1·kg−1 VSSS), which is a typical specific airflow for SS biodrying
The formation of N2O is complex, which can be produced by deni-
(Cai et al., 2013; Huiliñir and Villegas, 2015) and higher than the
trification when NO3− is converted to N2O and nitrogen gas, and by
specific airflows reported during conventional SS composting (Maulini-
incomplete nitrification during the conversion of NH3 to NO2−
Duran et al., 2013; Yuan et al., 2016). These high aeration rates used in
(Moënne-Loccoz and Fee, 2010). The N2O emission rates for the SS
biodrying are necessary to supply oxygen to microorganisms but also to
biodrying process are presented in Fig. 2b. During the first sampling
enhance water evaporation. The maximum specific airflow registered
day, a peak of N2O emission appeared, mainly because of the stripping
during the biodrying process (0.84 L·min−1·kg−1 VS0; 4.63
effect of remaining N2O present in the SS used for the experiment. Once
L·min−1·kg−1 VSSS), coincides with the peak of temperature found in
this first N2O was stripped out of the SS, there was no sign of N2O
order to maximise water evaporation during the period of maximum
production until the temperature of the material decreased to a meso-
biological activity. In contrast, the minimum specific airflow registered
philic range. At that point, an increase of the N2O emission appeared
(0.12 L·min−1·kg−1 VS0; 0.66 L·min−1·kg−1 VSSS) was found during the
until the end of the process. Results suggest that the temperature of the
first day of biodrying, which helped to rapidly reach thermophilic
material below the high-end of the mesophilic range (40 °C), together
conditions inside the reactor. The biodrying process was stopped on day
with the low carbon availability at the latter stages of the process, af-
13, when a 34.3% reduction of the moisture content of the material was
fected the microbial activity and, concomitantly, the formation and
achieved, obtaining a final material with a 35.9% of moisture content,
stripping of N2O. Under these conditions some denitrifying bacteria can
even lower to what is reported in other studies (Cai et al., 2013; Hao
promote the N2O formation by NO3− denitrification at the end of the
et al., 2018). The biodrying process time used is between typical re-
process (Ahn et al., 2011; Fukumoto et al., 2003). This fact should be
ported values (Huiliñir and Villegas, 2015; Tambone et al., 2011) and,
confirmed by characterizing the activity and the diversity of the bac-
even though moisture content could have been reduced even more, its
terial communities in future works. Moreover, and despite the forced
extension will imply higher aeration costs, especially at full-scale. The
aeration and the fact that the material was mixed every day, different
final DRI24h of the biodried material was 3.5 ± 0.1 g O2·h−1·kg−1 VS,
anoxic spots could had been formed inside the reactor and promote the
corresponding to a 44.4% reduction of the initial DRI24h. Despite the
formation of N2O by denitrification (Awasthi et al., 2018). Maximum
DRI24h reduction achieved, it is worth mentioning that the main goal of
and minimum N2O concentrations measured during the SS biodrying
SS biodrying is not to stabilize the organic waste, but to reduce its
process were 18.75 ppmv and 0.37 ppmv, respectively.
moisture content in a short-term process to obtain a product with a LCV
Table 3 shows the emission factor of each GHG in the SS biodrying
enough to be used as a biomass fuel. Moreover, no related literature
process as kg of CH4 or N2O per Mg DM0-SS and per Mg DM0 of mixture
presenting the biological stability of the final biodried material has
and in kg of CO2eq per Mg DM0-SS and per Mg DM0 of mixture, re-
been found for SS biodrying processes, as it happens with other wastes
spectively. These emission factors are valuable information to help
such as MSW (Evangelou et al., 2016). In contrast, conventional SS
comparing different treatment strategies and evaluating its environ-
composting seeks reducing the biological activity of the material but
mental impact. Besides, it is important to highlight the much higher
applying longer process times, obtaining final DRIs24h lower than 1 g
environmental impact in terms of Global Warming Potential of N2O
O2·h−1·kg−1 VS (Maulini-Duran et al., 2013). Finally, the LCV of the
(265 times higher than that of CO2) compared with CH4 (28 times
final material was analysed and was found to be 7.1 MJ·kg−1 product
higher than that of CO2) (IPCC, 2014). To contextualize the results

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D. González, et al. Bioresource Technology 291 (2019) 121857

Table 3
CH4, N2O, NH3, H2S, tVOCs and odour emission factors for the biodrying process. GHG emission factors are expressed in kg of pollutant and in kg of CO2
equivalent per Mg DM0-SS and Mg DM0 of mixture, respectively. Odorant emission factors are expressed in kg of pollutant per Mg DM0-SS and Mg DM0 of
mixture and odour emission factor is expressed in ou per Mg DM0-SS and Mg DM0 of mixture, respectively.
kg pollutant·Mg−1 DM0-SS kg pollutant·Mg−1 DM0
GHGs CH4 emission factor 4.54E-02 1.02E-02
N2O emission factor 1.02E-01 2.28E-02

kg CO2eq·Mg−1 DM0-SS kg CO2eq·Mg−1 DM0


GHGs CH4 emission factor a 1.27 0.28
N2O emission factor a 26.95 6.04
GHG emission factor a,b 28.22 6.32

kg pollutant·Mg−1 DM0-SS kg pollutant·Mg−1 DM0


Odorants NH3 emission factor 1.23 2.75E-01
H2S emission factor 1.68E-03 3.77E-04
tVOCs emission factor 1.38E-01 3.10E-02

ou·Mg−1 DM0-SS ou·Mg−1 DM0


Odour Odour emission factor 3.10E + 07 6.95E + 06

a
GHGs emission for CH4 and N2O, on a 100-yr frame, is 28 and 265 times higher than that of CO2, respectively (IPCC, 2014).
b
GHGs emission factor as the sum of the CH4 and N2O emission factors.

obtained, the GHG emission factors have been contrasted with GHG 2012; He et al., 2017), and it is known to occur at their maximum rate
emission factors obtained from SS composting, because, to the authors’ during the thermophilic phase of the biological process, since high
knowledge, no previous GHG emission factors from SS biodrying have temperatures favour NH3 volatilization by displacing the NH4+/NH3
been reported. For example, Yuan et al. (2016) reported GHG emission equilibrium to NH3. H2S during SS biological treatment also occurs
factors depending on the aeration rate in the range of 170.43–272.52 kg during the first stage of the process and it is enhanced by high tem-
CO2eq·Mg−1 DM0-SS during the composting of dewatered non-digested peratures. Its formation results from bacterial reduction of sulphate and
sewage sludge with cornstalks as bulking agent in a 60 L aerated bench- decomposition of sulphur-containing compounds present in the SS
scale reactor. On the other hand, Maulini-Duran et al. (2013) found under anaerobic conditions (Chen et al., 2010). VOCs have been also
lower GHG emission factors referred to the SS composting in a 50 L reported to be released at their highest production rate during the in-
aerated bench-scale reactor, using wood chips as bulking agent, ranging itial forced aeration of the biological treatment of SS. In this case, NH3,
from 4.98 to 9.90 kg CO2eq·Mg−1 DM0-SS. Pan et al. (2018) observed H2S and tVOCs maximum concentrations measured during SS biodrying
GHG emission factors ranging from 36.05 to 134.56 kg CO2eq·Mg−1 were 330 ppmv of NH3, 1 ppmv of H2S and 18 ppmveq isobutylene, re-
DM0 of mixture while composting dewatered SS with wheat straw and spectively, which were all observed during the peak of maximum
different acidic additives in a 150 L bench-scale composting reactor. temperature of the material in the reactor. In SS composting processes,
Moreover, the GHG emission factor related to SS biodrying process was different ranges of target pollutants concentration can be found in lit-
lower than those reported for conventional SS drying systems, which erature depending on the characteristics of the feedstocks or the com-
are in a higher range between 367 and 21900 kg CO2eq·Mg−1 DM0-SS posting process itself. Hort et al. (2009) reported NH3 concentrations
due to the use of fossil fuels and chemicals (Chen and Kuo, 2016). In above 70 ppmv during the bench-scale SS and yard waste composting,
comparison with the experimental emission factors reported for SS but no H2S was reported due to a proper aeration of the material during
composting processes, the SS biodrying treatment seems a feasible the first steps of the biological process. Besides, Pagans et al. (2006)
technology in terms of GHG emission impact. However, future studies reported maximum concentrations of 132 ppmv of NH3 and 260 ppmv of
are warranted to minimise N2O emissions by understanding the biolo- C-tVOCs while composting raw sludge in a forced-aerated 30 L lab-scale
gical pathways for N2O generation during the SS degradation and the reactor. On the other hand, González et al. (2019a) measured NH3 and
effect of the aeration rate on its emission in order to decrease the total tVOCs of 250 ppmv and 18 ppmv, respectively, during the SS com-
GHGs emissions related to the SS biodrying process. Ensuring aerobic posting in a full-scale composting plant.
conditions in the SS biodrying reactor is a key factor to minimize GHG To put the obtained results into context, the emission factors of the
emissions. As reported by different authors studying SS composting SS biodrying process have been compared with other reported emission
processes, low aeration and inadequate initial moisture content have a factors from different composting processes, since no information has
great impact on increasing GHG emission (Villegas and Huiliñir, 2014; been found about other biodrying processes. Maulini-Duran et al.
Yuan et al., 2016). Results reported herein are a good starting point for (2013) reported NH3 and tVOCs emission factors in the range of
future environmental impact assessment of the SS biodrying tech- 1.33–4.12 kg NH3·Mg−1 DM0-SS and 0.66–1.00 kg C-VOC·Mg−1 DM0-
nology, which can be used for Life Cycle Assessment studies. SS, respectively, during composting of raw sludge in a 50 L aerated
bench-scale reactor. Rincón et al. (2019) studied the gaseous emissions
3.3. Odorant compounds emissions from the SS composting in a 300 L pilot-scale reactor, reporting an NH3
emission factor of 2.16 kg NH3·Mg−1 DM0 of SS and a tVOCs emission
3.3.1. NH3, H2S, tVOCs and odour emissions factor of 1.21 kg C-VOC·Mg−1 DM0-SS. González et al. (2019a) studied
Emissions of NH3, H2S, tVOCs and odour from the SS biodrying the emission of NH3 and tVOCs in a full-scale sewage sludge composting
process were monitored during the whole process to fill the existing plant, reporting emission factors of 8.53 kg NH3·Mg−1 DM0 of mixture
knowledge gap about gaseous emissions associated to this SS biological and 2.09 kg C-VOC·Mg−1 DM0 of mixture. In addition, Gomez-Rico
treatment. Table 3 presents the emission factors obtained as kg of et al. (2008) and Deviatkin et al. (2019) reported higher tVOCs and NH3
pollutant per Mg DM0-SS and per Mg DM0 of mixture, respectively, and emission factors (0.59 kg C-VOC·Mg−1 DM0-SS and 1.03 to 6.00 kg
in ou per Mg DM0-SS and per Mg DM0 of mixture, respectively, when NH3·Mg−1 DM0-SS, respectively) during different conventional drying
monitoring the biodrying processes·NH3, H2S, tVOCs are the typical of SS at 100–120 °C at lab-scale. The variability between the different
precursors of odour nuisance generated during the biological treatment studies shows that, even by treating the same type of organic waste, the
of organic wastes such as SS·NH3 emissions during aerobic biode- substrates nature and process conditions (aeration level, initial
gradation of organic wastes have been widely reported (Colón et al., moisture, scale, etc.) affect the emission of the odorant pollutants.

6
D. González, et al. Bioresource Technology 291 (2019) 121857

However, results obtained in the present work represent a valuable 3.3.2. VOCs characterization
insight that will allow a better understanding of the environmental A chemical characterization was made by comparing the VOC fa-
impact related to this new technology. milies found in the different samples as well as by quantifying the
Fig. 2c shows the daily odour emission rates (OER) obtained during concentration of 17 out of the 35 detected compounds. Fig. 3 presents
the SS biodrying process. Similarly to other works where odour emis- the distribution of the different VOC families found in the samples of
sion from SS composting were studied (González et al., 2019b; Rincón two different days obtained during the SS biodrying process. Terpenes
et al., 2019) the odour emission profile reached its maximum during the –with α-pinene as predominant– are the main VOC family found in the
thermophilic phase, when biological activity was higher. Temperature gaseous samples analysed, with relative abundances between 70 and
is one of the key factors affecting the emission of odorant compounds 80%. Furthermore, other odorant species such as sulphur compounds
during SS biodrying. However, reaching thermophilic conditions during –dimethyl sulphide (DMS), dimethyl disulphide (DMDS) and dimethyl
the process, as well as in SS composting, is inevitable and needed to trisulphide (DMTS)–, ketones –mainly 2-butanone and 2-nonanone–
obtain a proper drying of the material. Maximum odour concentration and some alkanes and alkenes such as pentane or pentene appeared in
measured during SS biodrying was 3043 ou·m−3. As the process pro- different percentages. Generally, terpenes such as α-pinene, β-pinene or
ceeded, odour emissions decreased progressively down to low odour limonene may originate as intermediate products of aerobic biode-
concentrations between 275 and 290 ou·m−3. In this sense, few works gradation of organic matter. Besides, terpenes are also related to the PW
dealing with the OEFs of SS biological treatment have been found. used as bulking agent for the biodrying process (González et al., 2019b;
Rincón et al. (2019) evaluated the OEFs of different substrates in a 300 Schiavon et al., 2017). In the present work, its abundance was that high
L aerated pilot-scale reactor, reporting an OEF of 9.35E + 08 ou·Mg−1 probably due to the high SS:PW v/v ratio used. On the other hand,
DM0-SS and González et al. (2019b) obtained an OEF of 9.45E + 07 sulphur compounds are typical chemicals present in the gaseous emis-
ou·Mg−1 DM0-SS in a full-scale sewage sludge composting plant. sions generated during the SS treatment, which are normally formed
Nevertheless, some works have been conducted over different treat- and emitted during the first stages of the SS biological treatment (He
ment facilities to estimate their OEFs. Sironi et al. (2006) and Zarra et al., 2017; Schiavon et al., 2017). In the work presented herein, a 13%
et al. (2016) reported OEFs of 1.01E + 08 ou·Mg−1 of MSW and abundance of organosulphur compounds was found in the first sample,
4.15E + 06 ou·Mg−1 of MSW, respectively, from different MSW me- which coincide with the thermophilic phase of the biological process.
chanical-biological treatment plants. The obtained results in terms of Then, when the process fell into mesophilic temperature, the organo-
DM0 of biodryied mixture show that OEF referred to the SS biodrying sulphur compounds abundance decreased to 3%. Finally, some other
process are between one and two orders of magnitude below the OEFs odorant compounds typically found in the gaseous emissions generated
found in the few literature mentioned, what represents lower odour during the biological treatment of SS were found, such as ketones, al-
impact from this kind of technology. Even though these results are kanes or alkenes. Ketones were found at maximum abundance during
valuable information that can help to estimate odour emissions from the first stage of the SS biodrying (6.6% abundance), which was then
this biological process and the odour impact derived from similar reduced down to a 0.5% abundance during the mesophilic phase.
process, they must be carefully used when extrapolating into larger SS
biodrying treatment systems due to its dependence on different aspects 4. Conclusions
such as feedstock characteristics, operational parameters or plant ca-
pacity. Results indicated a proper performance of the SS biodrying process.
In summary, the main advantages that can be highlighted from SS The corresponding GHG and odorant emissions were accounted to be
biodrying over SS composting are that SS biodrying is a faster biological lower than that reported for conventional SS composting. GHG emis-
treatment that requires less space to treat the same flux of material, that sion factor and OEF referred to the bench-scale SS biodrying process
energy recovery is produced and that lower gaseous emissions are were 28.22 kg CO2eq·Mg−1 DM0-SS and 3.10E + 07 ou·Mg−1 DM0-SS,
generated. However, it can be a more expensive alternative than SS respectively. In conclusion, since there is no available scientific in-
composting due to the high aeration requirements. formation dealing with the gaseous emissions from SS biodrying to
compare with, this study shows a new insight into the gaseous

Fig. 3. Distribution of the different VOC families found in each sample, expressed in percentage of abundance respect the whole sample, from the outlet gases of the
biodrying reactor.

7
D. González, et al. Bioresource Technology 291 (2019) 121857

emissions generated during the SS biodrying process at bench-scale, He, P., Wei, S., Shao, L., Lü, F., 2017. Emission potential of volatile sulfur compounds
which will serve in further development of this treatment. (VSCs) and ammonia from sludge compost with different bio-stability under various
oxygen levels. Waste Manage. 73, 113–122.
Hort, C., Gracy, S., Platel, V., Moynault, L., 2009. Evaluation of sewage sludge and yard
Acknowledgements waste compost as a biofilter media for the removal of ammonia and volatile organic
sulfur compounds (VOSCs). Chem. Eng. J. 152, 44–53.
Huiliñir, C., Villegas, M., 2015. Simultaneous effect of initial moisture content and airflow
This study was carried out within the framework of the “SMART- rate on biodrying of sewage sludge. Water Res. 82, 118–128.
Plant” Innovation Action which has received funding from the IPCC, 2014. Climate Change 2014: Synthesis Report. Contribution of Working Groups I, II
European Union’s Horizon 2020 research and innovation programme and III to the Fifth Assessment Report of the Intergovernmental Panel on Climate
Change. IPCC, Geneva, Switzerland.
under grant agreement No. 690323. Johnson, M., 1997. Management of spent diatomaceous earth from brewing industry.
Kim, H., Hao, Z., Yang, B., Kim, S., Kwon, G., Jahng, D., 2018. Characterization and
Appendix A. Supplementary data treatment of emission gas condensate generated from biodrying of sewage sludge.
Environ. Eng. Sci. 35 ees.2017.0362.
Koppejan, J., van Loo, S., 2008. The Handbook of Biomass Combustion and Co-firing.
Supplementary data to this article can be found online at https:// Earthscan, London.
doi.org/10.1016/j.biortech.2019.121857. Maulini-Duran, C., Artola, A., Font, X., Sánchez, A., 2013. A systematic study of the
gaseous emissions from biosolids composting: raw sludge versus anaerobically di-
gested sludge. Bioresour. Technol. 147, 43–51.
References Moënne-Loccoz, P., Fee, J.A., 2010. Catalyzing NO to N2O in the nitrogen cycle. Science
330 (80), 10–11.
Adani, F., Baido, D., Calcaterra, E., Genevini, P., 2002. The influence of biomass tem- Pagans, E., Font, X., Sánchez, A., 2006. Emission of volatile organic compounds from
perature on biostabilization-biodrying of municipal solid waste. Bioresour. Technol. composting of different solid wastes: abatement by biofiltration. J. Hazard. Mater.
83, 173–179. https://doi.org/10.1016/S0960-8524(01)00231-0. 131, 179–186.
Ahn, H.K., Mulbry, W., White, J.W., Kondrad, S.L., 2011. Pile mixing increases green- Pan, J., Cai, H., Zhang, Z., Liu, H., Li, R., Mao, H., Awasthi, M.K., Wang, Q., Zhai, L., 2018.
house gas emissions during composting of dairy manure. Bioresour. Technol. 102, Comparative evaluation of the use of acidic additives on sewage sludge composting
2904–2909. quality improvement, nitrogen conservation, and greenhouse gas reduction.
Awasthi, M.K., Wang, Q., Chen, H., Wang, M., Awasthi, S.K., Ren, X., Cai, H., Li, R., Bioresour. Technol. 270, 467–475.
Zhang, Z., 2018. In-vessel co-composting of biosolid: focusing on mitigation of Pognani, M., Barrena, R., Font, X., Sánchez, A., 2012. A complete mass balance of a
greenhouse gases emissions and nutrients conservation. Renew. Energy 129, complex combined anaerobic/aerobic municipal source-separated waste treatment
814–823. plant. Waste Manage. 32, 799–805.
Cai, L., Chen, T., Gao, D., Zheng, G., Liu, H., 2013. Influence of forced air volume on Ponsá, S., Gea, T., Sánchez, A., 2010. Different indices to express biodegradability in
water evaporation during sewage sludge bio-drying. Water Res. 47, 4767–4773. organic solid wastes. J. Environ. Qual. 39, 706–712.
Capelli, L., Sironi, S., Del Rosso, R., Céntola, P., 2009. Predicting odour emissions from Ribes, A., Carrera, G., Gallego, E., Roca, X., Berenguer, M.J., Guardino, X., 2007.
wastewater treatment plants by means of odour emission factors. Water Res. 43, Development and validation of a method for air-quality and nuisance odors mon-
1977–1985. itoring of volatile organic compounds using multi-sorbent adsorption and gas chro-
Capelli, L., Sironi, S., Del Rosso, R., 2014. Odour emission factors: fundamental tools for matography/mass spectrometry thermal desorption system. J. Chromatogr. A 1140,
air quality management. Chem. Eng Trans. 40. 44–55.
Chen, J., Liu, H.-T., Lei, M., Chen, T.-B., Zheng, G.-D., Gao, D., Guo, S.-L., Cai, L., 2010. Rincón, C.A., De Guardia, A., Couvert, A., Le Roux, S., Soutrel, I., Daumoin, M., Benoist,
Reducing H2S production by O2 feedback control during large-scale sewage sludge J.C., 2019. Chemical and odor characterization of gas emissions released during
composting. Waste Manage. 31, 65–70. composting of solid wastes and digestates. J. Environ. Manage. 233, 39–53.
Chen, Y.C., Kuo, J., 2016. Potential of greenhouse gas emissions from sewage sludge Schiavon, M., Martini, L.M., Corrà, C., Scapinello, M., Coller, G., Tosi, P., Ragazzi, M.,
management: a case study of Taiwan. J. Clean. Prod. 129, 196–201. 2017. Characterisation of volatile organic compounds (VOCs) released by the com-
Choi, H.L., Sudiarto, S.I.A., Renggaman, A., 2014. Prediction of livestock manure and posting of different waste matrices. Environ. Pollut. 231, 845–853.
mixture higher heating value based on fundamental analysis. Fuel 116, 772–780. Shen, Y., Bin Chen, T., Gao, D., Zheng, G., Liu, H., Yang, Q., 2012. Online monitoring of
Colón, J., Cadena, E., Pognani, M., Barrena, R., Sánchez, A., Font, X., Artola, A., 2012. volatile organic compound production and emission during sewage sludge com-
Determination of the energy and environmental burdens associated with the biolo- posting. Bioresour. Technol. 123, 463–470.
gical treatment of source-separated Municipal Solid Wastes. Energy Environ. Sci. 5, Sironi, S., Capelli, L., Céntola, P., Del Rosso, R., Il Grande, M., 2006. Odour emission
5731–5741. factors for the prediction of odour emissions from plants for the mechanical and
Deviatkin, I., Lyu, L., Chen, S., Havukainen, J., Wang, F., Horttanainen, M., Mänttäri, M., biological treatment of MSW. Atmos. Environ. 40, 7632–7643.
2019. Technical implications and global warming potential of recovering nitrogen Tambone, F., Scaglia, B., Scotti, S., Adani, F., 2011. Effects of biodrying process on mu-
released during continuous thermal drying of sewage sludge. Waste Manage. 90, nicipal solid waste properties. Bioresour. Technol. 102, 7443–7450.
132–140. United States Environmental Protection Agency (USEPA), 1995. Compilation of air pol-
European Commission, 2014. http://ec.europa.eu/environment/waste/sludge/. [WWW lutant emission factors, AP-42, In: Stationary Point and Area Sources. vol. 1, fifth ed.,
Document]. Research Triangle Park, NC, USA.
Evangelou, A., Gerassimidou, S., Mavrakis, N., Komilis, D., 2016. Monitoring the per- US Dept. of Agriculture, US Composting Council, 2001. Test Methods for the Examination
formances of a real scale municipal solid waste composting and a biodrying facility of Composting and Compost Purpose. Edaphos International, Houston.
using respiration activity indices. Environ. Monit. Assess. 188. Villegas, M., Huiliñir, C., 2014. Biodrying of sewage sludge: kinetics of volatile solids
Frei, K.M., Cameron, D., Stuart, P.R., 2004. Novel drying process using forced aeration degradation under different initial moisture contents and air-flow rates. Bioresour.
through a porous biomass matrix. Dry. Technol. 22, 1191–1215. Technol. 174, 33–41.
Fukumoto, Y., Osada, T., Hanajima, D., Haga, K., 2003. Patterns and quantities of NH3, Water Environment Federation, 1995. Standard Methods for the Examination of Water
N2O and CH4 emissions during swine manure composting without forced aeration - and Wastewater.
Effect of compost pile scale. Bioresour. Technol. 89, 109–114. Wei, Y., Tong, J., Wang, Y., ChuLu, B., Yu, D., Sui, Q., Zhang, J., Chen, M., 2016. Who
German Institute for Standardisation, 2003. DIN 51900-3:2005. Testing of solid and li- contributes more to N2O emission during sludge bio-drying with two different
quid fuels – Determination of gross calorific value by the bomb calorimeter and aeration strategies, nitrifiers or denitrifiers? Appl. Microbiol. Biotechnol. 101,
calculation of net calorific value – Part 3: Method using the adiabatic jacket. 3393–3404.
Gomez-Rico, M.F., Fullana, A., Font, R., 2008. Volatile organic compounds released from Yuan, J., Chadwick, D., Zhang, D., Li, G., Chen, S., Luo, W., Du, L., He, S., Peng, S., 2016.
thermal drying of sewage sludge. WIT Trans. Ecol. Environ. 111, 425–433. Effects of aeration rate on maturity and gaseous emissions during sewage sludge
González, D., Colón, J., Gabriel, D., Sánchez, A., 2019a. The effect of the composting time composting. Waste Manage. 56, 403–410.
on the gaseous emissions and the compost stability in a full-scale sewage sludge Zarra, T., Naddeo, V., Oliva, G., Belgiorno, V., 2016. Odour emissions characterization for
composting plant. Sci. Total Environ. 654, 311–323. impact prediction in anaerobic-aerobic integrated treatment plants of municipal solid
González, D., Colón, J., Sánchez, A., Gabriel, D., 2019b. A systematic study on the VOCs waste. Chem. Eng. Trans. 54, 91–96.
characterization and odour emissions in a full-scale sewage sludge composting plant. Zhao, L., Gu, W.M., He, P.J., Shao, L.M., 2011. Biodegradation potential of bulking agents
J. Hazard. Mater. 373, 733–740. used in sludge bio-drying and their contribution to bio-generated heat. Water Res. 45,
Hao, Z., Yang, B., Jahng, D., 2018. Combustion characteristics of biodried sewage sludge. 2322–2330.
Waste Manage. 72, 296–305.

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