Sorptive remediation of perfluorooctanoic acid (PFOA) using mixed mineral and graphene/carbon-based materials
Supriya Lath
A D , Divina A. Navarro A B , Dusan Losic C , Anupama Kumar B and Michael J. McLaughlin A B
+ Author Affiliations
- Author Affiliations
A School of Agriculture, Food and Wine, The University of Adelaide, PMB 1 Glen Osmond, SA 5064, Australia.
B CSIRO Land and Water, PMB 2 Glen Osmond, SA 5064, Australia.
C School of Chemical Engineering, The University of Adelaide, Adelaide, SA 5005, Australia.
D Corresponding author. Email: supriya.lath@adelaide.edu.au
Environmental Chemistry 15(8) 472-480 https://doi.org/10.1071/EN18156
Submitted: 16 July 2018 Accepted: 25 September 2018 Published: 31 October 2018
Environmental context. Per- and poly-fluoroalkyl substances (PFASs) are contaminants of emerging concern, creating a need to develop efficient multi-functional adsorbents for improved remediation performance. By exploiting the versatility of graphene technology, we demonstrate that combining mineral and carbonaceous phases greatly increases and strengthens PFAS-binding to the adsorbent. The study highlights the benefits and potential applications of mixed adsorbents in PFAS-remediation.
Abstract. As the degradation of perfluorooctanoic acid (PFOA) and related per- and poly-fluoroalkyl substances (PFASs) is energy-intensive, there is a need to develop in situ remediation strategies to manage PFAS-contamination. The sorption of PFOA by graphene oxide (GO), an iron-oxide-modified reduced-GO composite (FeG) and an activated-carbon(C)/clay/alumina-based adsorbent, RemBindTM (RemB), are evaluated. Sorption by FeG and RemB (>90 %) is much greater than GO (60 %). While an increase in pH hinders PFOA-sorption by GO, owing to the increased repulsion of anionic PFOA, variations in pH and ionic strength do not significantly influence PFOA-sorption by FeG and RemB, which indicates that binding is predominantly controlled by non-electrostatic forces. Hydrophobic interactions are assumed at the graphene or C-surface for all adsorbents, with added ligand-exchange mechanisms involving the associated Fe- and Al-minerals in FeG and RemB, respectively. Desorption of adsorbed PFOA is greatest in methanol, compared to water, toluene, or hexane, which provides estimates of the binding strength and reversibility from an environmental-partitioning perspective; i.e. risk of remobilisation of bound PFOA owing to rainfall events is low, but the presence of polar organic solvents may increase leaching risk. Iron-mineral-functionalisation of GO enhances the amount of PFOA adsorbed (by 30 %) as well as the binding strength, which highlights the advantage of combining mineral and C-phases. Successful sorption of a range of PFASs from a contaminated-site water sample highlights the potential of using ‘mixed’ adsorbents like FeG and RemB in situ for PFAS-remediation, as they provide avenues for enhanced sorption through multiple mechanisms.
Additional keywords : PFASs, sorption.
References
Arias EVA, Mallavarapu M, Naidu R (2015). Identification of the source of PFOS and PFOA contamination at a military air base site. Environmental Monitoring and Assessment 187, 4111| Identification of the source of PFOS and PFOA contamination at a military air base siteCrossref | GoogleScholarGoogle Scholar |
Benskin JP, Li B, Ikonomou MG, Grace JR, Li LY (2012). Per- and polyfluoroalkyl substances in landfill leachate: patterns, time trends, and sources. Environmental Science & Technology 46, 11532–11540.
| Per- and polyfluoroalkyl substances in landfill leachate: patterns, time trends, and sourcesCrossref | GoogleScholarGoogle Scholar |
Bruton TA, Sedlak DL (2017). Treatment of aqueous film-forming foam by heat-activated persulfate under conditions representative of in situ chemical oxidation. Environmental Science & Technology 51, 13878–13885.
| Treatment of aqueous film-forming foam by heat-activated persulfate under conditions representative of in situ chemical oxidationCrossref | GoogleScholarGoogle Scholar |
Buck RC, Franklin J, Berger U, Conder JM, Cousins IT, de Voogt P, Jensen AA, Kannan K, Mabury SA, van Leeuwen SPJ (2011). Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and origins. Integrated Environmental Assessment and Management 7, 513–541.
| Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and originsCrossref | GoogleScholarGoogle Scholar |
Cheng J, Vecitis CD, Park H, Mader BT, Hoffmann MR (2010). Sonochemical degradation of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in groundwater: kinetic effects of matrix inorganics. Environmental Science & Technology 44, 445–450.
| Sonochemical degradation of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in groundwater: kinetic effects of matrix inorganicsCrossref | GoogleScholarGoogle Scholar |
Cong H-P, Ren X-C, Wang P, Yu S-H (2012). Macroscopic multifunctional graphene-based hydrogels and aerogels by a metal ion induced self-assembly process. ACS Nano 6, 2693–2703.
| Macroscopic multifunctional graphene-based hydrogels and aerogels by a metal ion induced self-assembly processCrossref | GoogleScholarGoogle Scholar |
Deng S, Zhang Q, Nie Y, Wei H, Wang B, Huang J, Yu G, Xing B (2012). Sorption mechanisms of perfluorinated compounds on carbon nanotubes. Environmental Pollution 168, 138–144.
| Sorption mechanisms of perfluorinated compounds on carbon nanotubesCrossref | GoogleScholarGoogle Scholar |
Dong Z, Wang D, Liu X, Pei X, Chen L, Jin J (2014). Biol.-inspired surface-functionalization of graphene oxide for the adsorption of organic dyes and heavy metal ions with a superhigh capacity. Journal of Materials Chemistry A: Materials for Energy and Sustainability 2, 5034–5040.
| Biol.-inspired surface-functionalization of graphene oxide for the adsorption of organic dyes and heavy metal ions with a superhigh capacityCrossref | GoogleScholarGoogle Scholar |
Dreyer DR, Park S, Bielawski CW, Ruoff RS (2010). The chemistry of graphene oxide. Chemical Society Reviews 39, 228–240.
| The chemistry of graphene oxideCrossref | GoogleScholarGoogle Scholar |
Du Z, Deng S, Bei Y, Huang Q, Wang B, Huang J, Yu G (2014). Adsorption behavior and mechanism of perfluorinated compounds on various adsorbents – A review. Journal of Hazardous Materials 274, 443–454.
| Adsorption behavior and mechanism of perfluorinated compounds on various adsorbents – A reviewCrossref | GoogleScholarGoogle Scholar |
Fan L, Luo C, Sun M, Qiu H, Li X (2013). Synthesis of magnetic β-cyclodextrin–chitosan/graphene oxide as nanoadsorbent and its application in dye adsorption and removal. Colloids and Surfaces B: Biointerfaces 103, 601–607.
| Synthesis of magnetic β-cyclodextrin–chitosan/graphene oxide as nanoadsorbent and its application in dye adsorption and removalCrossref | GoogleScholarGoogle Scholar |
Feng H, Lin Y, Sun Y, Cao H, Fu J, Gao K, Zhang A (2017). In silico approach to investigating the adsorption mechanisms of short chain perfluorinated sulfonic acids and perfluorooctane sulfonic acid on hydrated hematite surface. Water Research 114, 144–150.
| In silico approach to investigating the adsorption mechanisms of short chain perfluorinated sulfonic acids and perfluorooctane sulfonic acid on hydrated hematite surfaceCrossref | GoogleScholarGoogle Scholar |
Gao X, Chorover J (2012). Adsorption of perfluorooctanoic acid and perfluorooctanesulfonic acid to iron oxide surfaces as studied by flow-through ATR-FTIR spectroscopy. Environmental Chemistry 9, 148–157.
| Adsorption of perfluorooctanoic acid and perfluorooctanesulfonic acid to iron oxide surfaces as studied by flow-through ATR-FTIR spectroscopyCrossref | GoogleScholarGoogle Scholar |
Hellsing MS, Josefsson S, Hughes AV, Ahrens L (2016). Sorption of perfluoroalkyl substances to two types of minerals. Chemosphere 159, 385–391.
| Sorption of perfluoroalkyl substances to two types of mineralsCrossref | GoogleScholarGoogle Scholar |
Higgins CP, Luthy RG (2006). Sorption of perfluorinated surfactants on sediments. Environmental Science & Technology 40, 7251–7256.
| Sorption of perfluorinated surfactants on sedimentsCrossref | GoogleScholarGoogle Scholar |
Higgins CP, McLeod PB, MacManus-Spencer LA, Luthy RG (2007). Bioaccumulation of perfluorochemicals in sediments by the aquatic oligochaete Lumbriculus variegatus. Environmental Science & Technology 41, 4600–4606.
| Bioaccumulation of perfluorochemicals in sediments by the aquatic oligochaete Lumbriculus variegatusCrossref | GoogleScholarGoogle Scholar |
Ji L, Chen W, Xu Z, Zheng S, Zhu D (2013). Graphene nanosheets and graphite oxide as promising adsorbents for removal of organic contaminants from aqueous solution. Journal of Environmental Quality 42, 191–198.
| Graphene nanosheets and graphite oxide as promising adsorbents for removal of organic contaminants from aqueous solutionCrossref | GoogleScholarGoogle Scholar |
Kucharzyk KH, Darlington R, Benotti M, Deeb R, Hawley E (2017). Novel treatment technologies for PFAS compounds: A critical review. Journal of Environmental Management 204, 757–764.
| Novel treatment technologies for PFAS compounds: A critical reviewCrossref | GoogleScholarGoogle Scholar |
Kutsuna S, Hori H, Sonoda T, Iwakami T, Wakisaka A (2012). Preferential solvation of perfluorooctanoic acid (PFOA) by methanol in methanol–water mixtures: A potential overestimation of the dissociation constant of PFOA using a Yasuda–Shedlovsky plot. Atmospheric Environment 49, 411–414.
| Preferential solvation of perfluorooctanoic acid (PFOA) by methanol in methanol–water mixtures: A potential overestimation of the dissociation constant of PFOA using a Yasuda–Shedlovsky plotCrossref | GoogleScholarGoogle Scholar |
Lang JR, Allred BM, Field JA, Levis JW, Barlaz MA (2017). National estimate of per- and polyfluoroalkyl substance (PFAS) release to U.S. municipal landfill leachate. Environmental Science & Technology 51, 2197–2205.
| National estimate of per- and polyfluoroalkyl substance (PFAS) release to U.S. municipal landfill leachateCrossref | GoogleScholarGoogle Scholar |
Lath S, Navarro D, Tran D, Kumar A, Losic D, McLaughlin MJ (2018). Mixed-mode remediation of cadmium and arsenate ions using graphene-based materials. CLEAN – Soil, Air, Water 46, 1800073
| Mixed-mode remediation of cadmium and arsenate ions using graphene-based materialsCrossref | GoogleScholarGoogle Scholar |
Lee YC, Lo SL, Kuo J, Huang CP (2013). Promoted degradation of perfluorooctanic acid by persulfate when adding activated carbon. Journal of Hazardous Materials 261, 463–469.
| Promoted degradation of perfluorooctanic acid by persulfate when adding activated carbonCrossref | GoogleScholarGoogle Scholar |
Lein NPH, Fujii S, Tanaka S, Nozoe M, Tanaka H (2008). Contamination of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in surface water of the Yodo River basin (Japan). Desalination 226, 338–347.
| Contamination of perfluorooctane sulfonate (PFOS) and perfluorooctanoate (PFOA) in surface water of the Yodo River basin (Japan)Crossref | GoogleScholarGoogle Scholar |
Li C, Ji R, Schaffer A, Sequaris J-M, Amelung W, Vereecken H, Klumpp E (2012). Sorption of a branched nonylphenol and perfluorooctanoic acid on Yangtze River sediments and their model components. Journal of Environmental Monitoring 14, 2653–2658.
| Sorption of a branched nonylphenol and perfluorooctanoic acid on Yangtze River sediments and their model componentsCrossref | GoogleScholarGoogle Scholar |
Marcano DC, Kosynkin DV, Berlin JM, Sinitskii A, Sun Z, Slesarev A, Alemany LB, Lu W, Tour JM (2010). Improved synthesis of graphene oxide. ACS Nano 4, 4806–4814.
| Improved synthesis of graphene oxideCrossref | GoogleScholarGoogle Scholar |
Marttinen SK, Kettunen RH, Sormunen KM, Soimasuo RM, Rintala JA (2002). Screening of physical–chemical methods for removal of organic material, nitrogen and toxicity from low strength landfill leachates. Chemosphere 46, 851–858.
| Screening of physical–chemical methods for removal of organic material, nitrogen and toxicity from low strength landfill leachatesCrossref | GoogleScholarGoogle Scholar |
Meng P, Deng S, Lu X, Du Z, Wang B, Huang J, Wang Y, Yu G, Xing B (2014). Role of air bubbles overlooked in the adsorption of perfluorooctanesulfonate on hydrophobic carbonaceous adsorbents. Environmental Science & Technology 48, 13785–13792.
| Role of air bubbles overlooked in the adsorption of perfluorooctanesulfonate on hydrophobic carbonaceous adsorbentsCrossref | GoogleScholarGoogle Scholar |
Moody CA, Field JA (2000). Perfluorinated surfactants and the environmental implications of their use in fire-fighting foams. Environmental Science & Technology 34, 3864–3870.
| Perfluorinated surfactants and the environmental implications of their use in fire-fighting foamsCrossref | GoogleScholarGoogle Scholar |
Navarro DA, Kookana RS, McLaughlin MJ, Kirby JK (2017). Fate of radiolabeled C60 fullerenes in aged soils. Environmental Pollution 221, 293–300.
| Fate of radiolabeled C60 fullerenes in aged soilsCrossref | GoogleScholarGoogle Scholar |
Novoselov KS, Falko VI, Colombo L, Gellert PR, Schwab MG, Kim K (2012). A roadmap for graphene. Nature 490, 192–200.
| A roadmap for grapheneCrossref | GoogleScholarGoogle Scholar |
O’Hagan D (2008). Understanding organofluorine chemistry. An introduction to the C–F bond. Chemical Society Reviews 37, 308–319.
| Understanding organofluorine chemistry. An introduction to the C–F bondCrossref | GoogleScholarGoogle Scholar |
Renner R (2001). Growing concern over perfluorinated chemicals. Environmental Science & Technology 35, 154A–160A.
| Growing concern over perfluorinated chemicalsCrossref | GoogleScholarGoogle Scholar |
Ross I, McDonough J, Miles J, Storch P, Thelakkat Kochunarayanan P, Kalve E, Hurst J, Dasgupta SS, Burdick J (2018). A review of emerging technologies for remediation of PFASs. Remediation Journal 28, 101–126.
| A review of emerging technologies for remediation of PFASsCrossref | GoogleScholarGoogle Scholar |
Rumsby PC, McLaughlin CL, Hall T (2009). Perfluorooctane sulphonate and perfluorooctanoic acid in drinking and environmental waters. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences 367, 4119–4136.
| Perfluorooctane sulphonate and perfluorooctanoic acid in drinking and environmental watersCrossref | GoogleScholarGoogle Scholar |
Sundström M, Ehresman DJ, Bignert A, Butenhoff JL, Olsen GW, Chang S-C, Bergman A (2011). A temporal trend study (1972–2008) of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in pooled human milk samples from Stockholm, Sweden. Environment International 37, 178–183.
| A temporal trend study (1972–2008) of perfluorooctanesulfonate, perfluorohexanesulfonate, and perfluorooctanoate in pooled human milk samples from Stockholm, SwedenCrossref | GoogleScholarGoogle Scholar |
Wang F, Shih K (2011). Adsorption of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) on alumina: Influence of solution pH and cations. Water Research 45, 2925–2930.
| Adsorption of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) on alumina: Influence of solution pH and cationsCrossref | GoogleScholarGoogle Scholar |
Wang F, Liu C, Shih K (2012). Adsorption behavior of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) on boehmite. Chemosphere 89, 1009–1014.
| Adsorption behavior of perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA) on boehmiteCrossref | GoogleScholarGoogle Scholar |
Wang Y, Niu J, Li Y, Zheng T, Xu Y, Liu Y (2015). Performance and mechanisms for removal of perfluorooctanoate (PFOA) from aqueous solution by activated carbon fiber. RSC Advances 5, 86927–86933.
| Performance and mechanisms for removal of perfluorooctanoate (PFOA) from aqueous solution by activated carbon fiberCrossref | GoogleScholarGoogle Scholar |
Washington JW, Yoo H, Ellington JJ, Jenkins TM, Libelo EL (2010). Concentrations, distribution, and persistence of perfluoroalkylates in sludge-applied soils near Decatur, Alabama, USA. Environmental Science & Technology 44, 8390–8396.
| Concentrations, distribution, and persistence of perfluoroalkylates in sludge-applied soils near Decatur, Alabama, USACrossref | GoogleScholarGoogle Scholar |
Xiao X, Ulrich BA, Chen B, Higgins CP (2017). Sorption of poly- and perfluoroalkyl substances (PFASs) relevant to aqueous film-forming foam (AFFF)-impacted groundwater by biochars and activated carbon. Environmental Science & Technology 51, 6342–6351.
| Sorption of poly- and perfluoroalkyl substances (PFASs) relevant to aqueous film-forming foam (AFFF)-impacted groundwater by biochars and activated carbonCrossref | GoogleScholarGoogle Scholar |
Yusuf M, Elfghi FM, Zaidi SA, Abdullah EC, Khan MA (2015). Applications of graphene and its derivatives as an adsorbent for heavy metal and dye removal: a systematic and comprehensive overview. RSC Advances 5, 50392–50420.
| Applications of graphene and its derivatives as an adsorbent for heavy metal and dye removal: a systematic and comprehensive overviewCrossref | GoogleScholarGoogle Scholar |
Zareitalabad P, Siemens J, Hamer M, Amelung W (2013). Perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) in surface waters, sediments, soils and wastewater–A review on concentrations and distribution coefficients. Chemosphere 91, 725–732.
| Perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) in surface waters, sediments, soils and wastewater–A review on concentrations and distribution coefficientsCrossref | GoogleScholarGoogle Scholar |
Zhao C, Fan J, Chen D, Xu Y, Wang T (2016). Microfluidics-generated graphene oxide microspheres and their application to removal of perfluorooctane sulfonate from polluted water. Nano Research 9, 866–875.
| Microfluidics-generated graphene oxide microspheres and their application to removal of perfluorooctane sulfonate from polluted waterCrossref | GoogleScholarGoogle Scholar |
Zhi Y, Liu J (2015). Adsorption of perfluoroalkyl acids by carbonaceous adsorbents: Effect of carbon surface chemistry. Environmental Pollution 202, 168–176.
| Adsorption of perfluoroalkyl acids by carbonaceous adsorbents: Effect of carbon surface chemistryCrossref | GoogleScholarGoogle Scholar |
