Ultrasonic application in contaminated soil remediation

Journal Pre-proof 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. This is a PDF file of an article that has undergone enhancements after acceptance, such as the addition of a cover page and metadata, and formatting for readability, but it is not yet the definitive version of record. This version will undergo additional copyediting, typesetting and review before it is published in its final form, but we are providing this version to give early visibility of the article. Please note that, during the production process, errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain. © 2019 Elsevier B.V. All rights reserved.

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([email protected]); * Corresponding Author b Environmental Engineering Department, Institut Teknologi Kalimantan, Balikpapan, 76127, Indonesia ([email protected]) c Center for Environmental Studies, Institut Teknologi Bandung, Jl. Sangkuriang 42 A, Bandung 40135, Indonesia([email protected])

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 (2080 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 1.

Title & Authors Effect of ultrasound on removal of persistent organic pollutants (POPs) from different types of soil. Reena Amatya Shresta, Thuy Duong Pham, Mika Sillanpaa (2009)

2.

Application of ultrasound and Fenton’s reaction process for the treatment of oily sludge. Ju Zhang, Jianbing Li, Ronald Thring, Lei Liu (2013)

3.

Ultrasonic desorption of petroleum hydrocarbon from crude oil contaminated soils. Jianbing Li, Xinyuan Song,

Result The wave frequency used was 30 kHz with power up to 140 watts. Samples were made in the slurry phase. The best ratio of soil and water was 3 : 1. The ultrasonic process increased the working temperature. In clay soil, the temperature increased in the range of 20oC-520C for the first hour. pH in 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. In this study, a probe-type ultrasonic was used. Power used was 60 W at a frequency of 20 KHz with the duration of ultrasonication for 1, 3, 5, and 8 minutes. The oxidizing reagent used was H2O2. It was found that the decrease of 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. Ultrasonic experiments used probe types and they were operated for 10 minutes, at 20 kHz, with a power of 600 W. Three types of soil were examined; they were soil A (Ottawa sand), soil B (27.6% of silt and clay content), and soil C

Guangji Hu, Ronald Wallen Thring (2013)

4.

Ultrasonic and mechanical soil washing process for the removal of heavy metals from soils. Beomguk Park and Younggyu Son (2017)

5.

Effect of frequency and solidliquid ratio on ultrasonic remediation of petroleum contaminated soil. Marita Wulandari and Agus Jatnika Effendi (2018)

(55.3% of silt and clay content). The results showed that the 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 In this study, the ultrasonic frequency was 28 kHz. Washing solutions used were HCl at concentrations of 0.5 and 1 M with a soil/liquid (S/L) ratio of 1:2 and 1:3. The soil washing process used mechanical mixing (200 rpm). Low soil/liquid 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. For the removal of hydrocarbon contaminants on the soil in this study, the frequencies used were 28 kHz and 48 kHz using ultrasonic bath type. The soil/liquid (S/L) ratio was 1: 3 and 1:10 (gr/ml). The initial TPH concentration was 14362.455 mg/kg. TPH removal efficiency at the frequency 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([email protected]); * Corresponding Author Marita Wulandari Environmental Engineering Department, Institut Teknologi Kalimantan, Balikpapan, 76127, Indonesia ([email protected])

Tjandra Setiadi Center for Environmental Studies, Institut Teknologi Bandung, Jl. Sangkuriang 42 A, Bandung 40135, Indonesia([email protected])

ANNOTATED REFERENCES No

Reference Adewuyi, Y., (2001): "Reviews - Sonochemistry: Environmental Science and Engineering Applications," Ind. Eng. Chem. Res., vol. 40, pp. 4681-4715.

Content Sonochemistry enhances promotes chemical reaction and mass transfer. A number a previous 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, R., Sajjadi, B., (2016): Sonochemical reactors: Review on features, advantages, and limitations. Renewable and Sustainable Energy Reviews, 63, 302-314

As a result, it can be summarized that chosing appropriate power rating does not only increase the efficiency of operation but also to decrease in operating cost for a given process.

3

Avvaru Balasubrahmanyam, Venkateswaran Natarajan, Uppara Parasuveera, Iyengar Seresh B., Katti Sanjeev S.(2018). Current knowledge and potential applications of cavitation technologies for the petroleum industry. Ultrasonics - Sonochemistry , 42, 493–507

Authors claimed that cavitation effects such as microstreaming and turbulence are responsible for the breaking of interfacial films that stabilizes the emulsions, which may lead to coalescence of the droplets and causing better oil water separation.

4

Brotchie.A., Grieser. F., Ashokkumar. M. (2009) Effect of power and frequency on bubble-size distribution in acoustic cavitation. Physical Review Letter 102 (8). DOI: 10.1103/PhysRevLett.102.084302

It was found that the bubble size increased with increasing power and decreased with increasing frequency.

5

Chung H. I., and M. Kamon, (2005): Ultrasonically enhanced electrokinetic remediation for removal of Pb and phenanthrene in contaminated soils, Eng. Geol., vol. 77, 233- 242

6

Chatel Gregory, Novikova Liudmila, Petit Sabine. (2016). How efifiiently combine sonochemistry and clay science ?. Applied clay science 119, 193-201

7

Collings A.F, (2006). Processing Contaminated Soils and Sediments by high power Ultrasound. Journal Minerals Engineering, 450-453

The study emphasized the coupled effects of electrokinetic and ultrasonic technique were conducted using specially designed and 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. It is usually accepted that low frequencies (2080 kHz) preferentially lead to physical effects, whereas high ultrasonic frequencies (150-2000 kHz) favor the production oh HO • radicals in water, mainly leading to chemical effects. This paper describes the development of high power ultrasound to destroy persisten organic pollutants (POPs) in soils and sediments.

1

No

Reference Dewulf, J., Langenhove, H.V., 2001. Ultrasonic degradation of trichloroethylene and chlorobenzene at micromolar concentrations: kinetics and modeling. Ultrasonics Sonochemistry 8, 143-150.

Content This study focused on the degradation kinetics of chlorobenzene (CB) and trichloroethylene (TCE) in the micromolar range.

9

Feng, D. & Aldrich, C.(2000): Sonochemical treatment of simulated soil contaminated with diesel. Adv. Environ. Res. 4(2), 103–112.

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Ghafarzadeh Mahdi, Abedini Rezvan, Rajabi Rohollah. (2017). Optimization of ultrasonic waves application in municipal wastewater sludge treatment using response surface method. Journal of Cleaner Production,150, 361-370 Gogate PArag R., Sutkar Vinayak S., Pandit Aniruddha B., (2011). Sonochemical reactors : Important design and scale up with a special emphasis on heterogeneous systems. Chemical Engineering Journal, 166, 10661082

Factors such as power intensity, slurry concentration and irradiation duration 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. The frequency of the irradiated waves, other important factors affecting the ultrasonic process include power of the waves and duration of their irradiation.

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Hoffman, M.R., Hua, I., Hochemer, R., (1996). Application of ultrasonic irradiation for the degradation of chemical contaminants in water. Ultrason. Sonochem.3 (3), S163-S172

13

Ince.N, G. Tezcanli, R. Belen and G. Apikyan, (2001). Ultrasound as catalyzer of aqueous reaction systems: The state of art and environmental applications, Appl. Catal. B, 29, 167-176.

A typical range of optimum intensity of irradiation ( power dissipated per unit area of irradiating surfaces, W/cm 2) is 5- 20 W/cm2 which also dependet on the actual reactor system and the end application. The degradation of chemical compounds by acoustic cavitation is shown to involve three distinct pathways. The pathways include 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. Ultrasound is defined as any sound of a frequency above that to which the human ear has no response (i.e.above 16 kHz). In practice, 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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Reference

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Jia Lei Yong, Tian Yu, Fang Cheng, Zhan Wei, Duan Lu Chun, Zhang Jun, Zuo Wei, Wei Kong Xiao. (2019).Insights into the oxidation kinetics and mechanism of diesel hydrocarbons by ultrasound activated persulfate in a soil system. Chemical Engineering Journal, 378,122253

15

Kim, Y., and Wang M. C., (2003): Effect of ultrasound on oil removal from soils, Ultrasonics, vol. 41, 539542.

16

Kim, Y., Park J. H., Kim S. H., and Khim J., (2007). Ultrasonically enhanced diesel removal from soil. Japanese Journal of Applied Physics, Vol 46, No. 7B, 2007, pp. 4912–4914

17

Li J., Song X., Hu G., Thring R. W., (2013). Ultrasonic desorption of petroleum hydrocarbons from crude oil contaminated soils. Journal of Environmental Science and Health, Part A: Toxic/Hazardous Substances and Environmental Engineering, 48:11, 1378-1389

18

Lim, J.L., Okada, M., (2005). Regeneration of granular activated carbon using ultrasound. Ultrasonic Sonochemistry 12, 277-282

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Lim, M.H., Kim, S.H., Kim, Y.U., Khim, J., (2007).

Content 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. Another benefit of introducing US into soil system is it could promote the breaking down of soil aggregates, which is expected to enhanced the desorption of contaminants form soil (akin washing-off) and the diffusion of PS (persulfate) into soil aggregates (akin stirring), hence increasing the destruction efficiency. - The soil-flushing method enhanced by ultrasonic waves is a new technique that 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. - The effect of ultrasound on diesel removal from soils were investigated in this study. Laboratory soil-flushing experiments were 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. The great desorption enhancement by ultrasound on PHC fraction generally benefits from the concentrated high energy and the cavitation effect of ultrasound.

About 50 % of TCE was desorbed for 1 h. Because of sonochemical degradation of the 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. This study examine the degradation of

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Reference Sonolysis of chlorinated compounds in aqueous solution. Ultrasonics Sonochemistry 14, 93-98.

Lin Meiqing, Ning Xun-an, An Taicheng, Zhang Jianhao, Chen Changmin, Ke Yaowei, Wang Yujie, Zhang Yaping, Sun Jian, Liu Jingyong. (2016). Degradation of polycyclic aromatic hydrocarbons (PAHs) in textile dyeing sludge with ultrasound an Fenton processes : Effect of system parameters and synergetic effect study. Journal of Hazardous Materials, 30, 7–16 Little, C., Hepher, M.J. and El-Sharif, M. (2002). The sono-degradation of phenanthrene in an aqueous environment. Ultrasonics 40: 667-674

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Lu Y.F., Riyanto N., Weavers L. K., (2002). Sonolysis of synthetic sediment particles: particle characteristics affecting particle dissolution and size reduction, Ultrason Sonochem. 9, 181-188

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Luppachini Massimiliano, Mascitti Andrea, Giachi Guido, Tonucci Lucia, d’Alessandro Nicola, Martinez Jean, Colacino Evelina. (2017). Sonochemistry in nonconventional, green solvents or solvents-free reaction. Tetrahedron ,73, 609-653

Content chlorinated hydrocarbons. The degradation were analyzed as pseudo first order reactions and their reaction rateconstant were in the range of 10 -1- 10-3 /min. As we know, higher ultrasonic intensity in the reaction system would accelerate the reaction. The increase in the ultrasonic intensity could increase the number of active cavitation bubbles and also the size of the individual bubbles.

- In the study of the degradation of PAHs through ultrasonic irradiation, the 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 photospectrometry 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 However, degradation of contaminants following desorption would be expected to be highest with smaller particle sizes and 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. Accoustic waves that fall in the human hearing range (i.e ‘sonic’ waves) have frequencies that cover the 20 Hz-20 kHz interval. Below and above these extremes the ‘infrasounds’ and ‘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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Reference Mason, T. J. (2016). Ultrasonic cleaning: A historical perspective. Ultrasonics Sonochemistry, 29, 519– 523.doi:10.1016/j.ultsonch.2015.05.004

Content Perhaps the simplest method of estimating electrical power consumption by a cleaning bath 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 decontaminate heavy metals in dredged sediments, Journal Hazard Material, 85, 73-89

A maximum removal of 83 % was obtained for silt fraction when factor levels were at 1200 W 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.

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Mehrdadi Nasser, Kootenaei Farshad Golbabaei. 2018. An Investigation on effect of ultrasound waves on sludge treatment. 5th International Conference on Energy and Environment Research, ICEER

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.

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Merouani S, Hamdaoui O, Rezgui Y, Guemini M (2013) Effects of ultrasound frequency and acoustic amplitude on the size of sonochemically active bubbles—theoretical study. Ultrason Sonochem 20:815–819. https://doi.org/10.1016/j.ultsonch.2012.10.015

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Nguyen Tam Thanh, Asakura Yoshiyuki, Koda Shinobu, Yasuda Keiji. (2017).Dependende of cavitation, chemical effect, and mechanical effect thresholds on ultrasonic frequency. Ultrasonics Sonochemistry 39, 301–306

29

Park Beomguk.,(2017): Ultrasonic and mechanical soil washing process for the removal of heavy metal from soil. Ultrasonic sonochemistry, 640-645

It is quite clear that as the ultrasound frequency increases,the range of ambient radius for an active bubble becomes less wideness and the optimal ambient radius becomes smallest. This behavior was observed for all employed acoustic amplitudes. Experimentally, in addition to the size distribution decreasing with increasing acoustic frequency When cavitation is generate, OH radicals are released, that is why chemical effect is obtained in the solution. Below the electric input power of 2 W, the reaction rate is zero. Thereafter, the reaction rate increases with increasing electric power. - The sieved and dried soil sample was violently mixed with a washing liquid (0.5 or 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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Reference

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Peters D., (2001). Sonolytic degradation of volatile pollutants in natural groundwater: conclusions from a model study. Ultrasonics Sonochemistry 8, 221-226.

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Pham, T.D (2014). Ultrasonic and Electrokinetic Remediation of Low Permeability Soil Contaminated With Persistent Organic Pollutants. ISBN 978-952265-644-5. Lappeenranta University of Technology University Press: Finlandia

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Prabhu A. V., Gogate P. R., Pandit A. B., (2004). Optimization of multiple-frequency sonochemical reactors. Chem Eng Sci 59: 4991-8

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Romdhane M., and Gourdon C., (2002). Investigation in solid-liquid extraction: influence of ultrasound. Chem Eng J; 87: 11-9

Content 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. From the results obtained in pure and natural water contaminated by 1,2-DCA the following 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. On the other hand, as a novel and rapidly growing science, the applications of ultrasound in environmental technology hold a promising future. Compared to conventional methods, 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. - With the addition of another frequency using additional transducers, cavity sizes as well as the lifetime of the cavity are enhanced considerably with a relatively marginal drop in the collapse pressures and temperatures. Therefore, triplefrequency 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. It is clearly demonstrated that ultrasound ameliorates simultaneously the kinetics and the 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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Reference

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Saez, V., Esclapez, M.D., Bonete, P., Walton, D.J., Rehorek, A., Louisnard, O., Gonzalez-Garcia, J., (2011). Sonochemical degradation of perchloroethylene: the influence of ultrasonic variables, and the identification of products. Ultrasonic Sonochemistry 18: 104-113

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Sancheti Sonam V., Gogate Parag R., (2017). A review of engineering aspects of intensification of chemical synthesis using ultrasound. Ultrasonics Sonochemistry 36, 527–543 Shrestha R.A., Mudhoo A., Pham T. D., and Sillanpää M., (2012). "Ultrasound and Sonochemistry in the Treatment of Contaminated Soils by Persistent Organic Pollutants," in Handbook on Applications of Ultrasound: Sonochemistry for Sustainability, D. Chen, S. K. Sharma, and A. Mudhoo, Eds., FL: CRC Press Taylor & Francis Group, pp. 407-418

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Shrestha R.A., Pham T.D., Sillanpaa M., (2009): Effect of ultrasonic on removal of persistent organic pollutants (POPs) from Different types of soils. Journal of Hazardous Materials pp 871-875

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Son Y., Nam S., Ashokkumar M., Khim J., (2012). Comparison of energy consumption between ultrasonic, mechanical, and combined soil washing process. Journal Ultrasonic Sonochemistry, 19, 395398

Content transfer of the solute to the solvent, and also to the destruction of pores in which the solute can be trapped. We note major products of Cl- and CO2/CO, and also trichloroethylene (TCE) and dichloroethylene (DCE) at ppm concentrations as reported earlier. The formation at very low (ppb) concentration of small halocompounds (CHCl3, CCl4) and also of higher-mass species, such as pentachloropropene, hexachloroethane, is noteworthy. Cavitation generated using ultrasound can enhanced the rates of several chemical reactions giving better selectively based on the physical and chemical effects. Although ultrasonic applications in environmental areas are still in lab-scale and developing stage, they are growing rapidly, attracting more interest, because of the many advantages they offer environmental friendly (no toxic chemicals are used or produced), low 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 - The ultrasonic processors used in these experiments were UP100H with operating frequency of 30 kHz, power of 100Wfrom 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 The ultrasonic washing processs does not require external chemicals and can be considered as a “green” process. The mechanical mixing did not result in any 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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Reference

Content 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. First, this process could achieve high removal efficiency in a single attempt. Second, it could decrease the operating time markedly. In this study, the addition of 35 kHz ultrasound 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. - When a liquid is irradiated with high intensity sound or ultrasound, acoustic cavitation (the formation, growth, and implosive collapse of 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. Also, it is likely that continuous operation with high frequency irradiation leads to an erosion of the transducers surface. The power requirement for inception of cavitation events in a high frequency operation is also higher.

39

Son Y., Cha J., Lim M.; Ashokkumar M., Khim., (2011). J. Comparison of ultrasonic and conventional mechanical soil-washing processes for dieselcontaminated sand. Ind. Eng. Chem. Res., 50(4), 2400– 2407

40

Suslick K. S., (2001). "Sonoluminescence and Sonochemistry," in Encyclopedia of Physical Science and Technology, 3rd ed., R. Meyers, Ed., San Diego, Academic Press, Inc

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Sutkar V. S., and Gogate P.R., (2009). Design aspects of sonochemical reactors: techniques for understanding cavitational activity distribution and effect of operating parameters. Chem Eng J., 155: 26-36

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Swamy K., and Narayana K., (2001). Advances in Sonochemistry, 6, Theme Issue – Ultrasound in Environmental Protection, (Eds. Mason, T. J., and Tiehm A.), Elsevier.

Although there is plenty of experimental evidence that ultrasound improves leaching, the exact mechanism is not fully understood but a model has been suggested

43

Thangavadivel K., Megharaj M., Smart R. S. C., Lesniewski P. J., Bates D., Naidu R., (2011). Ultrasonic enhanced desorption of DDT from contaminated soils. Water Air Soil Pollut., 217(1–4), 115–125

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Vyas Shruti, Ting Yeng-Peng. (2018). A reviewof the application of ultrasound in bioleaching and insight from sonication in (bio) chemical processes. Resources, 7,3 Wang Jing, Wang Zhenjun, Vieira Carolina L.Z., Wolfson Jack M., Pingtian Guiyou, Huang Shaodan. (2019). Review on the treatment of organic pollutants in water by ultrasonic technology. Ultrasonics Sonochemistry , 55,273–278

In this study, using high-power low frequency ultrasound, heated slurries with anionic surfactant sodium dodecyl sulfate (SDS) were treated to enhance desorption of DDT from 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. The application of ultrasound in increasing the rate of chemical reactions, such as in chemical leaching, is widely accepted.

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Ultrasonic technology is a clean and efficient new treatment method for the degradation of toxic organic pollutants. Main factors affecting the process of ultrasonic degradation are ultrasonic frequency, intensity, dissolved gas,

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Reference

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Wood R. J., Lee J., Bussemaker M. J., (2017): A parametric review of sonochemistry: Control and augmentation of sonochemical activity in aqueous solutions.Ultrasonic Sonochemistry, 38, 351-370

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Wu J. M., Huang H.S., Livengood C. D., (1991). Development of an Ultrasonic Process for Detoxifying Groundwater and Soil: Laboratory Research. Annual Report. ANL/ESD/TM-32.

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Wulandari, M. and Effendi A. J., (2018). Proceeding of 5Th International Conference on Science and Applied Science (ICSAS) Effect of frequency and ratio solidliquid on ultrasonic remediation of petroleum contaminated soil (pp. 020120-1 - 020120-7). Published by AIP Publishing

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Zhang J., Li J., Thring R., Liu L., (2013). Application of Ultrasound and Fenton's Reaction Process for the Treatment of Oily Sludge. International Symposium on Environmental Science and Technology (2013 ISEST)

Content pH value, and temperature. Ultrasound, a sound field with frequency greater than ~20 kHz, has a plethora of applications in several actively researched areas

- Under such conditions, water decomposes into extremely reactive hydroxyl radicals (OH) and hydrogen atoms (H). During the 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 - A washing liquid was used to violently mixed the sieved and dried sample in the reactor. The dry soil mass was 300 and 100 g and the ratio of soil/liquid (mass/mass) was 1:3 or 1:10. Ultrasonic process, 28kHz and 48 kHz 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. - The ultrasonic probe was then placed into the sludge/water system for ultrasonic oxidation. The ultrasonic power was fixed 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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Reference

Content 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.

Zhao Y., Zhu C., Feng R., Xu J., Wang Y., (2002) Fluorescence enhancement of the aqueous solution of terephthalate ion after bi-frequency sonication. Ultrason Sonochem., 9: 241- 3

The fluorescence enhancement of the aqueous solution of terephthalate ion (TA) under orthogonal sonication of 28 kHz and 1.7 MHz 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.