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Ultrasonic Application in Contaminated Soil Remediation

Agus Jatnika Effendi, Marita Wulandari, Tjandra Setiadi

PII: S2468-5844(19)30032-7
DOI: https://doi.org/10.1016/j.coesh.2019.09.009
Reference: COESH 138

To appear in: Current Opinion in Environmental Science & Health

Received Date: 5 July 2019


Revised Date: 18 September 2019
Accepted Date: 24 September 2019

Please cite this article as: Effendi AJ, Wulandari M, Setiadi T, Ultrasonic Application in Contaminated
Soil Remediation, Current Opinion in Environmental Science & Health, https://doi.org/10.1016/
j.coesh.2019.09.009.

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Ultrasonic Application in Contaminated Soil Remediation

Agus Jatnika Effendia*, Marita Wulandari b, and Tjandra Setiadic


a
Environmental Engineering Department, Faculty of Civil and Environmental Engineering, Institut
Teknologi Bandung, Bandung, 40132, Indonesia(jatnika@indo.net.id); * Corresponding Author
b
Environmental Engineering Department, Institut Teknologi Kalimantan, Balikpapan, 76127, Indonesia
(maritawulandari@itk.ac.id)
c
Center for Environmental Studies, Institut Teknologi Bandung, Jl. Sangkuriang 42 A, Bandung 40135,
Indonesia(tjandra@che.itb.ac.id)

Abstract

Ultrasonic remediation is an emerging technology that is applied to recover contaminated soils. There

are 2 (two) main mechanisms that occur in the ultrasonic process: desorption and chemical

degradation. Soil particle size, temperature, ultrasonic power, ultrasonic frequency, ultrasonic intensity

and ultrasonic time are some factors found to affect the performance of ultrasonic remediation. Some

studies showed that ultrasonic could be placed as a pre-treatment process and integrated with other

remediation technology in order to improve the removal efficiency. Although the study related to

ultrasonic remediation is limited, ultrasonic was found to work both for organic and inorganic

contaminants, especially heavy metals or petroleum hydrocarbon contaminated soil as shown by some

studies.

Keywords: Ultrasonic, remediation, desorption, pre-treatment

Introduction

Ultrasonic technology is a clean and green method for treatments the degradation the toxic organic

pollutants (Wang et al.,2019, Son et al, 2011). Ultrasonic is defined as various types of sound with

frequencies above average that can be responded to by the human ear or at above 20 kHz (Wood et. al.,

2017). In practice, three ranges of frequencies are reported for three distinct uses of ultrasound: high

frequency, or diagnostic ultrasound, low frequency or conventional power ultrasound, and medium

frequency, or “sonochemical-effects” (Ince et al., 2001, Luppachini et al., 2017). Low frequency (20-

80 kHz) promoted the physical effects, whereas high ultrasonic frequencies (150-2000 kHz) can lead to

the chemical effects because of the HO• radicals formation in water or slurry phase (Gregory et al.,

2016). Ultrasonic has been studied and applied in many sectors in the field of environmental protection

and remediation because of its good strength to increase physical and chemical reactions, and mass

transfer (Adewuyi, 2001 and Pham, 2014). Ultrasonic is usually not applied as standing alone

technology but is integrated with several other techniques to develop the conventional methods to gain
better results. For example, ultrasonic is usually combined with electrokinetic remediation techniques

or soil washing techniques (Kim and Wang, 2003; Chung and Kamon, 2005; Pham, 2009). Generally,

ultrasonic application as a remediation technique is relying on two main effects to remove chemical

and biological contaminants from soil and water. The first is the mechanism of desorption produced by

local turbulence, and the second is the degradation (chemical effect) that results from free radical

oxidation reactions. The success rate of this ultrasonic method is influenced by several factors such as

soil type, soil/water ratio, water flow rate, irradiation duration, wave frequency, and energy used (Kim

and Wang, 2003; Feng and Aldrich, 2000).

Since the research and application of ultrasonic process in contaminated soil remediation is still

limited, this review is intended to describe the mechanisms of ultrasonic process and some factors that

are affected the performance of ultrasonic remediation. Therefore, those who are interested in applying

ultrasonic remediation would have a better understanding regarding environmental factors that could be

optimized in order to increase the process performance. Moreover, this review also describes the

current status of ultrasonic application in contaminated soil remediation, some facts and findings that

have been achieved so far.

Mechanism of Desorption & Degradation of Organic Materials with Ultrasonic

According to Romdhnae and Goudon (2002), ultrasonic energy accelerates leaching kinetics and

increases removal efficiency through diffusion to the outermost layer. Leaching using the effects of

ultrasonic processes results in higher removal efficiency with shorter processing times compared to

mechanical stirring (Son et al., 2012). The difference between the normal leaching and leaching in the

presence of ultrasonic is illustrated in the following figure (Swamy & Narayana, 2001).
Leaching process of contaminants from soil particles (a) normal leaching (b) leaching in the presence
of ultrasonic

Ultrasonic application into soil system could promote the desorption of contaminants by breaking

down the soil matrix (Jia et al., 2019). Conceptually, the desorption of contaminants from the soil

surface is very dependent on changes in Gibbs energy (∆Go) of a system. In the case of hydrocarbon

contaminates soil, ∆Go is needed to remove hydrocarbon molecules from the soil surface (Feng and

Aldrich, 2000). In order to remove hydrocarbons from the soil by mechanical methods, a certain

amount of energy must be available to change the total Gibb energy (∆G). Ultrasound enhanced a great

desorption rate on petroleum hydrocarbon fraction that generally benefits from the concentrated high

energy and the cavitation effect of ultrasound (Li et al., 2013, Avvaru et al., 2018, Shanceti et al.,

2017). Factors such as intensity, slurry concentration, and irradiation time are known to be influential

factors in the desorption of hydrocarbons from the soil. In addition, parameters such as pH of slurry,

the salinity of slurry, and the presence of surfactants were known to affect adsorption energy and also

play an important role in the desorption process of hydrocarbons in the soil (Feng and Aldrich, 2000).

Besides affecting the desorption process, ultrasonic also can increase the rate of chemical reaction

(Vyas et al., 2018). The chemical effect of organic degradation of pollutants due to ultrasonic

remediation is an oxidation reaction that usually occurs at interphase or in the liquid phase. According

to Hoffmann et al. (1996), degradation caused by ultrasonic cavitation occurs through three pathways:

sonolysis by free radicals, pyrolysis under certain pressure and temperature conditions, and

supercritical water oxidation. Oxidizers (such as hydrogen, hydroxyl, hydroperoxyl) produced from the

sonication process in water will react with organic pollutants and result in changes in the chemical

structure of a pollutant. Long carbon chains or aromatic hydrocarbons with complex structures and

high molecular weight can be broken down into simpler hydrocarbons (Feng and Aldrich, 2000). For

example, according to research by Lim and Okada (2005) and Saez et al. (2011), Trichloroethane

(TCE), and Perchloroethylene (PCE) could be degraded in the form of chloride ions, water, and carbon

oxide.

Factors Affecting Ultrasonic Remediation


There are several important factors that determine the success of ultrasonic remediation in removing

contaminants so that the desorption and degradation process can occur optimally. Some of them are:

• Particle Size; Meegoda and Perera (2001) found that removal efficiency of chromium was 83% in

silty sediments, while in the clay fraction there was no chromium leaching occurred since clay was

resistant to ultrasonication with a frequency of 20 kHz. Soils with finer/smaller particle sizes have

wider surface area and capillary forces making lower the efficiency of reducing contaminants

(Kim et al., 2007). In addition, Meegoda and Perera (2001) stated that the efficiency of

contaminant removal due to ultrasonic processes showed a higher number in coarse solids than

fine-grained ones. Smaller particles can reduce the acoustics of ultrasonic waves; therefore, they

can reduce the effects of cavitation that are responsible for the release and degradation of

contaminants (Lu et al., 2002).

• Temperature; Since ultrasonication induces a high concentration of energy, one of its physical

effects is heating, i.e. the increasing temperature of the bulk solution (Suslick, 2001). The

temperature of the bath is another important parameter that must be considered with ultrasonic

cleaning. Mehrdadi et al. (2018) stated that Temperature was increased in ultrasonic processes due

to the cavitation process and implodes of nano bubles. The rate of the temperature was increased

with the increase of sonification time. According to a study performed by Wu et al. (1991),

temperature had an effect on the detoxification rate. In this study with the working temperature at

15-60℃, Wu et al. (1991) demonstrated that the detoxification rate increased with increasing

operating temperatures which can increase the internal energy of molecules adsorbed, provide the

energy needed for the desorption process, and make adsorbed molecules easier to desorb the

contaminants.

• Ultrasonic Power; Along with the increase in ultrasonic power, it will increase the shearing force

on the soil surface matrix and the diffusion rate of the organic compounds in the irradiated

solution. As a result of this phenomenon, it will increase the efficiency of desorption of

compounds adsorbed on the soil. However, a drastic increase in power can disrupt bubble

dynamics because it makes bubbles grow abnormally during the expansion that can cause poor

cavitation and material (bubbles) growth (Merouani et al., 2013 and Brotchie et al., 2009).

Therefore, the frequency and power always correlate with the balance of bubble growth.
Ultrasonic power consumption is related to the consumption of electrical energy used by

generators or transducers so that it influences costs (Mason, 2016).

• Ultrasonic Intensity; Intensity is defined as the magnitude of the area of unity irradiated.

According to several studies, it can be concluded that the selection of suitable ultrasonic intensity

not only increases operating efficiency but also minimizes operating costs (Asgharzadehahmadi et

al., 2016). Ultrasonic intensity could increase the number of cavitation bubbles (Lin at al., 2016).

Therefore, it is expected that the higher ultrasonic intensity, the faster reaction. The normal value

of the optimum intensity of ultrasonic irradiation is 5-20 W/cm2 (Gogate et al., 2011).

• Ultrasonic Frequency; The frequency of the irradiated waves is an important factors affecting the

ultrasonic process (Ghafarzadeh et al., 2017). The physical effects of ultrasonic can occur at a

minimum frequency of 10-100 kHz. Besides having advantages, high frequencies also have

disadvantages. Transducers are prone to erosion for prolonged use and it has high consumption of

power use (Sutkar, 2009). One way to overcome this problem is to replace a single high frequency

with two or more multiple low frequencies. In addition, cavitation occurs more evenly when using

two or more frequencies. Many studies indicate that the efficiency of ultrasonic processing is

higher in the use of two or more frequencies compared to one frequency in one reactor (Prabhu et

al., 2004 and Zhao et al., 2002).

• Ultrasonic time; Many studies showed that ultrasonic time played an important role in the success

of soil remediation using the ultrasonic technique. Usually, the ultrasonic time ranges from a few

seconds to minutes. Considering the energy consumption required, it is important to determine the

optimum ultrasonic time. Thangavadivel et al, (2011) implemented ultrasonic to desorb DDT from

the soil with a high content of clay, silt and organic substances. It required 30 seconds to get 80%

desorption efficiency of DDT with a frequency of 20 KHz at the power of 932 Watt/L. Son et al.

(2011) found that ultrasonic increased the removal efficiency of conventional soil washing of

diesel-contaminated sandy soil with 1 minute sonication time. Shrestha et al. (2012) stated that no

significant decreased of contaminant was found when sonication time was applied between 1 to 6

hours.

Current Status of Ultrasonic Remediation


Ultrasonic was found to have a potential application for the remediation of contaminated soil or

sediments from various contaminants ranging from heavy metals to organic compounds (Shrestha et

al., 2012). Mason & Lorimer (1988) and Suslick (1989) conducted many kinds of research and reviews

of the effects of ultrasound on chemistry. However, research on ultrasonic applications on soil

remediation is still limited. The ultrasonic process can be used for compounds that are persistent with

the environment and are able to degrade stable contaminants such as polychlorinated biphenyls (PCBs),

polycyclic aromatic hydrocarbons (PAHs), pesticides, and other organochlorines adsorbed into soil

particles (Collings, 2006). In addition, there are many other organic pollutants that have been proven to

be degraded by ultrasonic such as chlorinated aliphatic hydrocarbons (CAHs), aromatic compounds,

polychlorinated biphenyls (PCBs), polyaromatic hydrocarbons (PAHs), several phenol compounds,

chlorofluorocarbons (CFCs), pesticides, and herbicides and others (Adewuyi, 2001; Dewulf and

Langenhove, 2001; Peters, 2001; Little et al., 2002; Collings, 2006; Lim et al., 2007). These studies

demonstrated that not only did sonication improve leaching, but it also destroyed contaminants. The

following table summarized some remediation studies and the application of ultrasonic remediation.

No Title & Authors Result


1. Effect of ultrasound on removal The wave frequency used was 30 kHz with power up to 140
of persistent organic pollutants watts. Samples were made in the slurry phase. The best ratio
(POPs) from different types of of soil and water was 3 : 1. The ultrasonic process increased
soil. Reena Amatya Shresta, the working temperature. In clay soil, the temperature
Thuy Duong Pham, Mika increased in the range of 20oC-520C for the first hour. pH in
Sillanpaa (2009) clay soil was in the range of 5.6-5.8. Remaining POPs
concentration with 1-hour sonication was almost the same as
6 hours. In power variation experiments, the best removal
efficiency of POPs increased with increasing power.
However, at 140 watts of power, it has decreased due to the
cavitation effect.
2. Application of ultrasound and In this study, a probe-type ultrasonic was used. Power used
Fenton’s reaction process for the was 60 W at a frequency of 20 KHz with the duration of
treatment of oily sludge. Ju ultrasonication for 1, 3, 5, and 8 minutes. The oxidizing
Zhang, Jianbing Li, Ronald reagent used was H2O2. It was found that the decrease of
Thring, Lei Liu (2013) Total Petroleum Hydrocarbon (TPH) in oil sludge when
using ultrasonic irradiation alone, Fenton only, and the
combination between Fenton and sequential ultrasonic were
22.6%, 13.8%, and 43.1%, respectively. The significant
effect found in combined processes was due to the increase
of contact between hydroxyl radicals and petroleum
hydrocarbons. From the results of this study, it was also
known that using ultrasonic alone, the decrease in TPH
increased from 1 to 5 minutes. However, after 5 minutes, the
decrease in TPH was not significant.
3. Ultrasonic desorption of Ultrasonic experiments used probe types and they were
petroleum hydrocarbon from operated for 10 minutes, at 20 kHz, with a power of 600 W.
crude oil contaminated soils. Three types of soil were examined; they were soil A (Ottawa
Jianbing Li, Xinyuan Song, sand), soil B (27.6% of silt and clay content), and soil C
Guangji Hu, Ronald Wallen (55.3% of silt and clay content). The results showed that the
Thring (2013) adsorption of crude oil on the three soils could be well
explained by the Langmuir isotherm model. Isotherm
analysis illustrated that ultrasonic irradiation has a
significant impact on increasing crude oil desorption,
especially on fine soil (eg, soil B and soil C). Desorption
experiments showed that desorption using ultrasonic gave
better removal results compared to desorption using
mechanical shaking on all soil types. Therefore, ultrasonic
irradiation can be a promising method for the remediation of
petroleum-contaminated soil. As shown in this study, in
particular, ultrasonic had a large desorption effect of
Petroleum Hydrocarbon on fine soil and could achieve the
desired pollutant removal in a very short time
4. Ultrasonic and mechanical soil In this study, the ultrasonic frequency was 28 kHz. Washing
washing process for the removal solutions used were HCl at concentrations of 0.5 and 1 M
of heavy metals from soils. with a soil/liquid (S/L) ratio of 1:2 and 1:3. The soil washing
Beomguk Park and Younggyu process used mechanical mixing (200 rpm). Low soil/liquid
Son (2017) ratio, in this case, means the more volume washing liquid
used. The lower the S/L ratio the greater removal efficiency
of Cu, Pb, and Zn would be. In addition, removal efficiency
when the mechanical process and ultrasonic combined gave
the best results compared to mechanical process or
ultrasonic process alone. Results also showed that with the
ultrasonic process alone (without mechanical mixing), the
decrease of heavy metals was insignificant. This indicated
that sono-physical effects only occurred in the slurry phase
and they must be mixed so that the desorption process
because of cavitation could occur.
5. Effect of frequency and solid- For the removal of hydrocarbon contaminants on the soil in
liquid ratio on ultrasonic this study, the frequencies used were 28 kHz and 48 kHz
remediation of petroleum using ultrasonic bath type. The soil/liquid (S/L) ratio was 1:
contaminated soil. Marita 3 and 1:10 (gr/ml). The initial TPH concentration was
Wulandari and Agus Jatnika 14362.455 mg/kg. TPH removal efficiency at the frequency
Effendi (2018) of 28 kHz was 55.61%, while at the frequency of 48 kHz it
was 67.09%. Based on the optimum time testing, it could be
seen that the decrease in TPH occurred significantly at the
initial 15 minutes of sonication while the rest was relatively
stable. The optimum S/L ratio was found at 1:10 and it
demonstrated a better TPH removal compared to the 1:3
soil/liquid ratio. Short and volatile chains of hydrocarbon
was not previously found in the initial conditions before
remediation. It indicated that the ultrasonic process was also
involving the degradation process.

Conclusion

Ultrasonic is a promising technology that could be well implemented for the remediation of

contaminated soil. Ultrasonic works with both organic and inorganic contaminants and any type of

soils. However, studies demonstrated that ultrasonic showed its best performance when integrated with

other remediation technologies. In order to achieve a better performance of ultrasonic remediation,

some factors affecting the process could be further investigated. Many environmental aspects are still

open to be optimized. Ultrasonic effect with higher power and higher frequency is expected to
significantly increase the chemical degradation. Also, optimizing velocity gradient of mixing (G) in

order to increase mass transfer and contact between contaminated soil and ultrasonic exposure should

be further investigated. Since ultrasonic process involving desorption, dissolution and chemical

degradation, this process can be treated as pre-treatment for bioremediation. Therefore, it is hoped that

the limitation of bioremediation to degrade clayey soil could be overcome when ultrasonic remediation

is configured as pre-treatment.

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Conflict of Interest Letter

o This manuscript has not been submitted to, nor is under review at, another
journal or other publishing venue.
o Declarations of interest: none

Agus Jatnika Effendi


Environmental Engineering Department, Faculty of Civil and Environmental Engineering, Institut
Teknologi Bandung, Bandung, 40132, Indonesia(jatnika@indo.net.id); * Corresponding Author

Marita Wulandari
Environmental Engineering Department, Institut Teknologi Kalimantan, Balikpapan, 76127, Indonesia
(maritawulandari@itk.ac.id)

Tjandra Setiadi
Center for Environmental Studies, Institut Teknologi Bandung, Jl. Sangkuriang 42 A, Bandung 40135,
Indonesia(tjandra@che.itb.ac.id)
ANNOTATED REFERENCES

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1 Adewuyi, Y., (2001): "Reviews - Sonochemistry: Sonochemistry enhances promotes chemical
Environmental Science and Engineering Applications," reaction and mass transfer. A number a previous
Ind. Eng. Chem. Res., vol. 40, pp. 4681-4715. studies have examined the transformation of
pollutants by ultrasonic irradiation or combined
ultrasound and other advanced oxidation
techniques to organic techniques to
intermediates with mineralization to inorganic
ions, CO2, and short-chain organic acids as final
products in some cases. The pollutants studied
and other environmental application include:
aromatic compounds, Chlorinated Aliphatic
Hydrocarbons (CAHs), Explosives, Herbicide
and Pesticide, organic dyes, organic and
inorganic gaseous, organic sulfur compounds,
oxygenated and alcohols, other organic
compounds.

2 Asgharzadehahmadi, S., Raman, A.A.A, Parthasarathy, As a result, it can be summarized that chosing
R., Sajjadi, B., (2016): Sonochemical reactors: Review appropriate power rating does not only increase
on features, advantages, and limitations. Renewable the efficiency of operation but also to decrease
and Sustainable Energy Reviews, 63, 302-314 in operating cost for a given process.

3 Avvaru Balasubrahmanyam, Venkateswaran Natarajan, Authors claimed that cavitation effects such as
Uppara Parasuveera, Iyengar Seresh B., Katti Sanjeev microstreaming and turbulence are responsible
S.(2018). Current knowledge and potential applications for the breaking of interfacial films that
of cavitation technologies for the petroleum industry. stabilizes the emulsions, which may lead to
Ultrasonics - Sonochemistry , 42, 493–507 coalescence of the droplets and causing better
oil water separation.

4 Brotchie.A., Grieser. F., Ashokkumar. M. (2009) Effect It was found that the bubble size increased with
of power and frequency on bubble-size distribution in increasing power and decreased with increasing
acoustic cavitation. Physical Review Letter 102 (8). frequency.
DOI: 10.1103/PhysRevLett.102.084302

5 Chung H. I., and M. Kamon, (2005): Ultrasonically The study emphasized the coupled effects of
enhanced electrokinetic remediation for removal of Pb electrokinetic and ultrasonic technique were
and phenanthrene in contaminated soils, Eng. Geol., conducted using specially designed and
vol. 77, 233- 242 fabricated devices to determine the effect of
both techniques. The electrokinetic techniques
was applied to remove mainly the heavy metal
and the ultrasonic technique was applied to
remove mainly organic subtances in
contaminated soil.
6 Chatel Gregory, Novikova Liudmila, Petit Sabine. It is usually accepted that low frequencies (20-
(2016). How efifiiently combine sonochemistry and 80 kHz) preferentially lead to physical effects,
clay science ?. Applied clay science 119, 193-201 whereas high ultrasonic frequencies (150-2000
kHz) favor the production oh HO • radicals in
water, mainly leading to chemical effects.
7 Collings A.F, (2006). Processing Contaminated Soils This paper describes the development of high
and Sediments by high power Ultrasound. Journal power ultrasound to destroy persisten organic
Minerals Engineering, 450-453 pollutants (POPs) in soils and sediments.
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8 Dewulf, J., Langenhove, H.V., 2001. Ultrasonic This study focused on the degradation kinetics
degradation of trichloroethylene and chlorobenzene at of chlorobenzene (CB) and trichloroethylene
micromolar concentrations: kinetics and modeling. (TCE) in the micromolar range.
Ultrasonics Sonochemistry 8, 143-150.

9 Feng, D. & Aldrich, C.(2000): Sonochemical treatment Factors such as power intensity, slurry
of simulated soil contaminated with diesel. Adv. concentration and irradiation duration
Environ. Res. 4(2), 103–112. influencing the ultrasonic irradiation could
affect the desorption of hydrocarbon from
quartz. Better result were obtained with a
multistage treatment process. Slurry pH and
salinity affected the diesel removal efficiency by
changing the zeta potential of the quartz. The
surfactant can improve the mobility of
hydrocarbon contaminants in soil-water systems
by solublishing the adsorbed hydrocarbons
through incorporation in surfactant micelles.
The long-chain hydrocarbons were broken down
into short-chain hydrocarbons (predominantly
alkanes) in the presence of ultrasound. These
short-chain hydrocarbons desorb more easily
from quartz surfaces. Long chain or aromatic
hydrocarbons are subject to higher dispersion
forces than short-chain hydrocarbons.
Conceptually, the desorption of diesel from
quartz surfaces is dependent on the change of
the Gibbs free energy (∆G) of the system, where
the ∆G required to remove a hydrocarbon
molecule from quartz surface.
10 Ghafarzadeh Mahdi, Abedini Rezvan, Rajabi Rohollah. The frequency of the irradiated waves, other
(2017). Optimization of ultrasonic waves application in important factors affecting the ultrasonic process
municipal wastewater sludge treatment using response include power of the waves and duration of their
surface method. Journal of Cleaner Production,150, irradiation.
361-370
11 Gogate PArag R., Sutkar Vinayak S., Pandit Aniruddha A typical range of optimum intensity of
B., (2011). Sonochemical reactors : Important design irradiation ( power dissipated per unit area of
and scale up with a special emphasis on heterogeneous irradiating surfaces, W/cm 2) is 5- 20 W/cm2
systems. Chemical Engineering Journal, 166, 1066- which also dependet on the actual reactor system
1082 and the end application.

12 Hoffman, M.R., Hua, I., Hochemer, R., (1996). The degradation of chemical compounds by
Application of ultrasonic irradiation for the degradation acoustic cavitation is shown to involve three
of chemical contaminants in water. Ultrason. distinct pathways. The pathways include
Sonochem.3 (3), S163-S172 oxidation by hydroxyl radicals, pyrolytic
decomposition and supercritical water oxidation.
Ultrasonic irradiation appears to be an effective
method for the destruction of organic
contaminants in water because of localized high
concentrations of oxidizing species such as
hydroxyl radical and hydrogen peroxide in
solution, high localized temperature and
pressures, and the formation of transient
supercritical water.
13 Ince.N, G. Tezcanli, R. Belen and G. Apikyan, (2001). Ultrasound is defined as any sound of a
Ultrasound as catalyzer of aqueous reaction systems: frequency above that to which the human ear
The state of art and environmental applications, Appl. has no response (i.e.above 16 kHz). In practice,
Catal. B, 29, 167-176. three ranges of frequencies are reported for three
distinct uses of ultrasound: (i) high frequency, or
diagnostic ultrasound(2–10 MHz), (ii) low
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frequency or conventional power ultrasound
(20–100 kHz), and medium frequency, or
“sonochemical-effects” ultrasound (300–1000
kHz). It is this latter range, where chemical
reaction processes are uniquely catalyzed
through very “extreme” temperatures and
pressures generated by the formation, growth
and collapse of cavitation bubbles.
14 Jia Lei Yong, Tian Yu, Fang Cheng, Zhan Wei, Duan Another benefit of introducing US into soil
Lu Chun, Zhang Jun, Zuo Wei, Wei Kong Xiao. system is it could promote the breaking down of
(2019).Insights into the oxidation kinetics and soil aggregates, which is expected to enhanced
mechanism of diesel hydrocarbons by ultrasound the desorption of contaminants form soil (akin
activated persulfate in a soil system. Chemical washing-off) and the diffusion of PS (persulfate)
Engineering Journal, 378,122253 into soil aggregates (akin stirring), hence
increasing the destruction efficiency.
15 Kim, Y., and Wang M. C., (2003): Effect of ultrasound - The soil-flushing method enhanced by
on oil removal from soils, Ultrasonics, vol. 41, 539- ultrasonic waves is a new technique that
542. potentially can become an effective method
for insitu remediation of the ground
contaminated by NAPL hydrocarbons.
- The test results indicated that sonication can
enhance pollutants removal considerably, and
that the degree of enhancement depends on a
number of factors such as sonication power,
water flow rate, and soil type. Increasing
sonication power will increase pollutant
extraction only up to the level where
cavitation occurs.
16 Kim, Y., Park J. H., Kim S. H., and Khim J., (2007). - The effect of ultrasound on diesel removal
Ultrasonically enhanced diesel removal from soil. from soils were investigated in this study.
Japanese Journal of Applied Physics, Vol 46, No. 7B, Laboratory soil-flushing experiments were
2007, pp. 4912–4914 conducted for various conditions involving
ultrasonic power, particle size, and diesel
contaminant concentration. The efficiency
of diesel removal was significantly affected
by particle size and the intensity of ultrasonic
energy. Diesel was more easily removed
from relatively coarse particles. This can be
attributed to their low roughness and surface
areas.
- The test results indicated that the rate of
contaminant extraction increased significantly
with increasing ultrasonic power.
17 Li J., Song X., Hu G., Thring R. W., (2013). Ultrasonic The great desorption enhancement by ultrasound
desorption of petroleum hydrocarbons from crude oil on PHC fraction generally benefits from the
contaminated soils. Journal of Environmental Science concentrated high energy and the cavitation
and Health, Part A: Toxic/Hazardous Substances and effect of ultrasound.
Environmental Engineering, 48:11, 1378-1389

18 Lim, J.L., Okada, M., (2005). Regeneration of granular About 50 % of TCE was desorbed for 1 h.
activated carbon using ultrasound. Ultrasonic Because of sonochemical degradation of the
Sonochemistry 12, 277-282 desorbed TCE the TCE concentration in liquid
phase was only 0,007 mg/l. The practically
measured its concentration inliquid phase was
only 34-43 % of that stoichiometrically
calculated on the assumption that 100 % of
desorbed TCE from GAC is sonochemically
mineralized to Cl-, H2O, and CO2.
19 Lim, M.H., Kim, S.H., Kim, Y.U., Khim, J., (2007). This study examine the degradation of
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Sonolysis of chlorinated compounds in aqueous chlorinated hydrocarbons. The degradation
solution. Ultrasonics Sonochemistry 14, 93-98. were analyzed as pseudo first order reactions
and their reaction rateconstant were in the range
of 10 -1- 10-3 /min.
20 Lin Meiqing, Ning Xun-an, An Taicheng, Zhang As we know, higher ultrasonic intensity in the
Jianhao, Chen Changmin, Ke Yaowei, Wang Yujie, reaction system would accelerate the reaction.
Zhang Yaping, Sun Jian, Liu Jingyong. (2016). The increase in the ultrasonic intensity could
Degradation of polycyclic aromatic hydrocarbons increase the number of active cavitation bubbles
(PAHs) in textile dyeing sludge with ultrasound an and also the size of the individual bubbles.
Fenton processes : Effect of system parameters and
synergetic effect study. Journal of Hazardous
Materials, 30, 7–16
21 Little, C., Hepher, M.J. and El-Sharif, M. (2002). The - In the study of the degradation of PAHs
sono-degradation of phenanthrene in an aqueous through ultrasonic irradiation, the
environment. Ultrasonics 40: 667-674 breakdown of an aqueous solution of
phenanthrene in a sonochemical reactor
utilising a 30 kHz probe system, operating in
batch mode, has been investigated. The
phenanthrene molecule was studied and used
as a model PAH molecule.
- Qualitative analysis using HPLC and
quantitative analysis using UV/Vis photo-
spectrometry confirmed that a 88% reduction
in the peak observed phenanthrene
concentration was achieved over 240 min of
sonocation. Whilst there was the potential for
the formation of recalcitration and
rearrangement products, no higher order
PAHs were observed and a 80% reduction in
total monitored UV fluorescence and hence,
aromaticity/ conjugation, was observed
22 Lu Y.F., Riyanto N., Weavers L. K., (2002). Sonolysis However, degradation of contaminants
of synthetic sediment particles: particle characteristics following desorption would be expected to be
affecting particle dissolution and size reduction, highest with smaller particle sizes and
Ultrason Sonochem. 9, 181-188 particles with larger liquid– solid surface areas
as they provide the most cavitation nuclei
reducing the detrimental effects of scattering
and attenuation of sound waves.
23 Luppachini Massimiliano, Mascitti Andrea, Giachi Accoustic waves that fall in the human hearing
Guido, Tonucci Lucia, d’Alessandro Nicola, Martinez range (i.e ‘sonic’ waves) have frequencies that
Jean, Colacino Evelina. (2017). Sonochemistry in non- cover the 20 Hz-20 kHz interval. Below and
conventional, green solvents or solvents-free reaction. above these extremes the ‘infrasounds’ and
Tetrahedron ,73, 609-653 ‘ultrasounds’ (US) lie, respectively. They
constitute the basis for a number of applications
in science and technology and are further
subdivided into ‘power US’ (20 kHz to 1 MHz)
and ‘high frequency US’ (1 MHz upwards).
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24 Mason, T. J. (2016). Ultrasonic cleaning: A historical Perhaps the simplest method of estimating
perspective. Ultrasonics Sonochemistry, 29, 519– electrical power consumption by a cleaning bath
523.doi:10.1016/j.ultsonch.2015.05.004 is to directly measure the power consumption
from the electrical mains supply. While certainly
this is important in terms of calculating the cost
of the process for industrialists it does not take
into account the electrical efficiency of the
generator or transducer.

25 Meegoda J.N, Perera R., (2001). Ultrasound to A maximum removal of 83 % was obtained for
decontaminate heavy metals in dredged sediments, silt fraction when factor levels were at 1200 W
Journal Hazard Material, 85, 73-89 power, 1: 50- to- water ratio and 90 min of dwell
time. Further analysis of clay fraction showed
that the chromium in clay is immobile and
stable. It was concluded that the clay fraction
could not be effectively treated by this
technology. However, due to the distribution of
chromium in the clay fraction, it was found that
the chromium is quite immobile in the clay
fraction of the treated sediments.

26 Mehrdadi Nasser, Kootenaei Farshad Golbabaei. 2018. Temperature was increased in ultrasonic
An Investigation on effect of ultrasound waves on processes due to the cavitation process and
sludge treatment. 5th International Conference on implodes of nano bubles. The rate of the
Energy and Environment Research, ICEER temperature was increased with the increase of
sonification time.

27 Merouani S, Hamdaoui O, Rezgui Y, Guemini M It is quite clear that as the ultrasound frequency
(2013) Effects of ultrasound frequency and acoustic increases,the range of ambient radius for an
amplitude on the size of sonochemically active active bubble becomes less wideness and the
bubbles—theoretical study. Ultrason Sonochem optimal ambient radius becomes smallest. This
20:815–819. behavior was observed for all employed acoustic
https://doi.org/10.1016/j.ultsonch.2012.10.015 amplitudes. Experimentally, in addition to the
size distribution decreasing with increasing
acoustic frequency
28 Nguyen Tam Thanh, Asakura Yoshiyuki, Koda When cavitation is generate, OH radicals are
Shinobu, Yasuda Keiji. (2017).Dependende of released, that is why chemical effect is obtained
cavitation, chemical effect, and mechanical effect in the solution. Below the electric input power
thresholds on ultrasonic frequency. Ultrasonics - of 2 W, the reaction rate is zero. Thereafter, the
Sonochemistry 39, 301–306 reaction rate increases with increasing
electric power.
29 Park Beomguk.,(2017): Ultrasonic and mechanical soil - The sieved and dried soil sample was
washing process for the removal of heavy metal from violently mixed with a washing liquid (0.5 or
soil. Ultrasonic sonochemistry, 640-645 1.0 M HCl solution) in the vessel. No
corrosive damage in the washing vessel was
observed over 30 operations in this study. The
mass of dry soil was 300 or 500 g and the
soil/liquid ratio (mass/mass) was 1:2 or 1:3.
Soil washing processes using only
mechanical mixing (200 rpm) was
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designated as a mechanical soil washing
process in this study. In the case of an
ultrasonic/mechanical soil washing process,
28 kHz ultrasound was irradiated from the
bottom with mechanical mixing.
- Higher removal efficiencies were observed
in the case of the lower soil/liquid ratio
(1:3) for all three heavy metals in both
mechanical processes and
ultrasonic/mechanical processes. Low
soil/liquid ratio, which means large amount of
washing liquid to a certain amount of target
soil.
- However no significant removal was observed
in ultrasonic soil washing processes without
the mechanical mixing. It meant that the
sonophysical effects were available for very
limited area in slurry phase due to the large
attenuation of ultrasound.
30 Peters D., (2001). Sonolytic degradation of volatile From the results obtained in pure and natural
pollutants in natural groundwater: conclusions from a water contaminated by 1,2-DCA the following
model study. Ultrasonics Sonochemistry 8, 221-226. promising conclucions for a sonolyc process can
be drawn : the highly volatile chlorinated
hydrocarbons treated are almost completely
destroyed in natural water within 60-120 min.
31 Pham, T.D (2014). Ultrasonic and Electrokinetic On the other hand, as a novel and rapidly
Remediation of Low Permeability Soil Contaminated growing science, the applications of ultrasound
With Persistent Organic Pollutants. ISBN 978-952- in environmental technology hold a promising
265-644-5. Lappeenranta University of Technology future. Compared to conventional methods,
University Press: Finlandia ultrasonication can bring several benefits such
as environmental friendliness (no toxic chemical
are used or produced), low cost, and compact
instrumentation. It also can be applied onsite.
Ultrasonic energy applied into contaminated
soils can increase desorption and mobilization of
contaminants and porosity and permeability of
soil through developing of cavitation.
32 Prabhu A. V., Gogate P. R., Pandit A. B., (2004). - With the addition of another frequency using
Optimization of multiple-frequency sonochemical additional transducers, cavity sizes as well as the
reactors. Chem Eng Sci 59: 4991-8 lifetime of the cavity are enhanced considerably
with a relatively marginal drop in the collapse
pressures and temperatures. Therefore, triple-
frequency sonochemical reactors show
considerably higher overall cavitational activity
as compared to the single- and dual-frequency
sonochemical reactors at equivalent power
dissipation levels.
- The best efficacy of the multiple-frequency
sonochemical reactors will probably result from
resonant combinations or with combinations
where the individual frequencies differ
marginally from each other. Also, lower
frequency combinations are preferable.
33 Romdhane M., and Gourdon C., (2002). Investigation It is clearly demonstrated that ultrasound
in solid-liquid extraction: influence of ultrasound. ameliorates simultaneously the kinetics and the
Chem Eng J; 87: 11-9 yield of the extraction. The good results
obtained with ultrasound in the different
experiments are probably linked to the increase
in the internal diffusion which controls the
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transfer of the solute to the solvent, and also to
the destruction of pores in which the solute can
be trapped.
34 Saez, V., Esclapez, M.D., Bonete, P., Walton, D.J., We note major products of Cl- and CO2/CO, and
Rehorek, A., Louisnard, O., Gonzalez-Garcia, J., also trichloroethylene (TCE) and
(2011). Sonochemical degradation of dichloroethylene (DCE) at ppm concentrations
perchloroethylene: the influence of ultrasonic variables, as reported earlier. The formation at very low
and the identification of products. Ultrasonic (ppb) concentration of small halocompounds
Sonochemistry 18: 104-113 (CHCl3, CCl4) and also of higher-mass species,
such as pentachloropropene, hexachloroethane,
is noteworthy.
35 Sancheti Sonam V., Gogate Parag R., (2017). A review Cavitation generated using ultrasound can
of engineering aspects of intensification of chemical enhanced the rates of several chemical reactions
synthesis using ultrasound. Ultrasonics Sonochemistry giving better selectively based on the physical
36, 527–543 and chemical effects.
36 Shrestha R.A., Mudhoo A., Pham T. D., and Sillanpää Although ultrasonic applications in
M., (2012). "Ultrasound and Sonochemistry in the environmental areas are still in lab-scale and
Treatment of Contaminated Soils by Persistent Organic developing stage, they are growing rapidly,
Pollutants," in Handbook on Applications of attracting more interest, because of the many
Ultrasound: Sonochemistry for Sustainability, D. Chen, advantages they offer environmental friendly
S. K. Sharma, and A. Mudhoo, Eds., FL: CRC Press (no toxic chemicals are used or produced), low
Taylor & Francis Group, pp. 407-418 energy demands, and compact and transportable
method that can be used on-site. Environmental
remediation by ultrasonication involves mostly
with organic pollutant destruction, through
thermal decomposition (pyrolysis) and the
formation of oxidative species like hydroxyl
radical that enhance the mineralization of
pollutants
37 Shrestha R.A., Pham T.D., Sillanpaa M., (2009): Effect - The ultrasonic processors used in these
of ultrasonic on removal of persistent organic experiments were UP100H with operating
pollutants (POPs) from Different types of soils. Journal frequency of 30 kHz, power of 100Wfrom
of Hazardous Materials pp 871-875 Hielscher Ultrasonic Ltd.
- Then, the slurries were kept in flume wood
for about 7 or more days to assure total
evaporation of solvents
- In case of synthetic clay, 1:1, 2:1 and 3:1
ratios increased in remediation as 1:2:4
- The temperature increased from 20 ◦C to
52◦C in first 1 h in synthetic clay
- The pH values of natural clay slightly
fluctuated in the range of 5.6–5.8
- In general, the concentrations of model
compounds reduced gradually with time.
However, there were not very big differences
between the concentrations after 1 h and 6 h.
- However, in the case of natural farm clay, the
two tests at 100W showed the highest POPs
concentration removed then decreased at
140W. The drop in contaminant removal
beyond about 100Wcan be attributed to the
effect of cavitation
38 Son Y., Nam S., Ashokkumar M., Khim J., (2012). The ultrasonic washing processs does not
Comparison of energy consumption between require external chemicals and can be
ultrasonic, mechanical, and combined soil washing considered as a “green” process. The
process. Journal Ultrasonic Sonochemistry, 19, 395- mechanical mixing did not result in any
398 significant damage on the surface of the soil
particles. In addition, there was no significant
difference in the SEM images for the
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ultrasonic and combined processes. Thus it
was found that the soil particle surface was
mainly damaged by sonophysical effects
which could increase the removal of the
contaminant from soil. Extended exposure of
the particles to ultrasound irradiation resulted in
severe breakage of the surface.
39 Son Y., Cha J., Lim M.; Ashokkumar M., Khim., First, this process could achieve high removal
(2011). J. Comparison of ultrasonic and conventional efficiency in a single attempt. Second, it could
mechanical soil-washing processes for diesel- decrease the operating time markedly. In this
contaminated sand. Ind. Eng. Chem. Res., 50(4), 2400– study, the addition of 35 kHz ultrasound
2407 irradiation to the conventional soil washing
process enabled the washing time to decrease
from 4 to 1 min for the removal of 75% diesel
from the contaminated soil.
40 Suslick K. S., (2001). "Sonoluminescence and - When a liquid is irradiated with high intensity
Sonochemistry," in Encyclopedia of Physical Science sound or ultrasound, acoustic cavitation (the
and Technology, 3rd ed., R. Meyers, Ed., San Diego, formation, growth, and implosive collapse of
Academic Press, Inc bubbles in liquids irradiated with sound)
generally occurs.
- If liquids containing solids are irradiated with
ultrasound, related phenomena can occur.
Near an extended solid surface, cavity
collapse becomes non-spherical, which drives
high-speed jets of liquid into the solid surface.
These jets and associated shock waves can
cause substantial surface damage and expose
fresh, highly heated surfaces.
41 Sutkar V. S., and Gogate P.R., (2009). Design aspects Also, it is likely that continuous operation with
of sonochemical reactors: techniques for understanding high frequency irradiation leads to an erosion
cavitational activity distribution and effect of operating of the transducers surface. The power
parameters. Chem Eng J., 155: 26-36 requirement for inception of cavitation events
in a high frequency operation is also higher.

42 Swamy K., and Narayana K., (2001). Advances in Although there is plenty of experimental
Sonochemistry, 6, Theme Issue – Ultrasound in evidence that ultrasound improves leaching, the
Environmental Protection, (Eds. Mason, T. J., and exact mechanism is not fully understood but a
Tiehm A.), Elsevier. model has been suggested

43 Thangavadivel K., Megharaj M., Smart R. S. C., In this study, using high-power low frequency
Lesniewski P. J., Bates D., Naidu R., (2011). ultrasound, heated slurries with anionic
Ultrasonic enhanced desorption of DDT from surfactant sodium dodecyl sulfate (SDS) were
contaminated soils. Water Air Soil Pollut., 217(1–4), treated to enhance desorption of DDT from
115–125 soils with high clay, silt, and organic matter
content and different pH (5.6–8.4). The results
were compared with DDT extracted using a
strong solvent combination as reference. Slurry
ranges from 5 to 20 wt.% were studied. For a
soil slurry (10 wt.%) at pH 6.9 with 0.1% v/v
SDS surfactant heated to 40°C for 30 min.
44 Vyas Shruti, Ting Yeng-Peng. (2018). A reviewof the The application of ultrasound in increasing the
application of ultrasound in bioleaching and insight rate of chemical reactions, such as in chemical
from sonication in (bio) chemical processes. Resources, leaching, is widely accepted.
7,3
45 Wang Jing, Wang Zhenjun, Vieira Carolina L.Z., Ultrasonic technology is a clean and efficient
Wolfson Jack M., Pingtian Guiyou, Huang Shaodan. new treatment method for the degradation of
(2019). Review on the treatment of organic pollutants toxic organic pollutants. Main factors affecting
in water by ultrasonic technology. Ultrasonics - the process of ultrasonic degradation are
Sonochemistry , 55,273–278 ultrasonic frequency, intensity, dissolved gas,
No Reference Content
pH value, and temperature.
46 Wood R. J., Lee J., Bussemaker M. J., (2017): A Ultrasound, a sound field with frequency greater
parametric review of sonochemistry: Control and than ~20 kHz, has a plethora of applications in
augmentation of sonochemical activity in aqueous several actively researched areas
solutions.Ultrasonic Sonochemistry, 38, 351-370

47 Wu J. M., Huang H.S., Livengood C. D., (1991). - Under such conditions, water decomposes
Development of an Ultrasonic Process for Detoxifying into extremely reactive hydroxyl radicals
Groundwater and Soil: Laboratory Research. Annual (OH) and hydrogen atoms (H). During the
Report. ANL/ESD/TM-32. subsequent cooling phase, the hydrogen
atoms and hydroxyl radicals can recombine to
form hydrogen peroxide (H202) and molecular
hydrogen. If organic compounds are present
in the water, they are rapidly destroyed in this
environment.
- A removal efficiency of about 80% was
observed for 4 min of irradiation;the removal
efficiency remained unchanged within a
temperature rangeof 20-60°C. These results
illustrate that, within this temperature range,
increasing the steady-state temperature of the
irradiation solutions seems to have little effect
on CCl4 destruction efficiency. In other
words, operating the system in the optimal
temperature range will yield high removal
efficiencies within reasonable operation times
48 Wulandari, M. and Effendi A. J., (2018). Proceeding of - A washing liquid was used to violently mixed
5Th International Conference on Science and Applied the sieved and dried sample in the reactor.
Science (ICSAS) Effect of frequency and ratio solid- The dry soil mass was 300 and 100 g and the
liquid on ultrasonic remediation of petroleum ratio of soil/liquid (mass/mass) was 1:3 or
contaminated soil (pp. 020120-1 - 020120-7). 1:10. Ultrasonic process, 28kHz and 48 kHz
Published by AIP Publishing ultrasound was irradiated from the bottom
with mechanical mixing.
- The TPH concentration at the beginning of
the study was 14362,455 mg/kg.
- The efficiency of TPH removal on soil with
28 kHz frequency was 55.62% while 48 kHz
at 67.09%.
- The TPH reduction increased until 15 min.
However, during duration of treatment which
more than 15 min did not improve the
performance of ultrasonic, indicating that
treatment efficiency might be reaching a
maximum value as the ulrasonic time
increases.
- The higher removal efficiencies were
observed when the soil/liquid ratio was lower
(1:10).
- The TPH components were changed after
ultrasonic treatment and this might be because
the ultrasound pyrolyzed organic molecules
with long carbon chain and generated
intermediate with low molecular weight.
49 Zhang J., Li J., Thring R., Liu L., (2013). Application - The ultrasonic probe was then placed into
of Ultrasound and Fenton's Reaction Process for the the sludge/water system for ultrasonic
Treatment of Oily Sludge. International Symposium on oxidation. The ultrasonic power was fixed
Environmental Science and Technology (2013 ISEST) at 60 W and the treatment duration was set
up as 1, 3, 5, and 8 min, respectively.
- Due to violent oxidation reaction, H2O2 was
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gradually added into the system until reaching
the specified volume by using a 1-ml pipette.
- It was found that the TPH reduction in oily
sludge reached 22.6%, 13.8%, and 43.1%
when using ultrasonic irradiation alone,
Fenton’s reaction alone, and the
combination of ultrasound with Fenton’s
reaction, respectively. For the combined
process, the oxidation reaction in sludge
system could be improved by increasing the
contact of the hydroxyl radicals with
petroleum hydrocarbons.
- The TPH reduction slightly increased from <
20% to 22.6% when the ultrasonic treatment
time increased from 1 min to 5 min.
However, longer treatment duration than 5
min did not improve the ultrasonic
performance, and the TPH reduction slightly
decreased to 16.3% after 8 min of US
treatment.

50 Zhao Y., Zhu C., Feng R., Xu J., Wang Y., (2002) The fluorescence enhancement of the aqueous
Fluorescence enhancement of the aqueous solution of solution of terephthalate ion (TA) under
terephthalate ion after bi-frequency sonication. orthogonal sonication of 28 kHz and 1.7 MHz
Ultrason Sonochem., 9: 241- 3 ultrasonic wave has been studied. It has been
found that the fluorescence intensity of TA
solution after bi-frequency ultrasonic irradiation
is obviously higher than the sum of those under
two individual ultrasonic irradiations.

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