Selecting sustainable approach for remediation of PFOA contaminated soils: AHP decision-making

doi:10.21203/rs.3.rs-3117302/v1

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Selecting sustainable approach for remediation of PFOA contaminated soils: AHP decision-making

https://doi.org/10.21203/rs.3.rs-3117302/v1

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Perfluorooctanoic acid (PFOA), which is an emerging persistent organic and one of the most commonly used PFAS, has a wide range of applications in industrial and production processes, and humans can regularly be exposed to it, so remediation of PFOA-contaminated soil is of great importance. This research presents the importance of PFOA soil pollution, soil remediation related technologies, their mechanisms and the order of remediation priority for three different hypothetical scenarios. Our comprehensive literature review shows that while some remediation methods have shown positive results, some, such as ultrasound, are ineffective in terrestrial ecosystems. Despite the fact that generally, the selection of a practical and compelling soil remediation technique depends on site assessments, our investigation and analysis by implementing an analytical hierarchy process and considering remediation time, environmental impacts, ecological impact, soil disturbance, post management, etc. as criteria, leads to the solidification/stabilization, oxidation, electrokinetic, phytoremediation and bioremediation as the most feasible and promising approaches for remediation of PFOA contaminated sites in our three suggested scenarios, but with different preferences. On the other hand, negative aspects of the electron beam, pulsed corona, and ball milling have placed them at the bottom of our selection list for field scale remediation.

PFASs

PFOA

Soil remediation

Soil decontamination

soil Contamination

Polyfluoroalkyl and perfluoroalkyl substances (PFASs) are amphiphilic emerging persistent chemicals with a high surface activity that some of them are listed in the Stockholm Convention on Persistent Organic Pollutants (POPs) and U.S. Environmental Protection Agency (USEPA) as a chemical of concern to human health (Askeland et al., 2020; Hou et al., 2022; Naidu et al., 2020; Sörengård et al., 2019; Xu et al., 2021). They are a class of fluorinated hydrocarbons that some of them have been increasingly reported for their extreme resistance to chemical and thermal degradation(Lehmler, 2005; Sörengård et al., 2021; Yu et al., 2020), long half-lives in the environment, bioaccumulation in food chains and plants(Liu et al., 2020; Stahl et al., 2013; Zhu et al., 2022), and health adverse effects(Bekele et al., 2020; Mccarthy et al., 2017) including, but not limited to, infertility, birth abnormalities, and a decrease in the immunological function of animals and humans (Betts, 2007; Grandjean and Budtz-Jørgensen, 2013; Hagenaars et al., 2013). PFASs have been widely and routinely used throughout the world for over sixty years(Zhu et al., 2022) in many industries (Zhan et al., 2020), household products(M B Ahmed et al., 2020), consumer products (Paul et al., 2009) and especially in the creation of aqueous film forming foams, also known as AFFF. However, as shown in Fig. 1, researches about PFASs before 2006 was rare, and after that, the number of articles dramatically increased, and over 12000 research has been done to date about these substances (Barzen-Hanson et al., 2017; Moody and Field, 2000; Place and Field, 2012; Turner et al., 2021; Yim et al., 2009) which probably is related to turning world wide attention to persistent organic pollutions as the results of Stockholm Convention entered into action on May 2004. Due to their high aqueous solubility and high mobility, these substances can be moved from polluted areas into the nearby soil, surface water, and groundwater; therefore, people can be exposed to them routinely(M B Ahmed et al., 2020; Aly et al., 2019; Eggen et al., 2010; Harris et al., 2022; Houtz and Sedlak, 2012; Shin et al., 2011).

Multiple PFASs have been identified in samples of human blood (Loi et al., 2013; Zhu et al., 2022) and, not only levels of perfluorooctanoic acid (PFOA) were much higher than almost all other PFASs(Xiao et al., 2015), but also during the national survey of U.S. this substance was identified in over ninety-five percent of blood samples(Liu et al., 2021). Therefore, PFOA attracted worldwide attention in the context of risk analysis (Wan et al., 2022). PFOA was listed in Stockholm Convention as a POP in 2019, and as shown in Fig. 1, researches on this substance have increased sharply since then. As shown in Fig. 2, PFOA (C₈HF₁₅O₂) is a long-chain amphiphilic PFAS with a strong carbon-fluorine bond and a molecular weight of 414.07 gr (Xiao et al., 2015; Yao et al., 2013). Its outstanding chemical and physical properties, including hydrophobicity, oleophobicity, and extraordinary chemical stability(Gong et al., 2016; Li et al., 2012; Loos et al., 2008), has led to its widespread use in polymerization aids (Yao et al., 2013), fast-food containers, water-resistant clothing, aqueous fire-fighting foams, painting materials, stain-resistant carpeting, surfactant, lubricants, wetting agents (Liu et al., 2021; Paul et al., 2009). Therefore PFOA can come from a variety of sources, including aqueous film-forming foams (Hodgkins et al., 2019; Houtz et al., 2013; Turner et al., 2021), landfill of PFOAs-containing wastes(Sepulvado et al., 2011), water and wastewater treatment plant sludge, biosolids or composts on agricultural lands (Jho et al., 2015; Röhler et al., 2021; Zhu et al., 2022), atmospheric wet deposition and manufacturing industries(Hou et al., 2022; Kewalramani et al., 2022; ).

Exposure to PFOA has been linked to a number of serious health problems, including thyroid illness(Melzer et al., 2010), genotoxicity, immunotoxicity, carcinogenicity, a disease known as attention deficit hyperactivity disorder (ADHD) in youngsters, and reduced immunological response to vaccines(Grandjean et al., 2012). In addition, numerous studies have pointed to a link between kidney and testicular malignancies and PFOA exposure as a possible causal factor. (Barry et al., 2013; Vieira et al., 2013). Although its manufacturing and usage have been restricted in line with the Stockholm Convention (Liu et al., 2022), not all countries have switched to safer alternatives, and PFOA is still in use in a few ones (Liu et al., 2021; Xu et al., 2022).

1.1. The importance of PFOA-contaminated soil remediation

Based on literature review it can concluded that, due to PFOA high and increasing frequency reports of detection in the ecosystem (Bao et al., 2012; Das et al., 2015; Houde et al., 2011; Loos et al., 2010; Turner et al., 2021), groundwater(Xu et al., 2021), agricultural soils(Xu et al., 2022), soil(Liu et al., 2022; Park et al., 2016; Wan et al., 2022; Xiao et al., 2015), strong C-F boning energy and environmental stability over the long time(Mohammad Boshir Ahmed et al., 2020; Harris et al., 2022; Xiao et al., 2015; Zhan et al., 2020), long-range atmospheric and oceanic transport(Ellis et al., 2004; Prevedouros et al., 2006; Shoeib et al., 2006), bioaccumulation capability, harmful effects on human and environmental health (Arias E et al., 2015; Liu et al., 2021; Moody and Field, 2000; Wilhelm et al., 2008) and over 2.7 years half-life for person exposed to contaminated water(Xu et al., 2021), PFOA which is one of the most representative, predominant and frequently substances in PFAS contaminated soil samples(Galloway et al., 2020; Hou et al., 2022; Lee et al., 2020; Rankin et al., 2016; Sammut et al., 2019), has raised many concern for soil remediation(Ren et al., 2018). However, to reinforce PFOA soil pollution's importance, we will also discuss our perspective in the following.

The above figure was obtained by visualizing the bibliography network by using VOS-viewer. Figure 3. (a). shows the average years of publications related to PFOA based on “term analyzes” which will be further explained in the material and methods section. It can be seen in Fig. 3(a) that not only the circle related to soil and groundwater has been shown with a low radius, but also, they have shown in yellow, which means these topics are the newest trends related to PFOA. As we can see in Fig. 3(b), many pieces of research are about PFOA water pollution, and soil is one of the most transparent points on the map, which means the number of research related to soil is low. These indicate a trend change in scientific research related to the remediation of PFOA, which can emphasize the importance of PFOA-soil pollution.

In addition, from our point of view, the focus on the water treatment approach and prevention of pollutant entrance to the human body through drinking contaminated water in early research had led to the neglect of remediation of soil media, which is an important sink for PFOA in the environment. As shown in Fig. 4, which provides the main sources and pathway of PFOA in the environment, soil connects the atmosphere to the hydrosphere and plays a crucial role in the transportation and accumulation of contaminants in terrestrial and aquatic systems. Especially knowing that the leaching of PFOA into groundwater can be very high and even reach 90% (M B Ahmed et al., 2020; Xu et al., 2021). In this regard, the high importance of removing, degrading, or even immobilizing the contamination in soil media is undeniable. It is generally because efficient and in-time remedial actions can prevent contamination infiltration into groundwater and reduce potential human health risks, especially where the society depends on groundwater; moreover, they also can decrease the adverse ecological effects of this pollutant.

1.2. Brief philosophy behind this research

Considering that most studies have been focused on lab-scale experiments and their advantages, extensive assessments of PFOA remediation approaches on a field scale are highly demanded. In addition, considering environmental impact, soil disturbance, noise, dust, etc. can make it more difficult to choose the right method for full-scale remediation.

Therefore, the objectives of this study were to (1) an overview of current remediation technologies for PFOA-contaminated soils, (2) assessments of scientific, economic, ecological, environmental, and social aspects of remediation technologies, (3) propose three hypothetical field-scale scenarios, (4) determining the best practices by using AHP decision-making approach as a multi-criteria decision-making method.

2.1. Data acquisition

The Web of Science databases were screened out in this review. These online databases provide the user with a wide range of options to search for papers. To construct a database of published studies on PFAS substances between 2000 to 2023, we retrieved related papers on Web of Science (WOS) on Feb 2023 by using the following general search items: title = (perfluoroalkyl or polyfluoroalkyl or PFASs or PFAS) or abstract = (perfluoroalkyl or polyfluoroalkyl or PFASs or PFAS) or keyword = (perfluoroalkyl or polyfluoroalkyl or PFASs or PFAS). The title, keywords, abstract, publication year, and authors were then imported to VOS Viewer, a widely used and publicly accessible tool for examining recurring themes and patterns in scientific publications. Moreover, the same procedure was used to collect manuscripts related to PFOA between 2000 and 2023, and 6160 documents were obtained. These papers indicate the number of publications about PFAS and PFOA without addressing any detail which can show the overall trends of publications about these substances.

2.2. Trends identifying

Text mining and machine learning, two approaches to qualitative and quantitative literature synthesis, were utilized by our team in order to determine the primary subjects that were covered in the publications that were included in our database. The "Term" analysis found in the VOS viewer was utilized to successfully complete this task. The entire paper's titles, abstracts, and keywords were accounted for in the analysis. Term analysis is more successful than typical keyword analysis for text content extraction, and the results are more comprehensive. (Chen, 2006; Mc Callen et al., 2019). Toponyms (like "USA" and "Texas") and often-used nouns and verbs were eliminated and the remaining ideas were sorted into categories, each of which stands for a distinct line of concept. We first implemented an overall visualization analysis to identify the shifts in concepts in our database from 2000 to 2023. Obtained density visualization helped us to figure out the concepts that did not take enough attention and the gaps in the research

2.3. Selecting the best remediation practices

United Nations Sustainable Development Goals (SDGs) aim to strike a balance between social, economic, and environmental demands, and the international community is constantly looking for new understanding of science, policy instruments, and other activities to help achieve these goals(Hou and O’Connor, 2020). In contrast to the focus of conventional remediation on the contaminated site and the human health concerns to site users, sustainable remediation considers the broader socio-economic implications of the cleanup. The term “ sustainable remediation” refers to an integrated strategy in which the environmental, social, and economic advantages of cleanup are maximized for every participant, both inside and outside of the site boundary, in both the present generation and the next(Hou et al., 2016; Hou and O’Connor, 2020; Song et al., 2018).

As mentioned in previous sections, there is a high demand for promising remediation of affected sites. While currently, a couple of remedial actions are technically examined, selecting the best practices for field-scale projects includes a variety of non-technical effective factors, and it could be challenging. After a broad investigation by the authors, and considering SuRf-UK indicators, social acceptability, soil disturbance, post management, sensitivity to pollution concentration, in-situ feasibility of the method and environmental impacts considered as non-technical but highly effective items for a comprehensive assessment. Due to the difficulty of accurately evaluating some of the Surf-UK indicators or their highly project-based nature, a few of the indicators are not considered, and some criteria of this research have considered several Surf-UK indicators simultaneously. Table 2 provides these criteria and indicators.

Table 2

Criteria considered in this research
This research’s criteria	SuRF-UK indicators	SuRF-UK indicators headlines
Cost	ECON1 ECON2	Direct economic costs and benefits Indirect economic costs and benefits
Time	ECON5	Project lifespan and flexibility
Soil Disturbance	ENV2 ENV3	Soil and ground conditions Groundwater and surface water
Post-Management	ENV5	Natural resources and waste
Ecological Impacts	ENV4	Ecology
Social Acceptability	SOC1 SOC2 SOC3 SOC4	Human health and safety Ethic and equality Neighborhoods and locality Communities and community involvement
Environmental Impacts	ENV1	Emissions to air
Sensitivity to Concentration	-	-
Deep remediation ability	-	-
Not considered in this research	ECON3	Employment and employment capital
Not considered in this research	ECON4	Induced economic cost

Due to the complexity of considering all mentioned criteria, overall assessment and analysis have been provided based on Analytic Hierarchy Process (AHP) as a multi-criteria decision-making technique. All AHP calculations, including the normalized decision matrix, weights of criteria, consistency ratio, and determining of the ideal solutions, have been done using Microsoft Excel^®. As mentioned, non-technical terms can be significantly affected by site assumptions; with respect to EPA contaminated sites categorization, the abovementioned Table 3 demonstrates the considered hypothetical scenarios.

Table 3

Scenarios information
Scenario number	Type of Sites*	Groundwater pollution probability
1	Small (abandoned buildings)	no
2	Large	no
3	Small/Large Sites	Yes
*EPA concurs that contaminated sites can range from abandoned buildings to large areas (U.S. Environmental Protection Agency, 2017)

Over the last decades, different multi-criteria decision-making (MCDM) techniques have been employed in studies concerning environmental engineering projects' planning, management, or policy assessment (Vassoney et al., 2017). MCDM is a technique that permits the development of an exhaustive comparison of alternatives based on their performances on various criteria for assessment(Cinelli et al., 2020; Neves et al., 2018). The three parts of MCDM are choices or options, criteria, and preferences. Alternatives are stand for possible actions that are assessed from multiple perspectives, criteria are these, and preferences display the value systems. One of the most frequently applied MCDM methods is AHP which was used for many sustainability assessments and environmental-related decision makings(Jiménez Capilla et al., 2016; Kumar and Katoch, 2015; Vassoney et al., 2021). Hence in this research, we use AHP as MCDM.

Developed by Thomas L.Saaty in the 1970s, the AHP is an effective tool that has been identified as one of the most reliable methods in scientific multi-criteria decision-making problems (Canco et al., 2021). The proposed methodology in this study consists of three main phases, including selecting alternatives and criteria, establishing a comprehensive decision matrix, and using the AHP approach to calculate the criteria’s weights and ranking remediation methods. Figure 5 shows the detailed flowchart of our approach toward finding efficient remediation methods.

Initially, and in the first phase, the process starts with defining the structure of the problem, goals, trends, gaps in previous studies, alternatives, results, and criteria. After that, the authors' judgments became the basis of determining the indexes and, subsequently, linguistic variables allocated to each remediation method. As we can see in Fig. 5, the third phase includes forming a pairwise comparison matrix based on criteria weighting scores, weight calculation of each criterion, calculation weights of remediation methods, and ranking methods. Establishing the pairwise comparison matrix is the first step of the last phase, and it is done by considering Eq. 1 and Saaty’s nine-point scale for pairwise comparison, which categorizes the importance ratio from the number 1 (indicating equal) to the number 9 (indicating the extreme importance of one parameter compared to the other.

$$\text{A}=\left[\begin{array}{ccccc}1& {\text{a}}_{\text{1,2}}& \cdots & \cdots & {\text{a}}_{1,n}\\ \frac{1}{{\text{a}}_{\text{1,2}}}& 1& \cdots & \cdots & {\text{a}}_{2,n}\\ ⋮& ⋮& ⋮& ⋮& ⋮\\ \frac{1}{{\text{a}}_{n,1}}& \frac{1}{{\text{a}}_{n,2}}& \cdots & \cdots & 1\end{array}\right]$$

The desirability of each criterion is one of the key points in these steps. In this regard, criteria are divided into positive and negative types, which are shown in Table 3.

Table 4

Negative and positive effects of each criterion
Criteria	Type of Criteria	Node No.
Time	Negative	1
Soil Disturbance	Negative	2
Post-Management	Negative	3
Ecological Impacts	Negative	4
Social Acceptability	Positive	5
Environmental Impacts	Negative	6
Deep remediation ability	Positive	7
Sensitivity to Concentration	positive	8

Weights of criteria which is the second step of the third phase, are obtained by normalizing the comparison matrix and averaging the values to obtain the corresponding rating. While the criteria weights are defined based on previous calculations, the consistency ratio should be checked to ensure a logical judgment of experts and prevent judgment conflict among the comparisons.

Table 5

Random Index values (Saaty, 1980)
n	1	2	3	4	5	6	7	8	9
Random index	0.00	0.00	0.58	0.9	1.12	1.24	1.32	1.41	1.45

Consistency ratio calculation approaches are provided in Eq. 2. Which, the${\lambda }_{max}$ is the maximum eigenvalue of the comparison matrix. RI is random consistency index values depends on the size of the matrix which are presented in Table 4, (Saaty, 1980). If the consistency ratio exceeds 10%, the criteria are assumed inconsistent, and the criteria values should be reconsidered.

$$\text{C}\text{I}=\frac{{{\lambda }}_{\text{m}\text{a}\text{x}}-\text{n}}{\text{n}-1}$$

$$\text{C}\text{R}=\frac{\text{C}\text{I}}{\text{R}\text{I}}$$

The consistency ratio should be checked to ensure the prevention of judgmental conflict among the comparisons. Therefore, if the CR exceeds 10%, the decision is assumed to be inconsistent (Taylor et al., 2007). After checking the consistency ratio is correct, obtained weight of each criterion should be applied to related values of every remediation method (alternatives), and then the sum of weighted elements of each row be calculated. Finally, the options should be ranked based on obtained values.

3.1. Brief philosophy behind the selection of criteria

Considering the complex decision-making and assessment of remediation techniques, selecting appropriate criteria has the highest importance in the whole process. In fact, selected criteria directly affect the final decision and ranking orders. In this study, the evaluation and selection of desirable criteria, which are done by the authors, are presented to give the reader an overview of why these choices were made. In the next sections, we categorized remediation approaches by considering their mechanisms, but from another point of view, we can divide them based on financial aspects, technical aspects, social impacts, soil security, environmental impacts, and administration.

Cost and time are the two main factors in selecting the right solution for all engineering issues, and without considering these factors, any evaluation and selection could encounter many errors. But, in contrast to time, which can be considered as a feature of technology, the cost depends on a variety of factors such as available technologies, available skilled workers, depth of the contamination, excavation difficulty in very loose or very compacted soils, need to create the access paths, disturbance in traffic, especially in the brownfield remediation, etc. So, considering cost is very site-specific, and in this research, we just considered time as a criterion. Social impacts as a qualitative factor mainly consist of how people conceptualize and interpret specific situations or events and how these interpretations influence their opinion. People's way of judging can be biased, strict, or contrary to the technical truth, but since they are the beneficiaries of all remediation projects, their opinion about a technology or chemical substance cannot be ignored. For instance, although using chemical additives can improve the efficiency of some remediation methods, regardless of whether the additives are environmentally friendly, the context of “chemical” can be worrying and could lead to public anxiety, especially in developing countries. In addition, aesthetically pleasing, low noise, and low dust emission methods with less heavy industrial equipment have more social acceptability. However, people are not aware of all aspects, and it is necessary to consider the views of macro policies like soil security. Soil security is a worldwide concept for maintaining soil resources which refers to soil management in such a way that none of the soil’s functions should be disturbed. Functions of the soil generally are identified by characteristics such as the ability to charge groundwater, preservation of plant/microbial ecosystems, the base of biomass production, etc. Obviously, any change in the natural structure of the soil (i.e., mixing, excavation, etc.) can disrupt these functions, so all of the ex-situ remediation methods not only have adverse environmental effects, such as transportation emissions and dust emissions, but also can threaten soil security. Although ex-situ remediation methods definitely change the structure and ecology of the soil, some of the in-situ methods also have adverse effects on these terms. Therefore, ex-situ and in-situ classifications are inaccurate and insufficient categorizations to consider the soil security factor of a remediation method, so soil disturbance and soil ecology disruption have been considered as two effective criteria in evaluating remediation methods that can impair soil security. Project complexity which can be affected by the type of remediation or the specific conditions of each project increases the probability of operational difficulty, operational mistakes, and environmental deterioration. For instance, remediation of a contaminated site with non-uniform distribution of pollution can adversely affect highly sensitive technologies and lead to more challenging project management. In addition, some remediation technologies generate highly contaminated wastewater or solid wastes, which must be disposed of or treated appropriately. So, we believe adding post management, sensitivity to pollution, and in-situ applicability is of great importance.

A deep understanding of PFOA remediation technologies requires knowledge about their mechanisms and the explanation of which can help to better understand the future discussion about the remediations. So, in this section, each of the immobilization, degradation, and plant uptake mechanisms, which is related to one or more of the remediation technologies, will be discussed.

4.1. Mechanisms of PFOA Immobilization

Adsorption has exhibited unique advantages, such as technological maturity and ease of operation, since the adsorption process is widely used in practical applications. The term "adsorption" refers to a phenomenon in which molecules of adsorbate migrate to a solid surface (Uriakhil et al., 2021). This occurs via four consecutive phases: bulk diffusion, external diffusion, intraparticle diffusion, and interaction with surface sites. After intraparticle diffusion and in the last step, adsorbates would engage with surface locations through either physical force or chemical bonding. Physical forces include electrostatic or hydrophobic interaction. PFAS ions engage with charged surface groups through electrostatic interactions, while PFAS hydrophobic interactions with surfaces originate predominantly from the perfluoroalkyl chains.

4.2. Mechanisms of PFOA degradation

4.2.1 Advance oxidation

Complete pollution destruction is the goal of several promising technologies that have arisen in the last few decades. These include advanced oxidation processes (AOPs), advanced reduction processes (ARPs), and combination AOP/ARP systems(Flores et al., 2007; Gu et al., 2017; Sarasidis et al., 2017; Xiao et al., 2017). Photolysis, photochemical, photocatalysis, cavitation, electrochemical, and sonochemical (ultrasound) processes constitute some of the common AOPs (Gągol et al., 2018; Ltaïef et al., 2017). One of the characteristics that distinguishes AOPs from ARPs is the former's capacity to produce highly oxidizing hydroxyl (•OH) and/or sulfate radicals (SO₄^•) (Khan et al., 2017; Wang and Wang, 2018), whereas the latter generates the extremely reducing hydrated electron (eaq). In the majority of situations, the AO/RPs are the ones responsible for the generation of both oxidizing and reducing species, such as •OH, eaq, and/or hydrogen radical (H^•)(Khan et al., 2019). The kinds of reactive radicals produced are determined by the AO/RP that was utilized in the reaction. Oxidizing hydroxyl is produced by the vast majority of AO/RP processes, including but not limited to ionizing radiation, UV photolysis, photocatalysis, ozonation, and electrochemical technique. It is generally agreed that SO4•, eaq, H•, and SO3• are the other reactive species that are formed in the AO/RP process(Khan et al., 2019, 2017; Wang and Wang, 2018).

4.2.2 Mechanochemical

Mechanochemical (MC) is an assuring technique for organic pollutants’ breakdown in solid media. In this clean up method, the reactions typically commence with crushing of particles, the breakdown of bonds, heating, etc., in the face of severe mechanical pressure which can be enhanced with the addition of suitable chemicals (Huang et al., 2016; Liu et al., 2016; N. Wang et al., 2019). The reductive environment produced by ball milling results in the release of electrons and the formation of reactive species. This approach generates free electrons and reactive radicals, leading to electron addition and radical PFAS. C-C bond breaking is likely to occur as a result of subsequent reactivity with free electrons and reactive radicals, leading to the release of the head group and subsequent defluorination. It is highly improbable that PFAS degradation follows a thermal breakdown mechanism, despite the high temperatures that can be created during remediation process. After the removal of the PFOA head group, the C-F bonds more susceptible to breaking because the fluorine atoms on the carbon chain can break out of a tight shape more easily.

4.2.3 Biodegradation

Although many organic contaminants can be degraded by microorganisms and eliminate from polluted soils and groundwater, it can be stated that the soil microbiome plays a crucial role in the biodegradation of PFAS. For instance, while E. coli was found to be incapable of biodegrading PFOA and PFOS by Pasquini et al., capability of yeasts and molds and chemoorganoheterotrophic bacteria, which can moderately decrease the concentration of these compounds is proven (Beškoski et al., 2018; Leung et al., 2022). In this method, enzymes that can add oxygen across the F-C bond, i.e. oxidation, or can add electrons across the F-C bond, i.e. reduction, are involved in the biodegradation of PFAS. This would then allow other normal assimilation enzymes to break down the rest of the compound. (Shahsavari et al., 2021; Tiedt et al., 2017).

4.3. Mechanisms of PFOA extraction

PFASs have strong resistance to degradation; therefore, in many cases, we have to utilize intensive methods for the remediation of polluted soil, which can adversely affect soil structure and microorganisms. Extracting contamination from soil media without soil distribution provides the capability of degrading the extracted pollution in a separate isolated, controlled experiment without soil distribution. Plant uptake and electric current are two extraction methods that have been used for soil remediation.

4.3.1 Plant uptake

Chemicals can be taken up by plants in two ways: actively and passively. Passive uptake is driven by mass flow or diffusion in response to a potential energy gradient, while active uptake requires expending energy to mediate via carrier proteins (such as water channels or anion channels). Fick's first law can be used to characterize carrier-independent passive processes, such as the diffusion of substances through a semipermeable membrane. Researchers have found that PFASs are taken up by terrestrial crops through both active uptake and passive transport(M. Wang et al., 2019; Wang et al., 2020; L. Zhang et al., 2019). PFOA in the soil may be taken up by the plant's roots and distributed to the stems and leaves. The accumulation of PFOS and PFOA in the leaf occurred continually as the transpiration flow moved from the stem to the leaf and the water evaporated(Ju et al., 2019; Wild et al., 2005).

4.3.2 Electrical gradient

Utilizing electrical gradient in soil media can mobilize PFOA, mainly via electromigration and electroosmosis mechanisms. Electromigration refers to the transportation of contaminants due to an electric field, with cations and anions moving toward the cathode and anode, respectively. Electroosmosis, or electroosmotic flow (EOF), refers to the drag of water molecules resulting from the electric field and is typically directed toward the cathode in a negatively charged soil matrix(Niarchos et al., 2022).

Due to resistance to degradation and low volatility, remediation of PFOA-contaminated soil using many conventional remediation methods (Schultz et al., 2006; Xu et al., 2021), such as sparging, soil vapor extraction, natural biodegradation under aerobic and anaerobic conditions is challenging (Fujii et al., 2007; Liou et al., 2010; Schultz et al., 2003; Turner et al., 2021; Vecitis et al., 2009). In recent years, research has been done about the degradation of PFOA in aqueous media. Still, these studies examined technologies that may suffer from lacking cost-effectiveness and appropriateness for use in soil media (Turner et al., 2021). Furthermore, researches focusing on the remediations of PFOA-contaminated soils is very rare (Luo et al., 2018). So, it can be claimed that there is a huge need for examining and developing technologies for the remediation of PFOA-contaminated soils. We have divided all remediation approaches into four different categories based on their strategy, including immobilization, extraction, degradation, and combined. While extraction approaches can be used to separate contaminants from soil media and immobilize methods to reduce pollution's mobility into the next media, degradation can eliminate or decompose the contaminant.

5.1. Solidification and stabilization

While this method can be considered a destructive approach, which immobilizes the pollution, not remediate it, its fantastic efficiency, lack of wastewater or solid waste generation, and no need for excavation, transport, and refilling are incredible advantages. As this method can be done with ordinary construction machinery, in comparison with other technologies, the effective depth of this in-situ technology can be very long. Turning a contaminated field into a confined matrix could make it a less publicly acceptable method, but using engineered capping which can turn this field into a safe new land use, including new buildings, entertainment centers, parks, etc. Although its severe adverse effect on soil ecology is a huge disadvantage of this method, it seems when it is necessary to reduce the leaching of pollution to groundwater as soon as possible; this method can be a great solution.

5.2. Persulfate oxidation

Sonolysis(Cheng et al., 2010), photocatalysis(Dillert et al., 2007), and UV photolysis are only a few of the advanced oxidation processes (AOPs) that have been proven to effectively degrade PFOA(Giri et al., 2011). Persulfate (S₂O₈^2-), a strong oxidant that can produce free sulfate radicals, is an oxidation technology feasible for field-scale PFOA-contaminated soil remediation. It has been expected that the oxidation of PFOA by heat-activated persulfate will take place along a straightforward unzipping pathway, shown in Fig. 7 (Park et al., 2016). However, due to different reactions with soil organic matter or mineral surfaces, the effectiveness of this technology for the remediation of PFOA in soil media is reduced. Another drawback is that one-phase injection is insufficient for in-situ PFOA-contaminated soil remediation, and injections must be performed multiple times to completely remove PFOA.

5.3. Pulsed corona discharge plasma

Non-thermal plasma (NTP), which is an overwhelmingly competitive remediation method (Mededovic Thagard et al., 2016), uses a high voltage to generate a sequence of free radicals, such as electrons, active species, and other free ions, in order to oxidize or deoxidize pollutants(Liu et al., 2012) without needs to injection of chemicals for producing active species(Bai and Zhang, 2017; Liu et al., 2018). Collisions between high-velocity electrons created by the high voltage and other species within the electric field result in the formation of radical species, which can destroy the pollutant(Singh et al., 2019; Zhan et al., 2020).

While this method can be an effective approach, which does not generate wastewater or solid waste, its need for excavation, transport, and refilling cause extreme disturbance in soil structure; on the other hand, the effective depth of this technology is low, which turn this approach a time-consuming method, especially for remediation of a large volume of contaminated soil. In most cases, the long period of remediation not only makes it an inefficient strategy for contaminated sites in demand of urgent remediation but also a negative term for public acceptability. In addition, severe adverse effects on soil ecology are another disadvantage in this regard. The mentioned drawbacks bring to mind that this method may not be a proper approach.

5.4. Ultrasound

Low-frequency ultrasound, which can just cause physical with little or no degradation effects and promote the desorption of contaminants like PAHs and PCBs from solid-liquid systems (like soil and sediment), has been used in many researches(Effendi et al., 2019; Kohan et al., 2022; Lei et al., 2020). In contrast with low-frequency, high-frequency ultrasound (between 500 kHz and 1000 kHz) causes the production of nanobubble(Kewalramani et al., 2022; Kohan et al., 2022). Using a low-frequency ultrasound can be a powerful approach for the desorption of PFOA from soil media, but high-frequency ultrasound is not able degradate PFOA. There can be two explanations for this happening, first, prevention of the high-frequency ultrasound sonochemical activity due to wave scattering and attenuation by the soil particles in the system, and second, prevention of PFOA formation at the bubble-liquid interface due to electrostatic repulsion between the negatively charged soil and the nanobubble surfaces. Therefore, soil-nanobubble interactions severely restrict the efficacy of sonochemical degradation of PFAS in soil slurries (Kewalramani et al., 2022)

While theoretically, using ultrasound can degrade PFOA in soil media, mentioned explanations shows that ultrasound is incapable of remediation PFOA-contaminated soil.

5.5. Electron beam technology

The electron beam (e-Beam) method utilizes compact electron accelerators to produce a variety of high-energy electrons from a power supply and has the ability to alter the status quo because it utilizes concurrent reduction and oxidation reactions (Ponomarev and Ershov, 2020). The electron beam technique, which can be implemented as an ex-situ method, generally is considered a highly efficient process; however, this method could have severe adverse effects on soil ecology, which requires more research in this regard. The electron beam mechanism has advantages and disadvantages at the same time; the absence of solid or liquid waste at the end of the remediation process is one of the most obvious positive points of this method, which makes it possible to manage it without the need for post managing, however, high soil disturbance and subsequently, low social acceptability are their main drawbacks which also originates from its mechanism. Although this method has other advantages, such as a high remediation rate of saturated soil, mentioned drawbacks indicate that this method probably has a low score in our selection.

5.6. Ball milling

Although mechanochemical processes for the removal of organic contaminants using ball milling were first realized on chlorinated compounds such as polychlorinated biphenyls (PCB) and dichlorodiphenyltrichloroethane (DDT)(Ren et al., 2015; Sui et al., 2018; Wang et al., 2014) it also can remove PFOA substances from contaminated soil. While ball milling can be a highly efficient technology that can degrade PFOA uniformly, its adverse effects on soil structure and ecology could be very disappointing. In addition, excavation, transportation, and refilling, which require heavy machinery and are inseparable components of this remediation method, not only make project management more difficult but also, in most cases are along with low social acceptability. On the other hand, the absence of solid or liquid waste at the end of the remediation process is one of the most obvious positive points of this method, which makes it possible to manage it without the need for wastewater treatment or solid waste management. Although mentioned advantages can draw attention, it is clearly predictable that its drawbacks make this method one of the low chances nominates for site remediation.

5.7. Bioremediation

It has been demonstrated that persistent pollutions like PFOA can be degraded via the Laccase-mediator system(Luo et al., 2018). A biological method for degradation would serve as a cheap and effective remediation (Harris et al., 2022). The use of enzymes to catalyze oxidative processes in soil remediation may have the potential to gain benefits from the fact that enzyme sorption on soil can increase soil stability, making it more resistant to the fluctuations of the surrounding environment than its free form. The bioremediation technique, which can be implemented as an in-situ or ex-situ method, generally is considered an environmental-friendly process; however, finding site-compatible species with no ecological adverse effects could be challenging. Its nature base instincts have advantages and disadvantages; at the same time, it makes this method highly socially accepted; however, its time-consuming and high sensitivity to contaminant concentration are their main drawbacks which also originate from its instincts. Sensitivity to contaminant concentration can dictate the employment of skilled labor, local and close monitoring, especially in vast areas. Because it is necessary to check the death and life of the species and their remediation ability during the process, and if needed, several doses should be used locally or generally. On the other hand, the absence of solid or liquid waste at the end of the remediation process is one of the most obvious positive points of this method, which makes it possible to manage it without the need for post-managing. Although mentioned drawbacks prevent the selection of this method in situations where a high speed of remediation is needed, it's clearly predictable that this method is one of the high chances nominates for small area lands.

5.8. Phytoremediation

Phytoremediation, which refers to using the plant for remediation of contaminated media, consists of plant uptake and accumulation and can provide an eco-friendly and efficient to manage emerging contaminants like PFOA at the field scale(Huff et al., 2020; D. Zhang et al., 2019; Zhu et al., 2022). Compared to bioaccumulation, the degradation rate of PFOA in phytoremediation is much lower, and, in this study, we assumed it as an extraction-based method. One of the most important aspects that can affect the phytoremediation of the PFOA process is the effect of contaminants on seedling germination and root function. For instance, (Zhou et al., 2016) observed that 800 ppm PFOA contaminated soil stimulatory affected seedling growth and root length of wheat and inhibited root and shoot growth, which can extremely affect the phytoremediation.

While phytoremediation can be an environmental-friendly approach, which does not need skilled labor, finding a proper plant species with a high capability of PFOA uptake that which do not become invasive species could be challenging. On the other hand, the phytoremediation process is time-consuming, and the survival of desired species in severe weather conditions is highly important, especially if the chosen plant can’t remain evergreen; the required time will increase so much that it does not seem appropriate. In most cases, the long period of remediation not only makes it an inefficient strategy for contaminated sites in demand of urgent remediation but also is challenging to prevent animals from feeding on contaminated plants during phytoremediation, which can bioaccumulate in their body, disrupt ecosystem cycles, and even entering the human body. Moreover, managing polluted shoots and leaves as extremely polluted solid waste can be considered an important term that dictates the significant need for post-management. Mentioned drawbacks may require additional cost, labor, and management, especially for large contaminated sites.

5.9. Electrokinetic

Electrokinetic is a promising non-invasive remediation technology(Yeung and Gu, 2011) and involves applying an electric field to contaminated media. This method is capable of successfully removing various pollutants, such as heavy metals (Jensen et al., 2007) and a variety of organic contaminants(Guedes et al., 2014; López-Vizcaíno et al., 2017; Yusni and Tanaka, 2015) like PFOA from soil media (Sörengård et al., 2019). Four main mechanisms of electrokinetic affect pollutant extraction in an electrokinetic practice; among them, electroosmotic and electromigration are the dominant process in the mobilization of the PFOA in soil media. Electroosmosis refers to water transport toward the cathode, which can also mobilize PFOA. Conversely, due to PFOA negative charge (mainly as an anion in the environment), electromigration will refer to the mobilization of PFOA toward the anode(Ganbat et al., 2022; Sörengård et al., 2019). Therefore, PFOA is influenced by both of these flows with opposing transport vectors.

As mentioned before, there is a huge possibility of PFOA transportation in groundwater, so electrolyte, which is used in most electrokinetic remediation cases, can significantly increase the potential of leaching. In addition, it should be collected and treated as a contaminated fluid; hence, implementing the electrokinetic remediation method needs post-management. While we can consider the demand for on-site or off-site contaminated electrolyte treatment as a negative point, if we can prevent contamination of unpolluted media through leachate or spill of electrolyte management, it is just a negligible factor. In addition, one of the most desirable features of the electrokinetic technology is that higher current does not necessarily result in better PFOA transportation, and; decent quality of remediation can achieve with a low current gradient and even using solar cells, which makes this remediation technique more cost-effective and energy efficient. Considering that electrokinetic is in-situ remediation without very low disturbance in soil structure and very low adverse effects on soil ecology, it is almost an environmental-friendly technology, especially for field scale usage. It can be clearly predictable that electrokinetic remediation is one of the nominated of choosing best practices.

As previously mentioned, due to resistance to degradation and low volatility, remediation of PFOA-contaminated soil using many conventional technologies is challenging (Fujii et al., 2007; Liou et al., 2010; Schultz et al., 2003; Turner et al., 2021; Vecitis et al., 2009) and researches focusing on the remediations of PFOA contaminated soils are very rare (Luo et al., 2018). In addition, most of the research has been done without considering sustainability criteria. Some of these criteria are very site-specific, and we did not consider them in the AHP ranking system.

According to the weights calculated by AHP, the ranking values of the candidate remediation technologies were obtained. The scores of alternatives for three hypothetical scenarios derived from the AHP method are presented in Fig. 10 and Fig. 11. The results showed that in Scenario 1, oxidation, solidification, and electrokinetic are the most appropriate alternatives. For scenario 2, phytoremediation, bioremediation, and solidification are the top-ranked technologies. In scenario 3, oxidation, solidification, and electrokinetic received the highest scores.

It seems that the greater importance of ecological factors, soil disturbance, and social acceptability for the remediation of vast sites compared to small sites, which is considered in our calculations, is the reason why biological methods are preferred over other methods, especially in scenario 2, which groundwater contamination has not been taking to account. In the first scenario, the time and post-management advantages of some methods have been overcome by biological methods, and the rank of the phytoremediation method has been reduced to 4. Although these methods can have more destructive effects than biological methods, due to the small size of the site and the limited and very local effect, these cases can be neglected. In the third scenario, the occurrence of underground water pollution requires the need for purification as soon as possible. In this scenario, destructive methods or those that require excavation may be chosen as better options than biological methods. It seems that the reason for this is that the first priority is to remediate in the fastest time, and the second priority is the social acceptability of the remediation. Providing uncontaminated water for irrigation, livestock breeding, and drinking as soon as possible is more important than soil disturbance or emission into the air.

This article aims to not only provide a summary of pertinent information regarding remediation technologies for PFOA-contaminated soils but also determine the priority of remediation methods. Generally, the soil's organic content, water content, time constraints, cost of remediation, and in-situ remediation capability are the primary factors influencing the selection of a remediation technique. For instance, in projects which include soil with high water content and there is no time constraint, phytoremediation is probably the best method for remediating PFOA-contaminated soils. On the other hand, oxidation could be the most effective option when PFOA leakage into groundwater must be reduced as soon as possible. Besides, Electrokinetic is the most effective technique for in-situ degradation and mobilization of PFOA in soil media and the desired direction or into the specific zone of a polluted area. While ultrasound is not capable of PFOA-contaminated soil remediation, when soil disturbance is not an issue, ball milling is one of the most effective methods for remediating PFOA-contaminated soils because with this technology because remediation of a large volume of contaminated soil can easily be achieved in a short period of time. In summary, achieving promising remediation techniques to overcome PFOA pollution in soil could be determined by extensive research on contaminated site assessment and detailed studies on PFOA and its synergy effects with other PFAS compounds in the future.

In addition to technical factors, choosing the appropriate method for remediation of a contaminated site depends on many terms like environmental impact, ecological impacts, time consumption, etc. For instance, ball milling, pulsed corona discharge, and electron beam can degrade PFOA in soil media, but excavation and refill can extremely disturb the soil. Mentioned drawback of technologies that need excavation makes them alternatives with extremely adverse effects on soil structure and the local ecology of the area. Considering the three hypothetical scenarios and AHP calculations that have been done, oxidation, solidification, and electrokinetic are the first priorities that should be considered to clean up any PFOA-contaminated site.

Declaration of interests
The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper.

Funding information

This research received no specific grant from any funding agency.

Author Contributions Statement:

Mehdi Soltanian: Conceptualization, Methodology, Data gathering, visualization, Writing - Original draft preparation, Writing-Review.

Saba Salmak: Methodology, Writing - Original draft preparation.

Majid Baghdadi: Supervision, Reviewing, and Editing.

Saeid Gitipour: Supervision.

Hamed Lamei Ramandi: Supervision.

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No competing interests reported.

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Selecting sustainable approach for remediation of PFOA contaminated soils: AHP decision-making

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Abstract

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1. Introduction

1.1. The importance of PFOA-contaminated soil remediation

1.2. Brief philosophy behind this research

2. Methods

2.1. Data acquisition

2.2. Trends identifying

2.3. Selecting the best remediation practices

3. AHP methodology

3.1. Brief philosophy behind the selection of criteria

4. Immobilization, degradation, and extraction

4.1. Mechanisms of PFOA Immobilization

4.2. Mechanisms of PFOA degradation

4.3. Mechanisms of PFOA extraction

5. PFOA remediation overview and discussion

5.1. Solidification and stabilization

5.2. Persulfate oxidation

5.3. Pulsed corona discharge plasma

5.4. Ultrasound

5.5. Electron beam technology

5.6. Ball milling

5.7. Bioremediation

5.8. Phytoremediation

5.9. Electrokinetic

6. AHP results

7. Conclusion

Declarations

References

Additional Declarations

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