Journal of Environmental Management 283 (2021) 111977

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Journal of Environmental Management

journal homepage: http://www.elsevier.com/locate/jenvman

Review

Comparison of currently available PFAS remediation technologies in water:

A review
Dushanthi M. Wanninayake
Faculty of Health Engineering and Science, University of Southern Queensland, Toowoomba, QLD, 4350, Australia

A R T I C L E I N F O A B S T R A C T

Keywords: Remediation of Poly- and perfluoroalkyl substances (PFASs) in the environment has rapidly increased due to
Poly- and perfluoroalkyl substances (PFASs) growing concerns of environmental contamination and associated adverse toxicological effects on wildlife and
Remediation humans due to bioaccumulation and extreme persistence. Although, PFASs are highly recalcitrant to conven­
Sonochemical
tional water treatment processes, there are some effective techniques available. Those techniques involve
Hybrid
exceedingly high costs due to high energy use, and high capital or operational costs. Thus, most remediation
Groundwater
Water techniques have limitations in field applications even though the laboratory scale experiments are promising. As
a result of stringent new health and environmental regulatory standards are being established, development of
suitable water treatment methodology is more challenging. Most of the separation and destruction techniques
have their own limitations in field applications while the biological approaches to treat PFASs are extremely
limited and are not currently considered as viable. In this review, extra consideration is given to novel advanced
techniques for wide array of PFAS classes including short chain PFAS removal, and compare their efficiencies,
effectiveness, energy use, sustainability, cost, and simplicity in laboratory scale to field applications. Electro­
chemical, sonochemical, advanced oxidation processers (AOPs) and plasma together with novel hybrid tech­
niques are considered as effective approaches for PFASs removal and have shown promising results for long chain
and some short chain PFASs, as well as extremely persistent per-fluoro alkyl acids (PFAAs). Therefore, it is
essential to better understand the removal mechanisms to optimise the advanced treatment processes like hybrid
techniques because, the unique physicochemical characteristics of various PFASs impose difficult challenges.
Careful selection of a combined effective treatment methodology in an integrated processing unit, would be a
revolutionary approach for complete elimination of PFASs from the environment. Considering the site-specific
water quality parameters together with community perspectives will also make it more viable in real world
field applications.

(Brendel et al., 2018; Johnson et al., 2007; Wang et al., 2017). Due to
their unique chemical properties and stability in the environment and in
1. Introduction
the higher organisms, they are recognized as ubiquitously persis­
tent/forever chemicals and are found in humans and ecosystems.
1.1. Introduction to PFASs
Therefore, more regulatory attention to this new class of emerging
contaminants is becoming a high priority. There are thousands of “PFAS
Poly- and perfluoro alkyl substances (PFASs) are predominantly
precursors”, which can transform in the environment and in higher or­
fluorinated anionic surfactants consisting of straight chain or branched
ganisms to create persistent perfluoroalkyl acids (PFAAs), such as PFOA
alkyl groups, with over 3000 individual synthetic organic chemicals that
and PFOS. As such, new health and environmental regulatory standards
have been made and used since the 1950s (Brendel et al., 2018; Johnson
are being established predominantly for PFOA and PFOS, in the parts per
et al., 2007; Wang et al., 2017). There are many PFASs those are
trillion (ppt) levels, see Table 1 below.
structurally similar to that of PFOS and PFOA or their precursors, still
A book chapter “Micropollutants and Aquatic Environment” written
being produced in large quantities, and are overlooked (Wang et al.,
by Stasinakis and Gatidou (2010) in “Treatment of Micropollutants in
2017). This class of chemicals has unique properties such as chemical
water and wastewater” describes that the major manufacturer phased
stability, water, oil and grease repellent, resistance to heat and as well as
out their PFOS production in 2002 and decreased the global production
hydrophobic - lipophobic tendencies with amphiphilic properties

E-mail address: dushanthi.wanninayake@usq.edu.au.

https://doi.org/10.1016/j.jenvman.2021.111977
Received 21 September 2020; Received in revised form 7 October 2020; Accepted 8 January 2021
Available online 28 January 2021
0301-4797/© 2021 Elsevier Ltd. All rights reserved.
D.M. Wanninayake Journal of Environmental Management 283 (2021) 111977

Abbreviations AC Activated Carbon

GAC Granular Activated Carbon
AFFF Aqueous film forming foam PAC Powdered Activated Carbon
PFAA Perfluoroalkyl acid CNT Carbon Nano Tube
PFAS Poly and perfluorinated alkyl substance IXR Ion Exchange Resin
PFCA Perfluoroalkyl carboxylic acid GIC Graphite Intercalated Compounds
PFSA Perfluoroalkyl sulphonoic acid EG Expandable Graphite
PFBA Perfluorobutanoic acid HMS High surface area mesoporous silica
PFPeA Perfluoropentanoic acid NOM Natural Organic Matter
PFHxA Perfluorohexanoic acid RO Reverse Osmosis
PFHeA Perfluoroheptanoic acid NF Nanofiltration
PFOA Perfluorooctanoic acid AOP Advanced Oxidation Process
PFOS Perfluorooctanesulfonoic acid ARP Advanced Reduction Process
PFBS Perfluorobutanesulfonoic acid UV Ultra Violate
PFHxS Perfluorohexanesulfonoic acid O3 Ozone
PFC Perfluoro carboxylate CO2 Carbon dioxide
POP Persistent Organic Pollutant ppt parts per trillion
Ti4O7 Titanium suboxide TOP Total Oxidisable Precursor
Cr2O7 2- Dichromate EO Electrochemical Oxidation
MnO2-4 Permanganate FPG Few layered porous graphite
ClO2-
4 Perchlorate H2O Water
.
H2O2 Hydrogen Peroxide OH Hydroxyl radical
H2SO4 Sulphuric acid

1.2. PFAS environmental chemistry and toxicology

Table 1
The health-based guideline values use in site investigations in Australia.
Health based guideline values Total (PFOS + PFOA
PFHxS)
ng μg ng
Tolerable daily intake (ng or μg/kg bw/day) 20 0.02 160
Drinking water quality value (ng or μg/L) 70 0.07 560
Recreational water quality value (ng or μg/L) 2000 2.0 10,000
Note: ng-nano grams; μg – micro grams; kg – kilo grams; L – litre; bw – body
weight.
Source: (Australian Government Department of Health, 2019) with permission
of PFOS from ~3500 metric tons in 2000 to ~175 metric tons in 2003.
However, the global production of PFOA increased from ~500 metric
tons in 2000 to ~1200 metric tons in 2004 (Stasinakis and Gatidou,
2010). Investigation in 2009 suggests that organic micropollutants in
European rivers, contain PFOA and PFOS in 97% and 94% (Stasinakis
and Gatidou, 2010) of samples tested, respectively. Contaminant
transport mechanism were described under two hypotheses: the oceanic
current and the atmosphere transport of volatile PFAS.
Commonly used PFASs are classified under three subclasses: per­
fluoroalkyl sulphonoic acids (PFSAs), perfluoroalkyl carboxylic acids
(PFCAs) and fluorotelomer-based substances (precursor compounds)
(Brendel et al., 2018; Wang et al., 2017), see Fig. 1 below. Their
high-energy C–F bond structure make them resistant to hydrolysis,
photolysis, biodegradation, and metabolic processes in living organisms
(Dufkova et al., 2012). That makes them the ideal choice for use in
several commercial applications like stain repellents, non-stick cook
ware, food packaging, waterproof and fire-resistant fabric and
fire-fighting foams also known as ‘aqueous film-forming foams (AFFFs)
(Anumol et al., 2016).
Those firefighting foams were used extensively in Australia and
worldwide since the 1970s, in firefighting training and operations in
airports, fire brigade training grounds and industrial facilities where
large volumes of flammable materials are stored and handled, until
being phased out more than a decades ago. This has resulted in envi­
ronmental contamination including human and wildlife.
PFASs are now widespread and have been found in the environment
in relatively high concentrations particularly in surface and ground­
water, humans, and animals worldwide (U.S. Department of Health and
Human Services, 2019). In recent years some of the PFAS chemicals have
μg
been recognized as toxic and bio accumulative chemicals due to their
0.16
stability in the environment (Anumol et al., 2016; U.S. Department of
0.56
10 Health and Human Services, 2019; Wang et al., 2019). Studies in aquatic
organisms and their surrounding water bodies showed that concentra­
tion of PFOS in benthic invertebrates were 1000-fold higher than the
water suggesting bioaccumulation; however, no acute toxicity of PFOS
and PFOA has been observed (Stasinakis and Gatidou, 2010). There are
various potential health effects that have been attributed to PFAS
exposure, particularly perfluorooctane sulfonoic acid (PFOS) and per­
fluorooctanoic acid (PFOA) which are highly toxic and suspected car­
cinogens. In response, regulatory attention has recently increased, and
health-based guidelines were developed, see Table 1 below. Currently
PFOS and PFOA and their salts are listed in the Stockholm Convention
under Persistent Organic Pollutants (POPs) as highly restricted chem­
icals while PFHxS is also recommended for listing in October 2019
convention and will be considered by the next Conference in 2021
(Sinclair et al., 2020; UNEP Stockholm Convention, 2020; Wang et al.,
2019).
As an alternative to long chain perfluorinated alkyl acids (PFAAs),
short chain PFASs (i.e. GenX and PFBS replaced PFOA and PFOS
respectively) have been introduced and widely used since the last
decade. According to Barlow et al. (2019) and USEPA (2018), the Draft
Fact sheet, oral toxicity studies show that the liver is sensitive to GenX
chemicals, and the kidney and thyroid are sensitive to PFBS.
(Brendel et al., 2018) revealed, short-chain PFAAs are not only as
persistent as long-chain, but also have properties with significant con­
cerns. Therefore, research is now being carried out to increase aware­
ness and regulate short chain PFASs. Due to the high-water solubility,
PFASs are highly mobile in the environment through soil and water and,
can travel long distances from where they are used or manufactured;
thus, leading to offsite contamination. Perfluoroalkyl substances
comprised of anionic, cationic and zwitterionic species which will
interact differently with soil and water (Ross et al., 2018). Therefore, it

2
D.M. Wanninayake
Fig. 1. “Family tree” of PFASs, including examples of individual PFASs and the number of peer-reviewed articles on them since 2002.
Source: Reprinted with permission from (Wang et al., 2017, Figure 1, p. 2510 ) Copyright (2017) American Chemical Society.
is difficult to remove PFASs from the environment. It is also difficult to
completely break the PFASs down into their parent elements and this is
one of the major limitations in currently available PFAS remediation
methodologies (Ross et al., 2018).
1.3. Introduction to PFAS remediation technologies and status
Various PFAS remediation technologies currently available for water
treatment. Those remediation technologies involve two main processes,
the separation, and the destruction process. The separation process in­
cludes conventional techniques of flocculation and coagulation, sedi­
mentation and filtration; sorption techniques such as the use of activated
carbon and biomaterials, minerals, ion exchange resins or polymers,
nanomaterials; foam fractionation and ozofractionation (Merino et al.,
2016); membrane technologies including nanofiltration and reverse
osmosis. The destruction techniques include advanced oxidation (i.e.,
chemical, electrochemical, and photochemical) (Anumol et al., 2016)
and reduction; ultrasonication, and biological remediation (Ateia et al.,
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Journal of Environmental Management 283 (2021) 111977
2019; Ross et al., 2018). Novel hybrid techniques (Stylianou et al., 2015)
and plasma technology with limited information (Magureanu et al.,
2018; Nzeribe et al., 2019) are also destruction techniques currently
available. PFAS remediation technologies are predominantly adopted
from existing remediation technologies that were developed to treat
other contaminants. However, the extreme chemical properties of PFASs
and their behaviour in water prompts careful consideration when
developing new remediation techniques for water treatment. The
available remedial options for PFASs are limited compared to many
other contaminants. This situation triggers demand for innovation. Most
of the available methods including biological remediation, conventional
techniques and in-situ foam fractionation are not very successful for
PFAS removal, due to various factors, including cost and inapplicability
(Ateia et al., 2019; Merino et al., 2016; Ross et al., 2018).
A detailed review by Ross et al. (2018) focuses on currently available
PFAS treatment technologies and their status and discusses their ad­
vantages and disadvantages. The authors reveal that there are some
established methods currently available, application of those
D.M. Wanninayake
technologies has limitations. These limitations are high energy re­
quirements, very low removal rates under field conditions, difficulty in
applying optimum conditions in full scale, high capital cost and the
requirement of destruction technology when separate or transfer con­
taminants from liquid to solid phase (Espana et al., 2015). Most
importantly, the review revealed no reliable evidence of viable biolog­
ical degradation, including approach to use fungal enzyme for PFASs
remediation. Thus, groundwater remediation is likely to involve
extraction and ex-situ treatment, as the potentially successful in-situ
treatment techniques are hard to find (Ross et al., 2018). The author
summarised techniques such as sonolysis, electrochemical, advance
oxidation and reduction, photolysis including fungal enzymes are still
under experimental or developmental stage.
Although plasma technology could greatly increase the PFASs
degradation efficiency, full scale application is still not ready due to very
high cost (Vo et al., 2020). Hybrid water treatment process works as a
combined processing unit which is operating at their highest efficiency
to perform more than one process task. This is considered as promising
innovative and sustainable processing option consisting of energy effi­
cient integrated design.
A review by Kucharzyk et al. (2017) considered laboratory
bench-scale, pilot scale and full-scale studies with a variety of in-situ and
ex-situ approaches with various treatment technologies and provides a
base line understanding for new research needs.
According to Xiao (2017) there are more than 4000 papers have been
published since 2000 in English-language academic journals pertaining
to PFOS and PFOA studies.
My current review covers literature from 2005 to 2020 and mainly
focuses on new and advanced water treatment technologies with more
emphasis on sonochemical and electrochemical technologies, AOPs,
hybrid techniques as well as plasma technology. A comparison of those
techniques with the established conventional techniques are used to
address issues identified in laboratory scale, and large-scale considering
site-specific conditions to develop viable full-scale filed applications.
2. Separation/concentration techniques for PFAS contaminated
water
Water treatment technologies consist of separation and destruction
techniques. Although there are well established separation techniques
available for a wide array of pollutants, destruction of persistent organic
pollutants (POPs) particularly PFAS is still a challenge. Destruction is
largely influenced by the pollutant’s potential to biodegradability and or
oxidation/reduction potential. Natural degradation of PFAS is highly
challenging due to its extremely persistence nature with little or no
potential to biodegradation.
Conventional water treatment is a commonly used methodology in
most drinking water treatment processes, with steps involving coagu­
lation and flocculation, sedimentation, and filtration. However, they are
not effective for PFASs removal and are inapplicable (Horst et al., 2018;
Ross et al., 2018). Other treatment technologies also have considerable
hurdles to overcome when moving into field applications.
2.1. Adsorption
Adsorption is an effective separation for many contaminants
including PFASs and considered to be a better technique for water
treatment due to cost efficiency, eco-friendliness, high efficacy,
simplicity of design, ease of operation, and insensitivity to toxic sub­
stances (Du et al., 2014). Selection of suitable adsorbent for a given
adsorbate is determined by the adsorption capacity and the adsorption
efficiency of the sorbent. A review by Du et al. (2014) extensively dis­
cussed adsorption behaviour and mechanism of PFAS compounds on
various adsorbents. The author revealed adsorption capacity is mainly
dominated by the sorbent properties, such as pore structure and surface
functional groups, increasing pore size, decreasing partial size and
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Journal of Environmental Management 283 (2021) 111977
hydrophobicity of the AC greatly increase the absorption capacity.
However, it can be unfavourable for AC with too small particle size due
to the destruction to pore structure during crushing mechanism (Wang
et al., 2019) and the suitable pore sizes can accommodate the formed
hemimicelles/micelles of PFCs and prevent the blockage in adsorbents.
A review by Du et al. (2014) compared adsorption kinetics and
adsorption capacities of PFOS and PFOA on different adsorbents using
previous adsorption studies and tabulated in Page 445, Table 1 is a good
source of information.
Adsorption behaviour is also affected by bulk solution chemistry
includes solution pH, initial level of pollutants and properties of the
adsorbate (i.e. PFOA & PFOS), and the adsorbent (AC, GAC etc.) and
their characteristics, dosage, rate of mixing and temperature (Omo-O­
koro et al., 2018; Darlington et al., 2019; Du et al., 2014). Of these, pH is
the most important parameter while there are complicated impacts from
other chemical properties. The solution pH can change the surface
charge on adsorbents either by protonation or deprotonation of some
surface functional groups. Higher pH tends to change the adsorbent
surface charge, more negatively or less positively, making stronger
electrostatic repulsion or weak attractions with anionic PFCs (Du et al.,
2014). Adsorption mechanism of PFASs is determined by many in­
teractions including electrostatic interaction, hydrophobic effects, π-π
bond, hydrogen bond, ion exchange, and van der Waals forces (Du et al.,
2014).
Adsorption technology is commonly used and widespread, well
established, ex-situ PFASs removal technique in water using activated
carbon (either granular or powdered), ion exchange resins or polymer
and some applications using several other natural adsorbents. As the
technique concentrates the PFASs from liquid phase to solid phase, it
requires suitable approach to treat or discard the spent adsorbent ma­
terial. This process involves transport, storage, and effective destruction
of adsorbed PFASs either by regeneration or discard of the spent
adsorbent. This is a major drawback in the adsorption technology due to
high cost in operation and maintenance particularly, high energy use for
regeneration or replacement followed by waste management and offsite
waste treatment.
2.1.1. Natural adsorbents – biomaterials and minerals
The use of natural adsorbents such as biomaterials and minerals are
attractive alternatives due to their relative abundance, low commercial
value, and environmental sustainability, yet they also have limitations
due to energy use for either offsite disposal and incineration after one
use or regeneration. In depth literature review by Zhang et al. (2019a)
on “Adsorption of PFASs in aqueous solution” compared adsorption ki­
netics and capacities of biosorbents in Table 6 of their review and sug­
gests that bio-adsorbents have great potential for cost effective, efficient
PFASs removal. This paper provides detail information about a broad
spectrum of adsorbent materials and their efficient and effective inter­
action with PFAS in removal technology. Sugarcane bagasse as a
biomaterial, either natural or modified, is considered as a potentially
low cost bio-sorbent material for heavy metal and dye removal in water
and wastewater (Gorgulho et al., 2018; Khoo et al., 2018) as well as an
efficient sorbent of anionic surfactants in water (Gorgulho et al., 2018),
indicates its possible application for PFASs removal in water. Sugarcane
waste (bagasse and mulch) is one of the common waste products
generated in the sugar industry. Its porous structure (see Fig. 2) together
with adsorption characteristics indicate, it could potentially be better
used as a cheaper option to remove wide range of pollutants, including
PFASs entering the water bodies through stormwater runoff, and as a
barrier to protect further groundwater contamination due to PFASs
contaminated sites (e.g. Airports and other firefighting training
grounds) until the contaminated soils are appropriately treated. Surface
Morphology of the sugarcane mulch observed under Scanning Electron
Microscope (SEM) is illustrated in Fig. 2 below. The crop waste material
like sugar cane waste, corncob and rice straw are good adsorbents with
an ability to burn off easily in air between 160 and 200 ◦ C and produce
D.M. Wanninayake
Fig. 2. SEM images of Sugarcane Mulch.
soft ash (Omo-Okoro et al., 2018). That would be an advantage to use
them as an adsorbent which can be discarded using low energy burning,
however defluorination/complete mineralisation of PFASs may be a
problem in lower temperatures.
Aksu (2005) discussed that the microbial adsorption is a promising
alternative or supplement for present treatment processes for organic
contaminants removal from the wastewater. However, author suggests
more studies are needed to develop a practical application and does not
fully support the concept of biosorption using fungal, yeast and bacterial
biomass to remove organic pollutants. Huang et al. (2011) study sug­
gests using animal bone char is a good source of available high-volume
food waste and the potassium hydroxide activation further converts the
bone char into an adsorbent material with superior electrochemical
performance. Considering its electrochemical properties with high sur­
face area (2157 m2/g) and large pore volume (2.26 cm3/g) (Huang et al.,
2011), activated bone char would be a possible good adsorbent for
PFASs remediation using combined adsorption and electrochemical
destruction technology.
Omo-Okoro et al. (2018) discussed the application of variety of
agricultural wastes as a precursor material for adsorption of PFASs in
water. Includes wood bark, sawdust, nuts, shells and husks of crops and
plants, chitosan, starch and cellulosic fibres of crops and plants. Some of
those materials have been widely used for preparation of activated
carbon while other materials have been used directly for the adsorption
of organics, including dyes, phenolics and pesticides from aqueous
media. However, there are limited reports of their use for PFASs
removal. Kaur et al. (2018) used sugarcane bagasse and bamboo to
adsorb hydrolysed dyes from textile effluent and from industrial waste.
Both waste materials mainly consist of cellulose, hemicellulose, and
lignin (over 90%) and they have better adsorption capacity for complex
chemicals that would make the possible adsorbent materials for PFASs.
According to Carrott and Carrott (2007), lignin is a good natural
adsorbent used to remove metals, dyes, bile acids, cholesterol, surfac­
tants, pesticides, and phenols. However, there is little or no literature
available on the use of lignin or lignin-based char coal to remove PFASs.
This is a significant gap in the knowledge. Waste management and
disposal of exceptionally large quantities of lignin waste from paper
mills is a worldwide problem. For all these reasons, it is worth testing the
applicability of lignin or lignin-based char coal for PFASs remediation.
Remediation using naturally available minerals including organo­
clay and their modified materials have been considered in this review. A
modified graphite called “few-layered porous graphite” is a mineral
adsorbent with high surface area: 2870 m2/g and greater adsorption
capacity (particle size: 1–3 nm) (Zhang et al., 2019a) provides inter­
esting information about new absorbent that can be considered for PFAS
removal (Wu et al., 2018; Zhang et al., 2019a). According to Darlington
et al. (2019) organoclays and their modified materials (modified phyl­
losilicates - e.g. montmorillonite, kaolinite and palygorskite), iron ox­
ides (goethite, hematite), and silica have extensively been studied. The
authors revealed that modification to organoclay with surfactants and
amine or amino groups improves PFASs (e.g. PFOA and PFOS) adsorp­
tion however, with very high cost, limits its large-scale application.
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Journal of Environmental Management 283 (2021) 111977
Therefore, it has been used in analytical chemistry applications for PFAS
analysis as a solid phase extraction (SPE) material.
2.1.2. Activated carbon (AC) adsorbents
Mueller and Yingling (2018) identified that full scale PFASs treat­
ment technologies in water is limited to adsorption using carbon, min­
eral media such as clay, or a combination of these. Even though, AC
(either granular or powdered) is a widely used adsorbent, it has some
limitations including cost, regeneration after it is exhausted, and
reduced adsorption efficiency due to loss of carbon after each regener­
ation cycle. There is an increasing interest in alternative materials with
relatively low cost and high adsorption efficiency with cost effective
regeneration or disposal.
The ACs are very efficient for the removal of a wide range of organic
and inorganic pollutants dissolved in aqueous or gaseous media because
they possess large porous surface area, controllable pore structure,
thermo-stability, acid/base properties, low cost and environmentally
sustainable if the preparation comes from waste-products (Huang et al.,
2011; Largitte and Pasquier, 2016). According to Zhang et al. (2019a),
GAC (71.6–290 mg PFOS g− 1 and 41.3–120 mg PFOA g− 1) and PAC
(~560 mg PFOS g− 1 and 290–500 mg PFOA g− 1) (Zhang et al., 2019a),
are better adsorbents compared with other adsorbents particularly
considering their real world application. Ross et al. (2018), suggests that
GAC is an effective adsorbent for long-chain PFAAs removal, but not
highly effective technique for short-chain PFASs and precursors
removal. Whereas, additional analytical costs involve for assessing
PFASs breakthrough timeframes in water treatment process, that may be
required for regular monitoring of PFAS breakthrough is a considerable
disadvantage when using GAC as an adsorbent in large-scale filed
applications.
Injectable AC is an interesting in-situ treatment technology for
groundwater; however, more understanding of particle distribution in
the aquifer when treating a range of PFASs is imperative. Won et al.
(2019) discusses in detail, the relationship between colloidal particles
and contaminants transport mechanism in groundwater that explains
how the small sizes of colloidal particles stay in water as a suspension
without settling and how the hydrodynamic forces work that help study
in-situ groundwater remediation. PFASs offsite contamination in
groundwater is attributed to colloidal particles and their transport
behaviour that help accurately measure the extent of offsite contami­
nation. As such more immobile colloidal particles lead to slowdown the
contaminant transport in groundwater. This information suggests that
injecting more immobile carbon nanoparticles into the groundwater
aquifer could slower the PFAS transport off site, that can be used as a
preliminary approach to in-situ groundwater remediation particularly
management of off-site groundwater contamination.
2.1.3. Ion exchange resin (IXR) or polymer adsorbents
Anion- IXR and synthesised materials can remove a wide array of
long and short chain PFAAs and are highly effective removal techniques
with adsorption capacity of 100–2000 mg PFASs/g IXR (Vo et al., 2020),
though it was not greatly effective for the shortest chain PFAAs. Du et al.
D.M. Wanninayake
(2014) suggests that IXRs are mainly regenerated by organic solvents
such as methanol that is toxic, flammable, and volatile; and some are
corrosive (sodium hydroxide). Those hazardous chemical wastes require
offsite waste management and further waste treatment, making IXRs
regeneration process more difficult and costly, as such not a sustainable
approach for large water treatment processes. Thereby, water treatment
using IXRs involve exceedingly high operation and maintenance costs,
prompts its inapplicability as it is not a financially viable option in large
scale field applications for water and groundwater treatment plants.
A review by Du et al. (2014) revealed that the porous chitosan beads
which is molecularly imprinted polymer have high adsorption capacities
of about 5.5 mmol/g (Du et al., 2014) for PFOS. This was mainly due to
the formation of micelles in the porous materials. The paper revealed
that anion-exchange resins and porous crosslinked chitosan have higher
adsorption capacity for PFOS and PFOA than other adsorbents consid­
ered in their study. Du et al. (2014) suggests that electrostatic interac­
tion is recognized as one of the major attracting forces for anionic PFC
adsorption with positively charged adsorbents. Thereby positively
charged IX resins would be a better adsorbent for anionic PFCs removal.
A review by Zhang et al. (2019a) suggests that ion exchange resins
exhibit better adsorption performance than non-ion exchange resins.
Anion exchange resins adsorb PFOA better than other ion exchange
resins because, PFOA behaves as an anion at environmental pH.
Furthermore, authors revealed that more the hydrophobicity of the
resin, higher the adsorption capacity for PFAS, whereas polyacrylic
resins exhibit faster adsorption rate and higher adsorption capacity (up
to 4–5mmolg− 1) (Zhang et al., 2019a) than the polystyrene resins due
to its hydrophobicity. A summary of the adsorption kinetics and capacity
of resins tabulated in Table 3 of their review is a good source of
information.
A recent research carried out by Dixit et al. (2020a) used basic anion
exchange (IX) resin to remove GenX and two other perfluorinated ether
acids (PFEAS) from natural surface water and recycled water with
promising results. The novelty in their approach is to address the critical
knowledge gap in the removal of GenX and other PFEAS chemicals and
study multicomponent interactions between those chemicals and com­
mon organic and inorganic compounds in natural water when using IX is
a highlight.
2.1.4. Nanomaterials
Nanomaterials inherit special properties that can address many
limitations associated with their counterpart bulk materials (Oyetade
et al., 2018) and different from conventional adsorption technology. As
such high surface area mesoporous graphitised carbon, carbon nano­
tubes are currently in evaluation stage for water treatment. These ma­
terials are significantly more expensive compared to their counterpart
bulk materials and the other adsorbents; this is a major drawback in
application of nanomaterials. However, they are considered as highly
efficient and effective materials for a wide range of pollutants removal.
Nassi et al. (2014) study provided a promising approach for toxic
PFOA removal from contaminated waters by adsorption onto high sur­
face area mesoporous silica materials (HMS). It showed the highest and
the fastest adsorption capacity in comparison to other sorbents and is
very stable in water due to remaining alkylamine functional groups on
its surface strongly interacting with the silanols. Furthermore, the au­
thors stated that the HMS is a promising material for practical applica­
tion in water treatment due to its environmental friendliness because
both synthesis and removal processes require low energy consumption.
It is recommended to expand more research in this area particularly
considering in-situ groundwater treatment technologies. Injecting
nanomaterial into groundwater may have a potential to slow down
offsite contamination.
A review by Du et al. (2014) revealed that although the hydrogen
bonding interaction would be insignificant in the adsorption process of
PFCAs on CNTs, a recent study suggests the adsorption mechanism of
ionizable compounds on CNTs could interact with carboxylate group of
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Journal of Environmental Management 283 (2021) 111977
the PFCAs and the oxygen containing functional group on the CNT
surface by charge-assisted hydrogen bond as outlined below;
RCOO − +H + + − O − CNTs→(RCOO…H…O − CNTs)
Such functional groups (e.g. NH, OH and COOH) in CNTs can also
capture water molecules in bulk solution via hydrogen bonding resulting
a competitive sorption with possible cluster formation of water mole­
cules on CNTs may interfere PFCAs sorption. As a result, adsorption
mechanism involves hydrogen bonding between CNTs and PFCAs
interaction is insignificant.
A review by Zhang et al. (2019b) suggests that CNTs and IXRs exhibit
higher adsorption capacities than other adsorbents and the both mate­
rials have a great potential of removing PFASs. The authors suggest that
modified CNTs (e.g., oxidation, applying electrochemical assistance)
could improve their adsorption performance significantly although,
pristine CNTs have lower adsorption capacity than conventional ad­
sorbents. A summary of a comparison of adsorption kinetics and
adsorption capacities of CNTs available in Table 5 of Zhang et al.
(2019b) provides useful information.
Zhang et al. (2019b) further revealed, in comparison with other
nano-photocatalysts (i.e. TiO2-based, Ga2O3-based) however, In2O3
based nanomaterials showed relatively higher PFOA decomposition and
defluorination with less energy consumption under ideal laboratory
conditions with higher PFAS concentrations than real water. Therefore,
the authors suggest that validation using real water under field condi­
tions is needed and effects of the treatment conditions on remediation
process also needs to be fully assessed, as pH, redox and NOM content
could significantly impact PFAS removal. Thus, the authors suggest that
the development of new In2O3 based nanomaterials should be consid­
ered in future studies giving further research opportunities. New and
modified nanomaterial to be made to easily separate from the bulk water
after treatment, considering high operational cost and the risk of sec­
ondary pollution due to spent nanomaterials entering to the treated
water. In effect, the paper (Zhang et al., 2019b) recommends that using
nanomaterial on a suitable substrate could immobilise the nanomaterial
and address the identified issues, opening a gate to further research
opportunities.
2.1.5. Modified natural mineral adsorbents – expandable graphite (EG)
Graphite is a naturally available mineral with a layered structure
consisted with many layers of graphene, and have sp2 bonded carbon
atoms, high surface area, high thermal conductivity, large charge carrier
mobility and strong mechanical strength (Xu et al., 2017). EG is a
modified graphite material which is called graphite intercalated com­
pound (GIC) and is made by inserting foreign materials (intercalants)
between the graphene layers, creating excellent physical and chemical
properties differing from pure graphite. This modification allows delo­
calised electrons to move freely, resulting in high electrical conductivity
(Xu et al., 2017). The non-porous nature of EG enables rapid adsorption
and regeneration while its highly conductive nature reduces the energy
required for electrochemical regeneration (Oki, 2015). Thus, it would be
more environmentally sustainable and economically viable adsorbent
compared to other adsorbents.
This technology is developed in both the nuclear and water sector
applications using EG/GIC as an adsorbent which is commercially
available as sulphuric acid intercalated graphite namely GIC. SEM im­
ages of sulphuric acid intercalated graphite/GIC are illustrated as Fig. 3
below.
Oki’s study in 2015, used EG intercalated with sulphuric acid
(H2SO4), called Nyex™ which has been researched and proven to be
commercially attractive for removing dissolved organic contaminants in
greywater with combined technology called electrochemical oxidation.
In Oki’s (2015) adsorption isotherm studies on Nyex™,
anionic-surfactants showed mono-layer adsorption while other organics
showed multi-layer adsorption, resulting in a 4% removal efficiency for
anionic-surfactants while 20% (Oki, 2015) treatment efficiency for other
D.M. Wanninayake
Fig. 3. SEM images of sulphuric acid intercalated graphite (GIC/EG).
organics in greywater. Oki’s (2015) study has observed that increasing
the mass of Nyex™ increased the surfactant removal, however Nyex™
does not remove inorganic contaminants due to their high solubility in
water suggesting that no competition due to inorganic contaminants in
source water. As a result, inorganic contaminates may not impact on
adsorption capacity of GIC. However, no information about the PFASs
adsorption onto GIC is provide in this review.
A study by Sliwinska-Bartkowiak et al. (2012), discussed the atomic
structure of Activated Carbon Fibre (ACF) is similar to graphite as
illustrated in Fig. 4 above. Most of its basic structural unit consists of a
stack of turbostratic layers. In graphite minerals, defective parallel
graphene sheets are arranged in a regular hexagonal pattern and stacked
irregularly or randomly folded. Depending on the manufacturing pro­
cesses, the graphene layers may arrange either turbostratic, graphitic or
hybrid structure (Sliwinska-Bartkowiak et al., 2012). The carbon atoms
within a layer are covalently bonded with sp2 hybridization (Sli­
winska-Bartkowiak et al., 2012), however, weak van der Waals forces
between two graphene layers allow d-spacing that is an advantage when
intercalating foreign material between graphene layers when making
GIC. Recent studies carried out by Wu et al. (2018), Few-layered porous
graphite (FPG) which is similar to GIC but with porous structure, was
used to remove fluoro surfactants in small scale laboratory application
and have received promising results. This information provides oppor­
tunity to move towards medium scale laboratory experiments to test and
compare FPG with GIC; this would be a new approach towards PFAS
removal using modified natural mineral adsorbents.
2.2. Reverse osmosis (RO) and nanofiltration (NF)
According to Ross et al. (2018), RO and NF are extremely effective in
removing many PFASs including PFAA precursors, regardless of their
chain length and chemical structure. However, they revealed the major
drawback in these techniques are maintaining membrane health
particularly for groundwater applications due to suspended solids and
water geochemistry and the expenses for large scale applications. Using
RO or NF technique as a polishing step in the treatment train may help
Fig. 4. Schematic illustration of Graphite Structure.
Source: (Sliwinska-Bartkowiak et al., 2012), Fig 5, pg. 7148) - Reproduced by
permission of the Royal Society of Chemistry. https://pubs.rsc.
org/en/content/articlelanding/2012/CP/c2cp22111j#!divAbstract.
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Journal of Environmental Management 283 (2021) 111977
minimising extent of the impacts to membrane health, rather than using
such technology alone for waters with complex matrices like ground
water and wastewater. However, NF and RO are not economically viable
option for large scale applications due to very high cost.
2.3. Ozofractionation and foam fractionation
Dickson (2014) patent suggests that ozofractionation is a technique
that combines foam fractionation with ozone. Due to the surfactant
nature of the PFASs, ozofractionation can be considered as a suitable
separation technique. According to Horst et al. (2018) full scale evalu­
ation using ozofractionation was shown to be effective for removal of
PFASs including Total Oxidisable Precursors (TOP); however, polishing
treatment step such as adsorption or filtration was used to achieve lower
discharge limits in wastewater treatment applications. This method has
widely been used in aquaculture industry to remove dissolved organics
such as fats and oils from the ponds and disinfection at the same time is
an advantage in such industry applications. Ross et al. (2018) revealed
that ozofractionation has a significant advantage over adsorption tech­
nology as it can remove other organics without compromising PFASs
removal efficiency. Further, they revealed that it can remove broad
spectrum of contaminants with wide range of PFAS concentrations
however, it struggles to achieve extremely low regulatory limits in ng/L
concentrations. Therefore, the authors suggested that several other
polishing and destruction steps need to be adopted to the treatment train
process as this is not an effective technique on its own. Due to the lim­
itation of this technology, it is recommended that there should be a
change in focus towards hybrid techniques.
Nakabayashi et al. (2011) study suggests that the foam fractionation
is a promising technique for the concentration or separation of compo­
nents from a mixture based on selective adsorption. The process involves
gas-liquid interface that is created by aeration of the solution allowing
surface-active substances dissolved in the solution to be selectively
adsorbed onto the bubble (Burghoff, 2012). However, surface-inactive
components remain in the bulk solution. The separation can be ach­
ieved in less than a minute using a low-cost simple apparatus. This is the
advantage in this process, which has been used for the separation or
concentration of viruses or bacteria, proteins, polysaccharides, antibi­
otics, pesticides, other organic compounds, and oil as well as some heavy
metals. According to Burghoff (2012) and Nakabayashi et al. (2011)
foam fractionation appears as a promising biotechnological downstream
processing; however, lack of large-scale applications due to the
complexity of various types of media makes it difficult to adopt.
Recently, a new plant has been designed and developed by an
Australian based private company called OPEC Systems (Phillips et al.,
2019) to treat PFASs contaminated ground water at Oakey near Too­
woomba. According to their recent report, the company is using Surface
Active Foam Fractionation technology to process up to 250,000 L per
day (Phillips et al., 2019) and the plant is capable of removing priority
PFASs below Australian Drinking water guidelines with exceptional
waste management outcomes, zero water consumption and conservation
of polishing resins (Phillips et al., 2019) (used to remove
D.M. Wanninayake
non-regulated/short chain PFASs).
Although the foam fractionation process has many advantages, cre­
ation of foam which leads to create a waste that requires further treat­
ment and waste management is its major drawback. A review by Ross
et al. (2018), briefly discussed regarding in-situ downhole foam frac­
tionation system, using compressed air to create foam within the well
which uses similar concept to Ozofractionation. There are some con­
cerns that it will only extract PFASs within the well and this is a limi­
tation in in-situ foam fractionation.
3. Destruction techniques for PFASs contaminated water
Destruction is largely influenced by the pollutant’s potential to
biodegradability and or oxidation/reduction potential. Natural degra­
dation of PFASs is highly challenging due to its extremely persistence
nature with little or no potential to biodegradation. Commonly used
separation technique for PFAS and other contaminants involve adsorp­
tion using various carbon-based adsorbents. Destruction techniques for
those adsorbents predominantly involve either discarding the exhausted
adsorbent material offsite or regeneration. An extensive by Ross et al.
(2018) discussed various destruction technologies including incinera­
tion, microbial destruction, chemical oxidation and reduction, electro­
chemical oxidation and sonolysis. Review by Nzeribe et al. (2019) and
Stylianou et al. (2015) and Vo et al. (2020) discussed more advanced
techniques such as plasma technology, photochemical oxidation, and
hybrid techniques in addition to other advanced processes. Those
destruction techniques are discussed in detail and compared with other
techniques in this review.
3.1. Biodegradation/biological treatment
Biological degradation of PFASs compounds is highly challenging
due to the strength of C–F bond and the high negativity in F− . Ross et al.
(2018), review suggested, only polyfluorinated forms very slowly
transform in to extremely persistent perfluoroalkyl acids (PFAA) and
some of the intermediate forms are still unknown. In order to biologi­
cally transform the PFASs, at least one H atom at the α – carbon is
required; thus, PFAA precursor compounds create shorter PFAAs than
their original PFAS.
In contrast, Colosi et al. (2009) and Kucharzyk et al. (2017) research
suggested that there is some evidence of biotransformation of PFOA by
fungi (horseradish peroxidase enzyme) and has shown 30% reduction in
PFOA concentrations. However, it is extremely slow even under ideal
laboratory conditions therefore research is ongoing. In Kwon et al.
(2014) study involved aerobic bacteria which are 99% similar to Pseu­
domonas aeruginosa, has shown 67% (Kwon et al., 2014) decomposition
in the presence of high level PFOS after 48-h incubation. However,
Avendano et al. (2015), raised serious concerns about Kwon et al. (2014)
findings as it failed to provide solid evidence to confirm, suggesting that
no viable bioremediation method has been identified.
Vo et al. (2020) revealed that a recent study using an enzymes
extracted from Cannabis sativa L. has proven its ability to fast degrade
PFASs although, aerobic and anerobic microorganisms takes more than
100 days to degrade 70%–80% (Vo et al., 2020) of initial PFASs which is
much longer than other techniques used to remediate PFASs. The paper
further discussed that the enzyme could degrade 98% of PFOS and
PFHxS in 1 h (Vo et al., 2020) is a remarkable outcome that gives new
hopes to PFASs bioremediation providing opportunity to expand study
in this area.
3.2. Incineration and heat treatment
Natural adsorbents derived from plant materials are usually dis­
carded by incineration while activated carbon is regenerated using heat
treatment, burning at high temperatures and reuse which is the common
practice and widely used technique. This process involves high
8
Journal of Environmental Management 283 (2021) 111977
operational costs due to high energy use and offsite waste disposal,
treatment and management, including transportation of waste which
raises cost and sustainability concerns. There are other disadvantages,
including approximately 10% (Jeswani et al., 2015) carbon loss after
each regeneration attempt, and reactivation also enlarge the pores of the
GAC, that could adversely impact the adsorption of small molecules
(Jeswani et al., 2015). According to Merino et al. (2016), incineration of
wide range of PFASs, including fluorotelomer alcohol (FTOH)-based
acrylic polymers, PFOS and PFOA can be done successfully at temper­
atures ranging from 600 ◦ C to1,000 ◦ C (Merino et al., 2016). As a result
there are various harmful emissions can be produced such as highly toxic
dioxins and furans and by products formation such as tetrafluoro
methane (CF4) and hexafluoroethane (C2F6) that is with longer term
(50,000 and 10,000 years) environmental impacts, with a potential to
global-warming 5700 and 11,900, respectively (Merino et al., 2016),
that is a significant concern and drawback in PFAS incineration with
other waste.
Extensive studies have been carried out the use of natural adsorbents
and their carbon-based adsorbent materials and have proven to be
highly effective PFAS removal techniques. Thus, it is the widely used
common practice to date. However, discarding natural adsorbents or
regeneration of spent AC involve high cost and sustainability issues due
to high energy use triggers further research needs and innovation (Wang
et al., 2019). In addition to that, generation of toxic gases such as di­
oxins, furans and fluorocarbons is a drawback due to incineration that
requires regular monitoring and investigation as well as more research
(Vo et al., 2020).
3.3. Using solvents to regenerate IXRs
Using solvents to regenerate Ion exchange resins and polymers is not
a destruction technique. Solvents use in this process are generally haz­
ardous organic solvents or inorganic solutions, that do not destroy/
destruct the PFASs. However, it only removes contaminants from solid
phase to liquid phase. Whereas involves high cost due to regeneration
and further treatments including transportation of spent IXRs and
polymers offsite, hazardous waste management, disposal and waste
treatment is a significant disadvantage. Therefore, researchers are still
trying to find an effective alternative technique and suitable solution to
reduce chemicals use and energy use in the commonly used regeneration
processers.
3.4. Advanced oxidation (AOP) and reduction (ARP) process
A review by Babu et al. (2016) discussed the concept of ‘‘advanced
oxidation processes’’ that was established by Glaze and co-workers in
1987. The paper suggests in the AOPs produce stronger and
non-selective OH∙ radicals which is the most powerful oxidant apart
from fluorine and react with the organic pollutants and break them into
non-toxic smaller molecules or even fully mineralised to CO2 and H2O.
The OH∙ radicals cleave carbon–carbon, carbon–nitrogen, carbon­
–sulphur and the other chemical bonds. The formation of such free
radicals takes place using O3, H2O2, potassium persulfate (KPS), cata­
lysts (transition metal ions, noble metals or photocatalysts), light illu­
mination (either ultraviolet light or visible light), ultrasound or electron
beam. The AOPs such as ultrasonication, electrochemical oxidation and
plasma processes have the ability to produce hydroxyl radicals and react
with recalcitrant contaminants to break them into smaller molecules or
their parent elements (Torres-Palma and Serna-Galvis, 2018).
Southern Nevada Water Authority has published a comprehensive
report regarding in-situ chemical oxidation technique using persulphate
followed by PFASs adsorbed onto GAC. However, this has not given
promising results for PFOA and PFOS destruction adsorbed onto GAC.
The report recommended further studies to develop low cost treatment
technique (Crimi et al., 2017). According to Ross et al. (2018) chemical
oxidation with some oxidants could breakdown perfluoroalkyl
D.M. Wanninayake
carboxylates but perfluoroalkyl sulfonates is a challenge. Advanced
oxidation process with O3/H2O2 and O3/UV was ineffective for PFOS
treatment at ppm level. Dichromate (Cr2O7 2-) and permanganate
(MnO2− 4 ) had no effect on a wide range of PFAAs, including PFOS. Due to
the strongly electronegative fluorine atoms attached to the carbon
skeleton, they are protected from oxidative attacks in the presence of
hydroxyl radicals. However, it appears to be more prone to reductive
attacks. Variable PFOA and PFOS removal efficiencies were observed
using Advanced Reduction Process (ARP) in laboratory scale, but their
large-scale field applications for in-situ remediation is challenging ac­
cording to Ross et al. (2018).
A research paper published by Stylianou et al. (2015) describes three
main types of oxidation processes include conventional oxidation pro­
cess, oxidation at elevated temperature and or pressure, and AOPs. AOPs
are widely used for removal of POPs and compounds difficult to remove
using conventional techniques because they can be used under normal
temperatures and pressures. Although carbonate species (HCO−3 and CO3
2-
), pH and NOMs and reduced form of metal ions (e.g. Fe (II) & Mn (II))
(Stylianou et al., 2015) affect formation of hydroxyl radicals as reactive
species enhance the reaction. Given the high cost of using AOPs, the
paper suggests it can be used as a polishing step for large volume water
and wastewater treatment processes.
Review by Nzeribe et al. (2019), discussed several PFASs destruction
technologies using AOPs such as activated persulphate, electrochemical,
ultrasound, photochemical, plasma; and compared their cost effective­
ness based on time, energy demand, chemicals cost etc. However,
chemical oxidation such as activated persulphate does not support total
mineralisation and this in addition to high cost due to energy demand is
a major drawback. In comparison with the treatment processes dis­
cussed, photochemical oxidation is shown to be the longest treatment
time with highest energy demand resulting in the highest total cost/m3
and this is another limitation of their field applications. Hydroxyl rad­
icals, hydrogen radicals, and the hydrated electrons are the highly
reactive free radicals created by reducing agents such as ferrous, sul­
phide, sulphite, iodide with a combination of UV, ultrasound, micro­
waves, and electron beam in ARPs. Nevertheless, ARPs require extreme
operational conditions such as high temperature, high reductant dosage
and high solution pH, and these are the major disadvantages.
3.5. Ultrasonication/sonolysis
In most applications ultrasonic waves are generated by a transducer
that includes a crystal that converts electrical energy (electric current) to
mechanical energy (sound waves). Ultrasonication or sonolysis uses
sound waves at frequencies generally between 20 kHz (kHz) to 1100 kHz
to facilitate cavitation and create microbubbles in water due to negative
pressure those are collapsed (implode) during compression cycles,
releasing significant heat energy, increasing temperature up to 5000 K
within the bubbles (Ross et al., 2018). Although cavitation phenomenon
was first identified and reported in 1895, increasing interest to use
ultrasonication in destruction of microorganisms since 1920’s only
occurred after Harvey and Loomi published their studies (Mahvi, 2009).
Thereafter the application of ultrasound in chemical processes, known
as “Sonochemistry”, expanded rapidly. More research was carried out to
understand the cavitation phenomenon and its application to the
destruction of microorganisms in 1960s (Mahvi, 2009).
A book chapter “Hybrid Advanced Oxidation techniques based on
cavitation for Micropollutants degradation” written by Virkutyte and
Rokhina (2010) well describes, the factors affecting the efficiency of
sonochemical degradation and it states that “Ultrasonic frequency is the
parameter, responsible for the critical size of the cavitation bubbles and
in turn, has a significant effect on the cavitation process”. Although
lower frequencies create more violently collapsed bubbles with higher
temperatures and pressures, higher frequencies create large number of
hydroxyl radicals compared to lower frequencies due to more cavita­
tional events thereby, increase the efficiency of the contaminant
9
Journal of Environmental Management 283 (2021) 111977
degradation. The book further discusses that the studies conducted in
the last decades revealed that higher ultrasound frequencies (200–1000
kHz) performed more efficiently than lower frequencies (Virkutyte and
Rokhina, 2010). The optimum frequency is determined by the physical
and chemical properties of the organic contaminant depending on the
reaction pathway either via radicals or pyrolytic reaction. To get the
same reaction efficiency (that was obtained in higher frequency) in
lower frequencies, substantial power input is required that may cause
loss of energy as heat and the degradation of the ultrasonic horn are
drawbacks (Virkutyte and Rokhina, 2010). Therefore, it is imperative to
assess and evaluate optimum frequency level that is suitable for effective
degradation of specific contaminant/s destruction mechanism.
Virkutyte and Rokhina (2010) further discussed general hypothesis
of sonochemical process using several theories with their reaction modes
such as hot-spot, electrical, plasma discharge and supercritical theory.
The hot-spot theory explains violent collapse of generated cavitation
bubbles with high temperature about 5000 K and high pressure up to
1000 atm. The book also discussed electrical theory hypothesis and
formation of electrical double layer on the surface of the cavitation
bubble and explains fragmentation of contaminants takes place due to
an intense electrical field rather than formation of micro plasms inside
the bubbles break the chemical compounds. Supercritical theory sug­
gests existence of supercritical water as an additional phase for chemical
reaction. Among all theories, Virkutyte and Rokhina (2010) suggests
hot-spot theory is a widely accepted sonochemical reaction in aqueous
environment. Cavitational effects to degrade contaminants involve two
mechanisms: physical and chemical reactions. Formation of oxidising
radicals is a result of chemical effect due to violent bubble collapse and
the equations below explain the reactions (Virkutyte and Rokhina,
2010).
H2 O→⋅H + ⋅OH O2 →2⋅O
⋅H + ⋅OH→H2 O ⋅H + O2 →⋅H O2
2⋅OH→H2 O + 1/2O2 2⋅H O2 →H2 O2 + O2
2⋅OH→H2 O2 H2 O2 + ⋅OH→H2 O + ⋅HO2
2⋅H→H2 ⋅H2 O2 + HO2 →H2 O + ⋅OH + O2
N2 →2⋅N ⋅OH + ⋅OH→H2 O + ⋅O
Babu et al. (2016) and Virkutyte and Rokhina (2010) describes,
sonochemical reactions in three zones: core of cavitation bubble gas
phase, bubble–liquid (supercritical) interface, and bulk solution. The
degradation of the micro pollutants takes place by pyrolysis (physical
mechanism) and/or free radical reactions (chemical mechanism) that is
illustrated in Fig. 5 below.
Nzeribe et al. (2019) proposed a several mechanisms of PFASs
degradation and describes that due to high surface activity and hydro­
phobicity, PFOA and PFOS adsorb onto the bubble-water interface and
cleavage of a C–C/C–S bond creating perfluorocarbon intermediates.
Then the total mineralisation of these intermediates occurs in the cav­
itational bubble gas phase via pyrolytic reaction. The study describes
formation of PFHpS and PFHxS intermediates as a result of PFOS
sonolysis. The other proposed mechanism for PFOA mineralisation is a
rapid reaction or no stepwise degradation via intermediates.
While operating parameters such as frequency, power density, so­
lution temperature, type of sparge gas and PFASs concentration, play
key roles in sonolytic degradation and defluorination efficiency, they
depend on the available interfacial adsorption sites, intensity of bubble
collapse, and the frequency of bubble oscillation. Increased frequency
accelerates bubble oscillation, which creates more active sites on bubble
interface for PFASs adsorption, resulting increase PFAS degradation
rates. The catalysts or additives such as persulfate, sulphate ions and
periodate may also enhance sonochemical reaction mechanism and
D.M. Wanninayake
Fig. 5. Conceptual model of reactions in three zones of ultrasonic cavitation bubble.
Source: (Adopted from, “Jurate Virkutyte and Ekaterina V. Rokhina (2010), Figure 9.1 (p.324) in Jurate Virkutyte, Rajender S. Varma and Veeriah Jegatheesan,
Treatment of Micropollutants in Water and Wastewater, ISBN: 9781843393160, © IWA Publishing”.) With permission National Centre for Biotechnology Information
(2020, 2021).
kinetics resulting increased PFASs degradation efficiency.
Mahvi (2009) describes in detail, the application of ultrasonication
technology for water and wastewater treatment, for a variety of pol­
lutants including bacteria, algae, fungi, pathogens, and organic sub­
stances such as phenols, herbicides, pesticides, surfactants and
explosives etc. The review suggests, no anticipated environmental con­
cerns as it does not involve additives and no toxic by-products genera­
tion; however, PFASs are not considered in their review.
Kucharzyk et al. (2017) suggested that PFASs destruction using
higher frequency ultrasound is favourable with moderate running cost
for energy use; however, large-scale applications are a challenge due to
high capital cost. In contrast Babu et al. (2016) suggested that ultra­
sonication with AOPs (hybrid techniques) are operationally simple,
efficient and have no apparent environmental issues, therefore,
large-scale industrial applications are economically viable. The authors
studied the use of ultrasound in remediation of wastewater contami­
nated with organic pollutants in the absence and presence of other AOPs
such as sono-ozone, sonophotocatalysis, sonoFenton and
sonophoto-Fenton techniques in detail. According to their findings,
hybrid AOPs have shown greater performance than those techniques
performed individually in many cases. Combination of ozone with ul­
trasound enhance the degradation of toxic organic pollutants including
PFASs through hydroxyl radical reactions that break them into smaller
molecules and even fully mineralised to F− , SO2- 4 ,CO2 and H2O (Babu
et al., 2016). Furthermore, hybrid AOPs have synergistic effect as
opposed to individual AOP systems in most environmental remediations
and the paper summarised that there is no doubt, ultrasound is a
powerful tool in AOPs (Babu et al., 2016).
3.6. Electrochemical oxidation
In recent years, electrochemical oxidation (EO) received increasing
interest for PFASs treatment due to its ability to degrade wide range of
10
Journal of Environmental Management 283 (2021) 111977
persistent micropollutants. However, it is less effective for shorter chain
PFASs degradation and potential issues of electrode corrosion as well as
possible generation of undesirable toxic by-products (e.g., hydrogen
fluoride, chlorine gas, bromate, perchlorate, and absorbable organic
halides) in the presence of co-contaminants, other organics and in­
organics such as chloride, or other harmful substances are major
challenges.
Ross et al. (2018), and Nzeribe et al. (2019) revealed that there are
two contaminant destruction mechanisms using electrochemical oxida­
tion (EO): direct and indirect. Indirect electrochemical process takes
place where strong oxidants are produced on the electrode (anode) and
the contaminants are degraded (oxidised) in the bulk solution. In
contrast, direct EO takes place at the electrode through active oxygen (e.
g., hydroxyl radical) when contaminants adsorbed onto the electrode.
Therefore, careful attention when selecting a suitable electrode material
is necessary as the anode plays a major role in electrochemical proc­
essers with relevant application. There are various electrode materials
available including titanium dioxide (TiO2) and titanium suboxide
(Ti4O7), lead dioxide (PbO2), stannous (tin) dioxide (SnO2), iirradium
oxide (IrO2), ruthenium dioxide (RuO2), and platinum (Pt) as well as
carbon or graphite. Among these, boron-doped diamond electrode was
found to be the best for PFASs treatment; thus, it has been used for PFASs
research due to its chemical, mechanical and thermal stability (Fang
et al., 2017; Nzeribe et al., 2019). A review by Ross et al. (2018), which
observed a 99.7% detectable PFASs removal using a boron-doped dia­
mond (BDD) anode confirms the above finding. The review further
suggests that the application of a Ti4O7 electrode was effective in the
degradation of both PFOS and PFOA, mineralisation to CO2 and F− with
only trace intermediate organofluorine compounds. However, the re­
view concluded that the electrochemical oxidation has some limitations
for commercial application and more research is needed with environ­
mental matrices to determine its suitability for PFASs remediation,
despite its robustness, versatility, ease of automation and most
D.M. Wanninayake
importantly, its advantage as a clean alternative to the other treatment
technologies.
Generally, in theory, the following reactions take place near anode
and cathode in presence of H2O.
Anode 2H2 O → O2(g) ↑ + 4H+ + 4e
Cathode 2H2 O + 2e→H2(g) ↑ + 2OH−
A review by Fang et al. (2017) suggested that degradation efficiency
in EO process can be improved by increasing productivity of radical
formation whilst suppressing the emission of O2 and O3. As such, the
selection of a suitable electrode is vital. A H2O molecule adsorbed onto
the electrode generate oxidising products including high energy radicals
such as ●HO, ●O− , ●HO2, ●O2− ; and H2O2, O2, O3 (Fang et al., 2017). If
there are other contaminants present such as Cl− that can generate Cl2,
HClO, HClO2, HClO3, HClO4 and the corresponding radicals; if SO2− 4 or deexcitation metastable species. The most abundance reactive species
present it can generate S2O2−8 and the corresponding radicals. The rad­
icals react with organic molecules. Then the degradation reactions occur
as a sequence of chain reactions, which involve initial and subsequent
steps, PFOA as an example shown below (Fang et al., 2017).
C7 F15 COOH + 14H2 O = 8CO2 + 15HF + 14H+ + 14e
Research by Trautmann et al. (2015) found, the EO rate of PFASs in
groundwater with high dissolved organic carbon using BDD electrode
slower in sulfonates than carboxylates. However, the rate increased with
increasing chain length. This resulted in the formation of shorter chain
PFCAs, but with prolonged (120 h) oxidation, 97% (Trautmann et al.,
2015) degradation was achieved. Therefore, shorter chain PFASs
removal using electrochemical oxidation requires more attention to in­
crease the reaction rates and optimise the process. This finding is further
supported by the recommendations of Trautmann et al. (2015) and Ross
et al. (2018) for further studies on process improvements. Notwith­
standing the limitations discussed above Trautmann et al. (2015)
concluded that EO is a promising approach for PFASs removal. However,
the author further suggested that more sensitive analytical techniques to
be used to confirm the analytical data in ultra-low levels to achieve the
regulatory limits.
A recent research paper published by Schaefer et al. (2019) for their
21-day study suggested, longer term studies are important because the
large-scale electrochemical field applications for PFASs treatment are
currently in implementation stage. They have experienced substantially
decreased system performance in longer term EO due to deteriorating
electrode caused by calcium and magnesium scaling. This issue was
successfully controlled by using acid cleaning. According to the elec­
trochemical degradation or defluorination study by Schaefer et al.
(2017) using PFOA and PFOS solution with model hydroxyl radical
scavenger showed no apparent effects. Thus, confirmed that PFOA
degradation rate in natural groundwater with scavenging species such as
Cl− , CO2-3/HCO− 3 and NOM has no effects to EO process (Schaefer et al.,
2017).
McQuillan et al. (2018) study found that electrochemical regenera­
tion of spent GAC was an effective alternative technique for thermal,
chemical, and microbial regeneration. After 5 h EO, 95% GAC was re­
generated with 2% (McQuillan et al., 2018) loss in adsorption capacity
was observed. The important message in this review is that the research
so far predominantly focused on variations in reactor configurations and
operating parameters, used with different types of adsorbents and model
contaminants. Although, optimisation of mechanism and kinetics are
important functional aspects in treatment process when scaling up
however, limited attention was given. The review further revealed that
non-porous materials have a greater capacity for use in combined
adsorption electrochemical treatment systems referring to Arvia tech­
nology as a successful industrial application.
According to the currently available literature, using EG/GIC
adsorbent and simultaneous electrochemical regeneration has been
11
Journal of Environmental Management 283 (2021) 111977
applied successfully to remove organic contaminants in wastewater
including phenols and dissolved organic matter in greywater (Hussain
et al., 2013a, 2013b; Oki, 2015). This technology is developed for both
the nuclear and water sector applications using sulphuric acid (H2SO4),
intercalated graphite (GIC- H2SO4) as an adsorbent. There is no pub­
lished information currently available for PFASs remediation using
combined adsorption and electrochemical regeneration involved hybrid
technology, according to my literature review.
3.7. Non-thermal plasma
Non-thermal plasma is an advanced treatment that involves forma­
tion of highly reactive species mainly initiated by collision of energetic
electron discharged with gas atoms or molecules under high voltage.
Reactive species are then produced by radical recombination reactions
are hydroxyl radicals, H2O2 and O3 formed in liquid or gas-liquid phase
which are then used for degradation of pollutants. In addition to that the
solution pH, molecular structure of the pollutant, composition of the gas
phase, plasma reactor and the energy level in the electrical discharge
affect degradation efficiency (Magureanu et al., 2018).
Virkutyte and Rokhina (2010) discussed similarities between sono­
chemistry and corona chemistry and introduced plasma theory to
explain cavitation. They argued that fragmentation process was due to
an intense electrical field rather than implosion, indicating the forma­
tion of micro plasmas inside the bubbles.
Plasma technology involves the use of electrons in the formation of
•HO radicals (Virkutyte and Rokhina, 2010) as outlined below:
e− +H2O → HO• +H+ e− e− +H2O → HO• +H−
e− +H2O+ → HO• +H• e− +H3O+ → HO• +H2 + e−
H− +H2O+ → HO• +H2 H− +H3O+ → HO• +H2 +H•
In the presence of another molecule, O2 combine with O• radical,
form O3; formation and accumulation of H2O2 in the liquid phase during
the plasma treatment (Virkutyte and Rokhina, 2010) as in the below
equations:
O2 + e− → 2O• + e−
O• +O2 +M→ O3 + M.
HO• +HO• → H2O2
In the last few years, numerous studies have been conducted to
investigate removal of organic contaminants, using non-thermal plasma.
A critical review by Magureanu et al. (2018) describes several plasma
reactors used in liquid and gas–liquid environment with variety of
configurations, such as point-to-plate, point to-point and wire-cylinder
corona, diaphragm discharge. The authors suggest that relatively
small-scale plasma system can be used for point source wastewater
treatment as they contain high concentrations of contaminants with
limited volumes because the plasma technology would not be effective
treatment for trace levels.
Magureanu et al. (2018) also discussed, plasma technology with
ozone as a promising technique that is better than ozone alone for the
removal of pesticides in water and wastewater. Numerous other studies
have been published on the plasma technology, predominantly on
phenols, organic dyes, pharmaceuticals, and pesticides removal in
water. It is found to be satisfactory with remarkably good results for
pesticides removal, achieving around 90% after 5 min (Magureanu
et al., 2018) treatment is an excellent outcome. The paper suggests that
combining plasma technology with other AOPs can enhance removal
efficiency, recommending plasma-ozone systems or plasma-catalysts
systems providing opportunity to move towards hybrid technology.
A comparative study was conducted by Saleem et al. (2020) for PFOA
in water treatment using three plasma reactors those are made based on
D.M. Wanninayake
different concepts; two reactors from previous studies (“7-wires” DC
plasma reactor and the ‘hollow electrode’ AC plasma reactor); and the
third one is, ‘self-pulsing discharge’ (SPD) DC plasma reactor specifically
designed for PFAS treatment. The authors compared overall perfor­
mance of SPD reactor with the other two reactors based on overall ef­
ficiency considering the time, and the energy required for PFOA
treatment. The authors revealed that the SPD reactor performance found
to be good, due to the extended plasma/liquid interface allowing the
reaction between PFOA and reactive species. Although, the reactive
species formed in the plasma, plasma/liquid interface and bulk liquid
phase are already identified in SPD reactor, ensuring PFOA degradation
mechanism is still underway, that is a considerable gap. The authors
further revealed that PFOA in tap water with argon as a feed gas
significantly improved energy efficiency (from 123 to 561 mg/kWh)
(Saleem et al., 2020), than PFOA in Milli-Q water with air, suggesting
conductivity of the solution and the feed gas are crucial factors for PFOA
degradation. This information provides valuable information to re­
searchers in water industry and remediation.
Singh et al. (2019) study conducted to assess breakdown products
from PFAS degradation in plasma basde water treatment has identified
several linear chain PFAA byproducts (C4 to C7) from PFOA and PFOS.
These byproducts include PFHeA, PFHxA, PFPeA and PFBA from PFOA
and PFOS degradation as well as PFHxS and PFBS from PFOS with
elevated amounts of fluoride, inorganic carbon and small organic acids
such as trifluioracitic acid, acitic acid and formic acid (Saleem et al.,
2020). In addition, 43 PFOA related by products and 35 PFOS related
byproducts were also identified and some of them are reported first time
in PFAS degradation experiments, those include cyclic PFASs (Saleem
et al., 2020). Although the study further revealed that 90% of PFOA was
removed in 60 min (Saleem et al., 2020) was an advantage, increased
concentration of other byproducts is a disadvantage in this process.
The plasma technology is new to PFAS contaminated water treat­
ment, and it is still under experimental stage. Its high cost and high
energy use are the major drawbacks, that could potentially be addressed
in future studies by moving towards hybrid processes involve plasma
technology.
3.8. Hybrid technology
Hybrid water treatment systems are defined as combination of two or
more individual treatment processes (different biological, adsorption,
AOPs or membrane processes etc.). These hybrid systems perform better
than single treatment processes alone and improve the treatment of
micropollutants. A research was conducted by Stylianou et al. (2015)
using hybrid Membrane-Ozone system consisting of novel ceramic
membrane contactor for bubbleless ozonation of emerging micro­
pollutants. Their research showed that membrane fouling is the major
drawback, although membranes are widely used better techniques for
natural water and wastewater treatment. In order to address the issue
several methods have been developed. Among them hybrid process
which integrates two or more membrane processes or membrane pro­
cesses combined with other water treatment processes are the most
popular.
A review by Ateia et al. (2019) suggests that hybrid sorption systems
of GAC and IX may provide possible alternatives to enhance the
short-chain PFAS removal and manage the competition from NOM and
long-chain PFAS. A review by Babu et al. (2016) discussed in detail
about ozone-sonolysis hybrid technique and suggests that O3 react with
organic pollutants either directly by electrophilic attack or indirectly by
radical chain reactions depends on the solution pH. Thermal decom­
position of O3 in the collapsing bubbles produce extra . OH radicals in
the hybrid process, enhance degradation of organic pollutants. Ac­
cording to Babu et al. (2016) findings, ultrasonication with AOPs have
shown greater performance than those techniques performed individu­
ally in many cases.
Virkutyte and Rokhina (2010) revealed that the results obtained
12
Journal of Environmental Management 283 (2021) 111977
from number of laboratory scale experiments in hybrid
ultrasound-based techniques have shown a greater potential of degra­
dation of micropollutants in water and wastewater. Although the au­
thors discussed that there are some concerns in economical feasibility in
large scale applications, some possible alternative technological ap­
proaches are available to consider system improvements and optimisa­
tion. This would give opportunity in research and innovation for
scientists and engineers to work together in adopting cost effective
practical solution/s for remediation of target contaminants, including
PFASs. Hybrid processers are discussed in detail under ultrasonication
and electrochemical processes with AOPs as well as plasma technology
in this review.
4. Short chain PFAS remediation in water
Short chain PFASs are comprised of less than or equal to six carbon
atoms in the chain, with PFHxA and PFHxS being the largest and tri­
fluoracetic acid being the shortest in the class of short chain PFAS
compounds. Limited data is available in short chain PFAS transport, fate,
and treatment as there is limited studies conducted, to date. Although
the short chain PFAS transport in the environment is not well under­
stood, Ateia et al. (2019) discusses two hypotheses which include
anionic and hydrophilic compounds direct transport by oceanic current
while neutral and volatile PFASs are transported through atmosphere.
In the last decade, increased use of short chain PFASs as an alter­
native to long chains (i.e. GenX and PFBS replaced PFOA and PFOS
respectively) (USEPA, 2018). However, current studies in short-chain
PFAS compounds suggests, replacement PFASs are equally persistent
and bioaccumulative as their long-chain counterparts. Therefore,
increased concerns regarding their health and environmental impacts
(USEPA, 2018) resulted, requirement of developing not only new water
treatment techniques and methodologies, but also analytical techniques
and methodologies to reliably identify and quantify in ultra-low levels
become more prominent.
A review by Ateia et al. (2019), suggested that a comprehensive
survey of available short chain PFASs is required. This could be attrib­
uted to limited data about their precursors due to the limitations in their
analytical methodologies. The authors have suggested that although,
conventional treatment plants fail to remove short chain PFASs,
destruction methods such as AOPs and ARPs; EO processes are prom­
ising but require new approaches. The paper suggested that the
requirement of the development of new selective adsorbent material and
recommended that the hybrid techniques maybe an alternative
approach to remove short chain PFASs. The authors also stated in their
paper that the measurement of short chain PFASs in water is limited
thus, further research is needed, also giving opportunities to the PFAS
researchers in developing suitable analytical methodologies.
Short chain PFAS compounds have relatively lower adsorption af­
finity on to activated carbon with compared to long chain PFASs (Wang
et al., 2019; Dixit et al., 2020b). However, the results obtained from a
study by Dixit et al. (2020b) suggested, normal ion exchange resin
(dosage of 0.45 mL/L, 100 mg/L or higher) (Dixit et al., 2020b) has
shown great potential for short chain PFAS such as GenX and PFEAS
removal from natural drinking water sources as it was able to achieve
PFEAS removal <70 ng/L with an ability to remove >60% NOM and
>80% (Dixit et al., 2020b) inorganic ions at the same time. This is a
great achievement in addressing short chain PFAS removal in the pres­
ence of NOM and inorganic ions using IX normal resins.
5. PFASs remediation process selection in field application
Mueller and Yingling (2018) extensively discussed in their report,
various factors affecting PFASs remediation process selection in field
applications, under different perspectives. These include but are not
limited to, site characteristics, characteristics of PFASs, changes in PFAS
properties and finally community acceptance. The site characteristics
D.M. Wanninayake
depend on the nature of the source, release pathways, affected receptors,
and fate and transport in the environment. The key factors of PFASs
characteristics such as ionic state, type of ionic group (sulphonic or
carboxylate), lipo and hydrophobicity, reactivity of alkyl group, mole­
cule size and the structure, partitioning co-efficient, solubility, volatility
and acidity are largely impacting. The other factor is changes in PFASs
chemical and physical properties due to natural or remediation pro­
cesses in the presence of other contaminants such as chlorinated solvents
and petroleum hydrocarbon which can affect PFAS distribution and
mobility in groundwater. The changes in PFASs properties include, alkyl
functional groups of some PFASs effect on total oxidisable compounds;
partial degradation of C–C bonds can generate shorter chain PFASs
which may be more mobile in the environment; and modification in
aquifer converts PFASs to the more stable and mobile perfluoro car­
boxylic acids. Finally, the community acceptance factor plays a signifi­
cant role, as it depends on cost, level of clean-up, residual contamination
and more importantly, the environmental and human health risks as­
pects, among other things.
6. Knowledge gap and recommendations
Pending new regulations, short chain PFASs (C ≥ 6 – e.g.: PFHxA and
PFHxS), and their impacts to human health and environment yet to be
fully evaluated and confirmed. This may result in expanding the scope of
PFASs research, not only PFASs remediation, human health and envi­
ronmental impacts, but also development of reliable and accurate
qualitative and quantitative analytical techniques and methodologies to
handle a wide array of PFASs classes. This is because detection and
identification of precursors are challenging due to the limited available
PFASs standards and requirement of high cost advanced analytical
instrumentation with limited expertise and skills.
According to Kucharzyk et al. (2017) lack of published literature for
full-scale and the pilot-scale in-situ applications for PFAS remediation is
a major limitation. More attention should be given to the optimisation of
functional aspects of the treatment process such as mechanism and ki­
netics, when scaling up (Kucharzyk et al., 2017). Generally, most of the
research are carried out in laboratory scale under ideal conditions in
short term studies. Hence, the developed methodologies in laboratory
scale need validation in real-world large-scale applications with longer
term studies. This is because, selection of water treatment tech­
nology/technologies when developing suitable methodology also de­
pends on site-specific conditions, including PFASs properties, behaviour
and concentrations; water quality, treatment goals, hydrogeology and
various other social, economic and environmental factors such as
various risks, cost, environmental sustainability, and social acceptance.
They may have longer term impacts that can be direct and or indirect, in
addition to the benefits. Therefore, it is important to take them all in to
careful consideration when implementing a suitable treatment plant for
the specific site.
7. Conclusion
Among more than 3000 PFASs compounds around the globe, PFAAs
are the most stable group of PFASs. Although the polyfluorinated pre­
cursors are likely to be biodegradable, they finally turn into extremely
persistent PFAAs, which show no sign of biodegradation. Currently
existing groundwater remediation technologies usually involve extrac­
tion and ex-situ treatment as there is a very little or no potentially
successful in-situ treatment technologies available to date. Generally,
most researchers have considered PFOS and PFOA in their studies while
the other PFASs have rarely been considered, leaving a significant
knowledge gap in water treatment technologies for a broader array of
PFASs and their precursors including shot chain PFASs.
Most water treatment technologies involve adsorption by trans­
ferring PFASs from liquid to a solid matrix, which then needs to be
disposed of, or regenerated. As evidenced by this literature review, very
13
Journal of Environmental Management 283 (2021) 111977
limited technology has been identified which can both remove and
destroy PFASs simultaneously and there is no information about large-
scale field applications. This provides researchers with substantial op­
portunities to develop more effective and sustainable remediation so­
lutions as the increasing number of PFASs become regulated.
Selection of water treatment technology/technologies depend on
site-specific conditions, including PFASs concentrations, water quality,
treatment goals, hydrogeology and some other considerations. Simple
conventional chemical/physical and biological water treatment tech­
nologies as well as advanced sorption and filtration techniques do not
provide effective and sustainable solutions for both removal and
destruction of PFASs. Advanced oxidation and chemical oxidation have
been demonstrated to be potentially applicable for some PFAAs
destruction, however there are concerns due to the formation of shorter
chain PFAAs. Although non-thermal plasma is a new technique with
limited studies, it is one of the effective techniques for the degradation of
PFASs; however, this is with a limitation due to significantly high cost
and high energy use.
A combination of two or more (hybrid) techniques may be more
effective than a single techniques alone. As such, advanced hybrid
techniques provide evidence of their ability to eliminate PFASs from the
environment cost effectively and energy efficiently thereby, improving
sustainability. Among all the techniques considered in this review,
either sonochemical and or electrochemical technique/s (considered as
green technology) combined with other applicable AOPs involve hybrid
process would be a better solution for the remediation of PFASs
contaminated water and eliminate PFAS from the environment and
address the limitations of the currently available PFAS treatment
methodologies.
Declaration of competing interest
The author declares that there is no known competing financial in­
terests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgement
I wish to acknowledge and thankful to Dr Lesley Bowtell, supervisor
at University of Southern Queensland for his support, guidance, and
assistance for my PhD program. I wish to acknowledge and grateful to
Prof Godwin Ayoko, co-supervisor at Queensland University of Tech­
nology, for reviewing and editing, providing advice, assistance, and
support to this manuscript.
I wish to acknowledge and be grateful to the Research Librarian Dr
Tricia Kelly for providing me continuous professional advice, guidance
and support. I also wish to thankful to Learning adviser Dr Douglas
Eacersall and Liaison Librarian Ms Rowena McGregor at the University
of Southern Queensland for their advice, assistance and support.
I wish to acknowledge and be thankful to the in-kind support pro­
vided by Symbio laboratory, in Brisbane for experimental samples
analysis using LCMS/MS and HR LCMS for my PhD research project.
At the time of publication this research has not received any specific
grant from funding agencies in the public, commercial, or not-for-profit
sectors.
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