Accepted Manuscript

Application of hydrodynamic cavitation to improve the biodegradability of ma-

ture landfill leachate

M. Bis, A. Montusiewicz, J. Ozonek, S. Pasieczna-Patkowska

PII: S1350-4177(15)00053-X
DOI: http://dx.doi.org/10.1016/j.ultsonch.2015.03.003
Reference: ULTSON 2809

To appear in: Ultrasonics Sonochemistry

Received Date: 1 October 2014

Revised Date: 17 February 2015
Accepted Date: 2 March 2015

Please cite this article as: M. Bis, A. Montusiewicz, J. Ozonek, S. Pasieczna-Patkowska, Application of
hydrodynamic cavitation to improve the biodegradability of mature landfill leachate, Ultrasonics Sonochemistry
(2015), doi: http://dx.doi.org/10.1016/j.ultsonch.2015.03.003

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Application of hydrodynamic cavitation to improve the biodegradability of mature landfill
leachate

M. Bis a,*, A. Montusiewicz a, J. Ozonek a, S. Pasieczna-Patkowska b

a
Lublin University of Technology, Faculty of Environmental Engineering, 20-618 Lublin,
Nadbystrzycka St. 40 B, Poland
b
Maria Curie Skłodowska University, Department of Chemical Technology, Faculty of Chemistry, 3
Maria Curie-Sklodowska Square, 20-031 Lublin, Poland
*Corresponding author. Tel.: +48 81 538 47 82; fax: +48 81 538 19 97. E-mail address:
m.bis@wis.pol.lublin.pl (M. Bis).

Abstract
In this study, the application of hydrodynamic cavitation to improve the biodegradability of
mature landfill leachate was investigated. Three configurations of cavitation device were examined
and operational parameters of the process were selected. The study indicated that the orifice plate
with a 3/10 mm diameter conical concentric hole, characterized by the cavitation number of 0.033,
is a reasonable choice to ensure the enhanced biodegradability of mature leachate. Using such a
configuration and maintaining 30 recirculation passes through the cavitation zone at inlet pressure
of 7 bar, the highest increase of biodegradability index (BI) of approximately 22% occurred, i.e.,
from the value of 0.046 to 0.056. The FT-IR/PAS analysis confirmed a degradation of refractory
compounds that typically prevail in mature leachate.
An evaluation of energy efficiency was made in terms of the actual consumed energy
measured by using the Kyoritsu KEW6310 Power Quality Tester. A cavitational yield of 9.8 mg
COD kJ-1 was obtained for the optimum configuration and 30 recirculation passes. Regarding
energy efficiency, the application of 10 cavitation cycles appeared to be the most profitable. This
was due to an almost threefold higher cavitational yield of 27.5 mg COD kJ-1. However, the
preferable option should be selected by considering a satisfactory effect in the biodegradability
enhancement.

Keywords
Hydrodynamic cavitation; Mature landfill leachate; Leachate pretreatment; Advanced oxidation
processes; Enhanced biodegradability

1. Introduction
Landfill leachate is a highly contaminated liquid created by the degradation of disposed
waste, in combination with rainwater percolating through the refuse layers. It varies hugely with
regard to amount and composition, significantly depending on numerous factors. The major
determinants involve landfill technology, morphology and the type of waste gathered, compaction
of refuse layers, seasonal weather variation, hydrogeology, site operations and management, as well
as landfill age with the corresponding refuse decomposition stage [1,2]. According to the latter,
three types of leachate have been distinguished: young, intermediate and mature. Each of these are
different in composition and biodegradability.
With an increase in landfill age, there is a change in the main contribution of the organic
compounds due to the degradation of volatile fatty acids that typically prevail in leachate, generated
in less stabilized items. Thus, for the mature ones, the more stable refractory compounds with high
molecular weights, such as humic and fulvic substances, tend to prevail. In this case, the leachate
1
biodegradability significantly decreases [3]. Generally, mature leachate is characterized by a
moderately high strength of COD (<4000 mg/L). Furthermore, it has a concentration of ammonium
nitrogen that exceeds 400 mg/L, with extremely high values of 3000–5000 mg/L [4,5]. The
BOD5/COD ratio, considered to be a measure of biodegradability and known as biodegradability
index (BI) [6], usually reaches the level below 0.1 [5]. Some researchers also suggest that the
complexity of components, as well as the molecular size of the dissolved organic matter, increase
according to landfill age. Thus, the mature leachate has a wider range of molecular weight with a
high molecular weight fraction [7,8]. According to Huo et al. [8], the increment in the landfill age
favors aromatic polycondensation and increases the level of conjugated chromophores, as well as
the degree of humification of dissolved organic matter. In mature leachate, these scientists found a
44% concentration of humic acids, approximately 51% content of fulvic acids and 7% hydrophilic
fractions of dissolved organic matter. At the same time, the contents of the young leachate were
reported as follows: 0.4%, 23.6% and 76%.
Recently, the presence of humic substances in leachate has gained special attention [9].
Humic substances are natural organic matter made up of complex structures of polymerized organic
acids, carboxylic acids and carbohydrates with molecular masses, ranging from several hundreds to
tens of thousands [10,11]. They represent the non-biodegradable fraction of COD and show
recalcitrant properties. Due to their structural complexity, humic substances affect the behavior of
some pollutants in natural environments, for example trace metal speciation and toxicity [7]. Zhao
et al. [9] reported that such substances diminish the effect of UV radiation due to UV light
absorption. At present, there are several methods that are used to remove humic substances. These
include coagulation-flocculation, electro-coagulation, oxidation and membrane technology
[12,13,14,15]. However, none of these are considered to be commercially profitable due to their
unrealistically high costs [16].
Generally, the unique characteristics of mature landfill leachate demand individual selection
of various – frequently combined – biological and physicochemical pre- or post-treatments
[1,17,18]. Among the physicochemical methods, advanced oxidation processes (AOPs) have
recently been revealed as an effective technology in improving the biodegradability of leachate
[2,4,19]. According to Vilar et al. [20,21], favorable results can be achieved by using solar photo-
Fenton oxidation. Likewise, de Morais and Zamora [22] noted that the ultraviolet light / hydrogen
peroxide and photo-Fenton pretreatment lasting 60 minutes was an efficient method to enhance the
BOD5/COD value from 0.13 to circa 0.4. These results were consistent with Bila et al.’s study [23]
which involved the ozonation of leachate followed by a biological process. The researchers reported
the increment in BOD5/COD value from 0.05 to approximately 0.3. They noted that, even though
the BOD5/COD ratio was adequate for biological treatment, the process did not have a good
performance. This was most likely due to the high toxicity associated with the high ammonia
concentration.
Among many investigated AOPs, cavitation has been found to effectively destruct complex
organic chemicals. In recent decades, increasing attention has been devoted to investigating this
phenomenon as a tool of disinfection [24,25,26,27,28], cell disruption [29,30] and degradation of
various organic compounds, e.g., pharmaceutical residues [31,32], phenols [33], pesticides [34],
insecticides [35] and textile dyes [36,37]. However, most studies mainly addressed the process with
regard to the synthetic wastewater containing only specific pollutants. Moreover, it is generally
accepted that sole cavitation cannot be recognized as an efficient and cost-effective technique for
wastewater treatment [38]. Thus, this phenomenon has often been studied in conjunction with other
AOPs, i.e., processes incorporating Fenton reagent, hydrogen peroxide or carbon tetrachloride
[32,39,40,41,42]. Interestingly, different chemical and physical mechanisms of pollutant
degradation via cavitation have been proposed: thermal decomposition, shockwaves, shear forces,
pressure gradient and the reaction of •OH radicals with the pollutant [6,26].
With regard to the application of the cavitation phenomenon, the focus of previous studies
has rarely been on biodegradability enhancement. Until now, the subject area has only been studied
by Padoley et al. [6], focusing on pretreatment of distillery wastewater with the use of
2
hydrodynamic cavitation, and by Sangave and Pandit [43], who employed ultrasounds for the same
purpose. Other reports have not been found. It is particularly worthwhile to investigate the practical
aspects of the phenomenon applied to enhance the biodegradability of mature landfill leachate rich
in recalcitrant organic compounds (i.e., humic substances). This would allow to evaluate the
possibility of subsequently using the biological treatment methods.
The present study examined the advisability of the application of hydrodynamic cavitation
as a pretreatment technique for improving the biodegradability of mature landfill leachate. The
effect of the constriction geometry on the cavitational results was investigated using three
configurations of the cavitation device. The operational parameters were selected and discussed.
The results of the study were evaluated in terms of leachate biodegradability enhancement, as well
as cavitational yields. The evaluation of energy efficiency was made on the basis of measuring the
actual energy consumed.

2. Materials and methods

2.1. Materials
Leachate was sourced from the Rokitno (Lublin, Poland) municipal solid waste landfill of
over 15 years of age. The leachate was considered as the mature one. It was sampled eightfold, with
an average collected sample of 90 L, taken from a storage tank and transported immediately (within
one hour) to the laboratory using plastic containers. The content analysis was carried out upon
delivery. The leachate composition is presented in Table 1 and discussed in Section 3.1.
<Table 1>
2.2 Experimental set-up
The laboratory closed-loop installation consisted of a cavitation reactor – connected via
pipes to the circulation tank – and a centrifugal pump (maximum operating pressure 16 bar, 1000-
3000 revolutions per minute, power rating 2.2 kW), which generated pressure in the system (Fig. 1).
The reactor was composed of a cavitation inducer (replaceable orifice plate) housed by two flanges
bolted together. It also had a transparent organic glass tube (of methyl polymethacrylate), allowing
the observation of the cavitation phenomenon. The experimental set-up was equipped with control
valves and a measuring system consisting of Keller PR-33X piezoelectric pressure gauges with a 1
mbar resolution. These were connected to a digital data measurement/acquisition system and a
M1500 AA electromagnetic flow meter (Badger Meter Inc.) with the resolution of 0.05 L min-1. The
valves were located at appropriate places to manipulate and maintain the required flow rate in the
installation. The pump output was controlled by a thyristor regulator, allowing the speed of the
electric motor to be varied. The inlet pressure p1 was determined using a manometer. The Keller
pressure gauges measured the fully recovered downstream pressure p2 required for calculation of
the cavitation number (Cv). The temperature was measured using a thermocouple. The entire set-up
consisted of stainless steel pipelines with the inside diameter of 28.76 mm.
Cavitation constrictions used in the experiments were steel orifice plates of 64 mm external
diameter and 10 mm thickness, drilled with holes and mounted in the body of the cavitation reactor.
Three configurations were investigated (Fig. 1):
• Constriction A – orifice plate with a 3/10 mm diameter conical bore located on its axis
(concentric hole),
• Constriction B – orifice plate with 5 holes of rectangular cross-section (1 mm x 5 mm),
• Constriction C – orifice plate with 9 cylindrical holes with diameter of 1 mm, one located on
the axis and the remainder evenly spaced around the disk half-way out to the circumference.

<Fig. 1>

3
 The specified plates were chosen on the basis of different geometry and variable hydrodynamic
flow conditions. Although A and C represented the same total hole areas, the first one had only one
hole. Additionally, it was similar to the circular Venturi tube in respect of the hydrodynamic flow
conditions, the stream shape with a long divergence zone and the boundary stationary vortices
creating the stream constriction zone beyond the orifice. The B and C constrictions differed in terms
of the flow surface and hole shapes. According to Balasundaram and Harrison [30], the circular
shape of holes should be used over others. This is because it assures the higher number of orifices
for a given flow area.
Table 2 presents the detailed hydraulic characteristics of the constrictions. These are located and
discussed in Section 3.2.
2.3 Experimental methodology
Hydrodynamic cavitation was studied as a leachate pretreatment aimed to enhance its
biodegradability. The experiments were carried out at the pressure of 7 bar which was maintained
every time in the inlet zone of the cavitation device (on the manometer denoted as p1 in Fig. 1).
According to the authors’ previous study [44], such a value was found to be the most profitable for
achieving a maximal cavitation efficiency in the system under investigation. The required pressure
was assured by adjusting pump rotating speed. The leachate subjected to cavitation was driven by a
pump from a circulation tank (with a volume of 30 L) to the cavitation reactor and then returned to
the circulation unit. Cavitation experiments were carried out fivefold for each investigated plate (A,
B and C). This was to avoid random errors and verify the repeatability of the results achieved.
However, some data had to be eliminated because of measurement errors. Thus, three replications
were finally considered. It was assumed that, for each experiment, the same number of cycles
(passes) should be operationally ensured, allowing the comparison of the obtained results. On the
other hand, in order to minimize the energy consumption costs, there was another condition, namely
the number of passes that ensured the operation time below 33 minutes. Consequently, in the
experiment using constriction C, a threefold decrease of the number of cavitation cycles was
required compared to A and B (as primary tests showed). It should be noted that the number of
liquid passes through cavitation constriction was defined as volumetric flow rate (Q0) multiplied by
time of operation (t) per total volume of leachate in the circulation tank (V).
After choosing the most efficient configuration of the orifice (based on an increment in the
BOD5/COD ratio), the biodegradability studies were continued with the examination of the
DOC/TOC ratio, as well as the changes of organic matter using FT-IR analysis. For these cavitation
experiments, the leachate was sampled threefold to ensure the measurements in triplicate.
Raw leachate was sampled according to the procedure reported in Section 2.1. Throughout
cavitation, the samples were collected using an assumed schedule based on the time-dependent
intervals (appointed periods), conformed to the number of passes: 2, 5, 10 and 30, respectively.
The following parameters were analyzed in raw and cavitated leachate: total chemical
oxygen demand (COD), biochemical oxygen demand (BOD5), volatile fatty acids (VFA), total
organic carbon (TOC), total solids (TS), volatile solids (VS), alkalinity and pH level. The same
schedule was used for determining the values of the parameters that characterized the leachate
supernatant. These parameters included dissolved organic carbon (DOC), ammonium nitrogen (N-
NH4 +), nitrite and nitrate nitrogen (N-NOx-) and ortho-phosphate phosphorus (P-PO43-). The
supernatant samples were obtained by filtering through a 0.45µm pore-size filter. All analytical
determinations were performed in three replicates for each plot.
Most analyses were carried out in accordance with the procedures listed in the Polish
Standards Methods (BOD5, TS, VS, alkalinity and pH). Some analyses were performed with a
FIASTAR 5000, using FOSS analytical methods (N-NH4+, N-NOx-, P-PO43-). Ammonium was
determined according to ISO 11732, nitrite and nitrate according to ISO 13395 and ortho-phosphate
in accordance with ISO/FDIS 15681-1. The COD and VFA were measured with the HACH DR
3900 spectrophotometer. The TOC and DOC were determined using the Shimadzu TOC-5050A
total organic carbon analyzer according to PN-EN 1484:1999. The pH value was determined using
4
an electronic pH meter.
Preparing samples for the Fourier transport infrared spectroscopy analysis (FT-IR) required
leachate (both raw and cavitated) to be formerly dried using sublimation (lyophilized). The samples
with a volume of 50 mL were frozen at -25ºC in the laboratory freezer and then dried at a
temperature of -56ºC by the freeze dryer Alpha 1-4.
FT-IR/PAS spectra of lyophilized leachate, both raw and cavitated (i.e., before and after
cavitation), were recorded by means of a Bio-Rad Excalibur 3000 MX spectrometer equipped with
a photoacoustic detector MTEC 300 (in helium atmosphere in the detector) at RT over the 4000-
400 cm−1 range at the resolution of 4 cm−1 and maximum source aperture. The spectra were
normalized by computing the ratio of a sample spectrum to the spectrum of a MTEC carbon black
standard. A stainless steel cup (internal diameter of 10 mm) was filled with a sample (thickness of
<6 mm). Before each data collection, the photoacoustic cell was purged with dry helium for
five minutes. Interferograms of 1024 scans were averaged for each spectrum.
Power quality analysis and power consumption of the set-up was measured using a Kyoritsu
KEW6310 Power Quality Tester. The measurements were carried out in the inlet pressure which
was consecutively increased from 1 to 7 bar. The evaluation of the energy efficiency was made on
the basis of the cavitational yield given at the pressure of 7 bar, maintained for the experiments in
the inlet zone of the cavitation device.
The obtained data were graphed using Microsoft Excel 2010. Statistical analysis was
performed using repeated measures ANOVA (Tukey’s test was applied) and the t-student test with
Statsoft Statistica software (version 10). The differences were considered statistically significant at
p-values less than 0.05.

3. Results and discussion

3.1. Leachate characteristics
According to Jördening and Winter [45], three characteristic phases of degradation were
defined for landfills. These are different in respect of the various parameters. On the basis that the
BOD5/COD ratio was below 0.2, the methanogenic phase was confirmed. Taking into account the
values of both the organic (COD, TOC, DOC and VFA) and inorganic leachate parameters (Table 1
in Section 2.1), Rokitno’s leachate can be considered as the mature one and originated most
probably from a landfill operating at the methanogenic phase. This was indicated by a comparison
of the values of its constituents, with the average data quoted by Li et al. [4] for the stage
mentioned. The leachate had a high concentration of recalcitrant organic matter (indicated as COD)
and low biodegradability (BOD5/COD ratio below 0.1).

3.2. Selection of the orifice plate based on the hydrodynamic cavitation parameters
Initially, the geometry of the constrictions used in the experiments was analyzed. In order to
allow direct comparison of the various orifice shapes, α and β0 parameters, the leachate velocity (at
assumed inlet pressure value) and the cavitation number (Cv) were determined [46,47,48]. The
details of the constriction characteristics are presented in Table 2.
<Table 2>
Estimation of the results of mature leachate cavitation using different constrictions was
made on the basis that both COD and biodegradability change. The cavitation efficiency achieved
for the orifice plates with different combinations of number and dimensions of holes is presented in
Fig. 2.
<Fig.2>
The constrictions under investigation had different geometries. It should be noted that the
authors evaluated the usefulness of constrictions at the same inlet pressure, although at a variable

5
energy consumption level due to the different head pressure losses. This was particularly important,
taking into account the practical applications. According to this, using a given plate imposed
stability on the cavitational parameters such as α, β0, orifice velocity, Cv and made the type of plate a
variable in characterizing cavitation effects. Another variable was the number of leachate
recirculation passes through the cavitation zone (i.e., the number of cavitation cycles).
In the investigations, a comparable – although small (only a few percent) – removal
efficiency of the organic compounds (expressed as COD) was achieved for all plates when the same
number of cavitation cycles was analyzed (10) (Fig. 2a, 2b, 2c). An analogous tendency appeared in
the comparison of plates A and B for 30 recirculation passes. It is known that the higher the
pollutant concentration, the lower the efficiency of degradation. A highly-loaded leachate, rich in
recalcitrant compounds, could be expected to limit the cavitation efficiency. Interestingly, the
differences observed between the average value of COD, before and after cavitation, were validated
as statistically significant (using ANOVA and Tukey’s test, α=0.05) for each type of plate. This
finding indicates that COD removal efficiency does not depend on the configuration applied.
Considering the increases in the BOD5/COD ratio (BI) resulting from cavitation, the most beneficial
change (about 22%) was observed in constriction A. Here, there was one orifice and an attainment
of 30 recirculation passes (Fig. 2d). In alternative cases, there was not a sufficiently high increment
in the biodegradability index (Fig. 2e, 2f). Using ANOVA and comparing plates A and B for the
same number of passes (up to 30), it was validated that the type of plate significantly differentiated
the BI improvement via cavitation. On the contrary, analyzing the A, B and C configurations for a
lower number of cavitation cycles (up to 10) indicated a lack of such differentiation.
Considering another variable (the number of cavitation cycles), regardless of the type of
constriction investigated, a statistically significant drop in COD was observed within the initial
period of cavitation, i.e., when two passes succeeded (Fig. 2). The corresponding duration was
approximately 2.0, 1.5 and 6.5 minutes, respectively for A, B and C plates. Subsequent
enhancement of COD removal, accompanying the consecutive passes, was slight and with no
statistical significance (Tukey’s test with α=0.05 showed that the average COD values did not differ
for 2, 5, 10 and 30 cycles). A similar tendency occurred for each type of configuration regarding the
average value of BI, which increased to the greatest extent involving two initial passes. The
increments in the BOD5/COD ratio via cavitation were validated as statistically significant for all
plates when 2, 5 and 10 recirculation passes were carried out. Comparing the BI values after
cavitation, such differences did not occur. In contrast, the results for plate A and B, that operated in
the range of 0 to 30 cycles, differed significantly. Configuration A ensured a significant increase in
BI – not only via cavitation, but also by extending the number of passes from 2 and 5 to 30. The
results for plate B were worse and statistically invariable. The most beneficial increment in BI was
achieved using plate A and maintaining 30 passes through the cavitation zone (during
approximately 28 minutes). Given such a number of cavitation cycles and a sufficient residence
time within the cavitation zone (ensured by the smooth, long divergence beyond the constriction
and larger time scales than for the multi-orifice plates), the BOD5/COD ratio raised from 0.046 to
0.056. Fewer passes (namely, 10) with the responding duration of 9.5 minutes led to a lower BI
enhancement of 17.4%. Interestingly, similar conditions were selected by de Morais and Zamora
[22] in their optimization of the UV/H2O2 system which was applied to mature leachate treatment.
These researchers found that, at the natural pH of the leachate (amounting to 8.4), the largest
degradation gradient occurred between 0 and 30 minutes.
According to the data given, the type of configuration (i.e., geometrical parameters, orifice
velocity and cavitation numbers), together with the number of cavitation cycles, was found to
influence the biodegradability improvement. Furthermore, plate A was justified to be a preferable
option. Considering the α parameter, this plate (having one concentric hole) demonstrated the
lowest value compared to the others (Table 2). Generally, a higher number of orifices produces
more jet streams. This results in greater cavitation effects in systems with constant cavitation
intensity. However, in the present study cavitation intensity differed for a given inlet pressure.
Interestingly, the best results were related to the constriction that imposed the highest orifice
6
velocity (almost three times greater than for plates B and C). The findings were consistent with the
research of Franke et al. [49], who noted optimal chloroform decomposition through an orifice plate
with 2.8 mm in diameter. This is quite similar to plate A used in the present study. Regarding the β0
parameter, plate A demonstrated analogous quantity as plate C (having the same flow area), while
plate B had an almost 3.5 times higher value (Table 2). Since, as is known, a lower β0 favors the
cavitational efficiency and yield, the poorer results reported for plate B were not surprising. The
highest BI increments achieved for plate A could be attributed to the concentric position of the hole
(i.e., the grade of displacement of the hole from the plate’s center δ=0). According to Braeutigam et
al. [50], such a localization of the orifice substantially influenced the results. This is because it
affected both the flow and the collapse conditions, favoring a higher turbulence intensity and a large
shear layer area with significant velocity gradient. Moreover, Basiri Parsa and Ebrahimzadeh
Zonouzian [51] noticed that increasing the orifice radius in constant flow area led to a greater
collapse in pressure and a subsequent increase in the cavitation efficiency. Importantly, Gogate and
Pandit [52] suggested that, depending on the application, the diameter of the constriction needs to
be optimized. This recommendation concerned higher diameters for applications which require
intense cavitation (an increase of biodegradability could be included among them) and lower
diameters with larger number of holes for applications with reduced intensity. It is worth noting that
plate A demonstrated quite a different geometry (hydrodynamically similar to the circular Venturi
tube). Thus, it had different hydrodynamic conditions compared to constrictions B and C.
According to the research of Arrojo et al. [26], the Venturi tube tended to give denser cavitation
clouds due to the increasing available time for bubble growth. This resulted in larger cavities and
more cavitation events per unit time. The hydrodynamic conditions inside the cavitation device
involving plate A were characterized by the lowest cavitation number. In keeping with this, cavity
clusters grew bigger and the length of the cavitation zone extended from the restriction. As a result,
larger cavitation clusters developed and collapse pressure increased [36,53]. The results were
consistent with the research of Saharan et al. [54], who noted that the total effect of hydrodynamic
cavitation on degradation of the organic pollutants depends on the maximum size attained by a
bubble cavity before its collapse and the rate of pressure recovery. Interestingly, Raut-Jadhav et al.
[35] found that the most efficient degradation of imidacloprid (insecticide) responding to the
cavitation number of 0.067 (with an order of magnitude similar to that reported in the present study)
was observed while examining the circular Venturi tube at an inlet pressure of 15 bar.
The results obtained in the present study indicated that mechanisms leading to cavitation
effects most likely varied for the different plates. Regarding configuration A, the enhanced
biodegradability of mature leachate seemed to be attributed to the physical, rather than chemical
effects. Such a configuration promoted bubble growth, fast pressure recovery and higher cavitation
intensity. At the same time, the reaction of •OH radicals with the pollutant was of less importance
[26]. High leachate alkalinity can also limit the latter, since carbonates and bicarbonates tend to
inhibit the formation of •OH radicals. A consequent increase of BOD5 from 282 to 319 g m-3,
concomitant with a drop of COD (from 6097 to 5718 g m-3), was observed for a specified number
of leachate recirculation passes. This confirmed that, for plate A, the oxidation of biodegradable
organic compounds releasing as products of the decomposition of recalcitrant organic matter was
probably limited. In the case of plates B and C, chemical effects appeared to be of greater
significance. This is because smaller bubbles and faster collapses (related to their geometry) favor
diffusion of •OH radicals. The BOD5 value that decreased (for plate B) or negligibly increased (for
plate C), concomitantly with a decrease of COD, confirm the more efficient oxidation of
biodegradable organic compounds via cavitation.
In conclusion, the orifice plate A, with a 3/10 mm diameter concentric hole and
characterized by the lowest cavitation number of 0.033, proved to be a justified choice to ensure the
enhanced biodegradability index of mature leachate under specified conditions.

7
3.3. Biodegradability improvement
The study indicated that using plate A and maintaining 30 recirculation passes through
cavitation zone at inlet pressure of 7 bar (for 28 minutes) led to a significant increase of mature
leachate BI from 0.046 to 0.056. Repeating the experiments three times and comparing the values
before and after cavitation produced a linear relationship, according to the equation y = 1.0126x +
0.0062 (R2 = 0.9358). Supplementary confirmation of the enhanced leachate biodegradability was
evaluated on the basis of DOC/TOC changes. Similarly to BI, a linear relationship existed, given by
equation y = 0.7219x + 0.3027, although a stronger correlation of the variables was achieved (R2 =
0.996). According to the function, an increment in the concentration of dissolved organic carbon,
through cavitation, was found. This indicated the degradation of complex organic compounds,
demonstrated by a rise in DOC/TOC ratio with a significant difference (between raw and cavitated
leachate). This was recognized on the basis of the t-test for dependent variables (p = 0.006979, t = -
11.9078). The results suggested that hydrodynamic cavitation could rearrange the molecular
structures of organic matter and convert the non-biodegradable organic compounds (typically
present in mature leachate) to more biodegradable forms. This was consistent with the studies of
other researchers, who reported advanced oxidation methods that were capable of generating more
biodegradable products, mainly acids [55] and transform organic recalcitrant substances into easily
biodegradable compounds, thus improving the efficiency and reducing the cost of further biological
steps [22].
Additionally, to provide insight into the changes of organic matter in mature leachate,
Fourier transform infrared spectra (FT-IR) analysis was conducted. This is commonly known to
identify functional groups by measuring the vibrational frequencies of molecules scanned with
infrared light. Remarkably, the main sample handling problem in the FT-IR analysis of solid
materials is that nearly all of them are too opaque in their normal forms for direct transmission
analysis in the mid-IR spectral region. One of the major disadvantages of the transmission method
is the necessity of preparing the pellet from a mixture of tested material and the compound
transparent to IR radiation (usually potassium bromide), serving also as a matrix. Application of
KBr pelleting may cause deformation and, consequently, the wrong interpretation of the spectrum.
Another disadvantage of the transmission method is the hygroscopicity of potassium bromide. The
adsorbed water is visible in the IR spectrum at ~3500 and ~1630 cm-1 and these bands are intense
enough to be able to cover bands derived from the sample. The most broadly applicable mid-IR
solution to the opacity and water influence is photoacoustic spectroscopy (FT-IR/PAS) [56]. This
technique is non-destructive and can be used in the analysis of materials which are difficult to
homogenize, or else the structure or the chemical composition change during the grinding. FT-
IR/PAS allows a spectrum of the sample to be obtained without previous preparation. FT-IR/PAS
spectra analysis results of leachate before and after cavitation are shown in Fig. 3 (4000-2400 cm-1
range) and Fig. 4 (2000-600 cm-1 range). Spectra in the 4000-2400 cm-1 range (Fig. 3) had
absorbance bands with maxima at ~3416 cm-1 (O-H stretching of hydroxyl groups from hydrogen
bonding and N-H asymmetric stretching of peptide groups), 3190 cm-1 (H-bonded O-H in COOH
groups and N-H symmetric stretching of peptide groups) and 3075 cm-1 (=C-H in aromatic
structures). They also showed an absorbance band at 2950-2850 cm-1 (aliphatic C-H stretching)
[57]. For the leachate sample after cavitation, all those bands had a lower intensity than for the
sample before it.
Within the 2000-600 cm-1 range (Fig. 4) several bands indicated the presence of carboxylic
compounds and amino acids: 1845, 1695 cm-1 (C=O stretching), 1662 cm-1 (C=O stretching of
amide groups), the bands within 1620-1580 cm-1 (amide groups and aromatic C=C conjugated with
C=O of COO-), 1331-1321 cm-1 (COO-), 934 cm-1 (H-bonded out-of-plane bending of C=O in
COOH). There were also bands indicating the presence of aromatic compounds: 1562, 1500 cm-1
(C=C in aromatic rings, N-H), 1476 cm-1 (C=C, C-H and N-H), 870-700 cm-1 (aromatic =C-H out
of plane deformation vibrations) [58,59,60]. The band at ~1911 cm-1 was the overtone and
combination band due to the C-H out of plane deformation vibrations of aromatic rings [57]. All the

8
above-mentioned bands indicated the existence of humic and fulvic acids in mature leachate. These
bands had lower intensity in the case of the cavitated sample relative to the sample before
cavitation. The decomposition of acid groups could also be confirmed by the pH changes through
the cavitation. The pH of the raw leachate was 8.08 and via cavitation it increased to 8.44.
<Fig. 3>
<Fig. 4>
Some bands within the 1120-990 cm-1 and 870-700 cm-1 range also indicated the presence of
inorganic compounds, namely silica, carbonates, phosphates and nitrates (1121, 1082, 1045, 1032,
994, 833, 705 cm-1) [60,61]. The intensity of these bands remained almost unchanged both for the
samples before and after the cavitation, despite the fact that the intensity of the other bands,
indicating the presence of organic compounds, decreased. The drop in the intensity of bands
indicating the presence of oxygen, peptide groups and aromatic rings in the IR spectrum of leachate
after cavitation (Fig. 3 and Fig. 4) could be considered as evidence of the reduction in the number of
compounds containing these functional groups, and thus a positive effect of cavitation on
decomposition of organic matter in the leachate.

3.4. Evaluation of energy efficiency

Energy efficiency was analyzed by calculating the cavitational yield for the examined
configurations. The quantity was evaluated in terms of the amount of COD removed per total
energy supplied. In order to determine the energy consumption of the three-phase pump that was
applied in the study, the actual consumed energy was measured.
The comparison of the electrical power consumption, energy efficiency and power density in
the pressure ranging from 1 to 7 bar is summarized in Table 3. According to the data given, plate A
was found to have the lowest power consumption in comparison to the other plates. Additionally,
similar values initially achieved for plates A (172.5 J s-1) and C (203 J s-1) at 1 bar inlet pressure
became significantly different when the pressure increased. The value raised much faster for plate C
than A, achieving at 7 bar inlet pressure sequential values of 1500 and 690 J s-1. This is due to the
much higher pressure resulting from the leachate passing through plate C.
<Table 3>
The cavitational yields determined for each experiment, assuming an inlet pressure of 7 bar,
are given in Table 4. The calculations were carried out for 10 and 30 recirculation passes. Due to the
longest time of the 30 cavitation cycles, in the case of plate C (98 min 54 s) compared to plate A (28
min 12 s) and B (23 min 32 s), the total energy supplied to the system had the greatest value (8901
kJ). In terms of energy efficiency within 30 cavitation passes, plate A consumed over three times
less energy than plate B and over seven times than plate C. Furthermore, the first constriction
demonstrated the highest biodegradability improvement relative to the other plates. It can be
established that within 30 passes, plate A showed a four times higher cavitational yield in
comparison to plate B (for plate C, the quantity could not be calculated because of the lack of COD
data). During the 10 cavitation cycles, the same trend appeared. The cavitational yield determined
for plate A was almost four times higher compared to plate B and exceeded the values achieved for
plate C as many as eight times. Interestingly, the obtained values coincided with those reported by
Badve et al. [62] for 20 minutes of hydrodynamic cavitation for wastewater in the wood finishing
industry. Additionally, in the present study the quantity within 10 passes was found to be much
higher when compared to the cavitational yield of 30 passes. Hence, with regard to energy
efficiency, the application of 10 cavitation cycles was more profitable. On the contrary, the
biodegradability index enhanced to a lesser extent of 17.4%, whereas 30 cavitation cycles allowed a
BI increase of 21.7%. The practical application of 10 or 30 passes should be experimentally proven.
This is because the use of only 10 cavitation passes is insufficient to obtain a satisfactory effect in
the further process of biological leachate treatment. Thus, the application of 30 cavitation passes is
a preferable option.
9
 <Table 4>

4. Conclusions
The study indicated the orifice plate, with a 3/10 mm diameter conical concentric hole
(hydrodynamically similar to the circular Ventouri tube) and characterized by the lowest cavitation
number of 0.033, to be the most favorable for ensuring the enhanced biodegradability index of
mature leachate. Using this configuration and maintaining 30 recirculation passes through the
cavitation zone at inlet pressure of 7 bar, the highest increase of biodegradability index (BI) of
approximately 22% occurred, i.e., from the value of 0.046 to 0.056. The results of the FT-IR/PAS
analysis suggested a possible decomposition of complex high-molecular weight compounds to the
more biodegradable substances. The effects were attributed to the physical rather than the chemical
mechanisms of cavitation.
The evaluation of energy efficiency showed the highest cavitational yields for the
configuration previously chosen (the plate with a 3/10 mm diameter concentric hole). The value
determined on the basis of the amount of COD removed per total energy supplied for 30
recirculation passes was 9.8 mg kJ-1. With regard to energy efficiency, the application of 10
cavitation cycles appeared to be more profitable. This was due to a significantly higher cavitational
yield of 27.5 mg COD kJ-1. For the final decision, the preferable option should be selected primarily
considering a satisfactory effect in the biodegradability enhancement. Thus, the practical application
of the number of passes should be proven experimentally.

Acknowledgements
Authors would like to acknowledge the financial support of the Polish Ministry of Science and
Higher Education research grant No 7514/B/T02/2011/40. Dr Dariusz Majerek and Dr Marcin
Widomski are greatly appreciated for their valuable statistical support. Special acknowledgements
go to Mr Marcin Depta and Mr Janusz Urbański for their technical assistance during the course of
this research.

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Figure captions

Fig. 1. Scheme of experimental set-up (cavitation loop) and orifice plate configurations (units given
in mm): 1 – circulation tank, 2 – centrifugal pump WILO MVIE, 3 – electromagnetic flow meter, 4
– manometer, 5 – hydrodynamic cavitation reactor, 6 – valve, 7 – piezoelectric pressure gauges, 8 –
computer control

Fig. 2. Changes in COD and BOD5/COD ratio with the number of cavitation cycles for three
cavitating constrictions at 7 bar inlet pressure (the mean values are given, error bars represent
standard deviation)

Fig. 3. FT-IR/PAS spectra of leachate before and after cavitation (4000-2400 cm-1 range)

Fig. 4. FT-IR/PAS spectra of leachate before and after cavitation (2000-600 cm-1 range)

14
Table 1. The characteristics of leachate samples
Average value
Parameter Unit Minimum Maximum
± standard deviation
-1
Total chemical oxygen demand (COD) mg L 6051 ± 71 5498 6530
Biochemical oxygen demand (BOD5 ) mg L-1 277 ± 89 126 428
BOD5/COD – 0.046 ± 0.014 0.022 0.069
Total organic carbon (TOC) mg L-1 1792 ±158 1657 1937
Dissolved organic carbon (DOC) mg L-1 1594 ± 75 1517 1666
pH – 8.08 ± 0,2 8.02 8.18
Alkalinity mg L-1 16094 ± 232 15500 16750
Volatile fatty acids (VFA) mg L-1 1164 ± 28 1066 1348
Total solids (TS) g kg-1 15.5 ± 0.2 14.9 16.2
Volatile solids (VS) g kg-1 2.8 ± 0.2 1.5 3.4
Ammonium nitrogen (N-NH4+) mg L-1 2069 ± 815 1390 2973
Ortho-phosphate phosphorus (P-PO43-) mg L-1 26 ± 15.9 6.2 39.2

15
Table 2. The hydraulic characteristics of orifice plates used in the experiments
Parameter Unit A B C
Number of holes – 1 5 9
Diameter/Linear dimensions of holes mm 3 5x1 1
Total area of holes mm2 7.0686 25 7.0686
Cv cavitation number of orifice plate – 0.0330 0.2976 0.3852
α mm-1 1.333 2.4 4.0
β0 – 0.0023 0.0082 0.0023
Total perimeter of holes mm 9.42 60 28.26
Orifice velocity m s-1 75.44 25.73 21.46
Flow rate L s-1 0.5333 0.6433 0.1517

16
Table 3. The energy efficiency for different configurations in the pressure range of 1-7 bar
Plate A Plate B Plate C
Inlet Electrical power Energy Electrical power Energy Electrical power Energy
pressure consumption efficiency* consumption efficiency* consumption efficiency*
[bar] [ J s-1 ] [ kJ ] [ J s-1] [ kJ ] [ J s-1 ] [ kJ ]
1 172.5 291.1 401 561.0 203 1204.6
2 253 426.9 840 1175.2 441 2616.9
3 345 582.2 1128 1578.1 667 3958.0
4 414 698.6 1500 2098.5 910 5399.9
5 540.5 912.1 1890 2644.1 1090 6468.1
6 598 1009.1 2250 3147.8 1270 7536.2
7 690 1164.4 2670 3735.3 1500 8901.0
*
The value calculated on the basis of the process time for 30 recirculation passes

17
Table 4. The cavitational yields at inlet pressure of 7 bar
Plate A Plate B Plate C
Parameter Unit 10 30 10 30 10 30
passes passes passes passes passes passes
Electrical power consumption
J s-1 690 2670 1500
– power input (PI)
Process time (t) s 562.5 1687.5 466 1399 1978 5934
Energy efficiency – total
kJ 388.1 1164.4 1244.2 3735.3 2967 8901
energy supplied (PI·t)
Volume (V) mL 30000 30000 30000
-1
Power density (PD=PI·t/V) kJ mL 0.013 0.039 0.041 0.125 0.099 0.297
COD removed (CODrem) mg mL-1 0.3560 0.3790 0.3110 0.3030 0.3590 -
Cavitational yield
mg kJ-1
(CODrem/PD) 27.5 9.8 7.5 2.4 3.6 -

18
Highlights
• Hydrodynamic cavitation was studied as a pretreatment of mature landfill leachate
• Orifice plate with a 3/10 mm diameter and 0.033 cavitation number was recommended
• Biodegradability index increased from 0.046 to 0.056 in 30 recirculation passes
• Energy efficiency was evaluated
• Degradation of refractory compounds was confirmed

19