A graphene-based hydrogel monolith with tailored surface chemistry for PFAS passive sampling

Bečanová, Jitka; Saleeba, Zachary S. S. L.; Stone, Aidan; Robuck, Anna R.; Hurt, Robert H.; Lohmann, Rainer

doi:10.1039/d1en00517k

Cited by 25 publications

(26 citation statements)

References 62 publications

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“…Each trial consisted of a 14 day deployment, where duplicate 50 mL water grab samples were taken at the beginning and end of each deployment to verify PFAS concentrations during deployments (Figure S3). Water samples were extracted and analyzed in accordance with methods detailed in literature and used to calculate sampling rates for corresponding individual passive samplers using eq . , For additional details on the experimental tank design and construction, see the SI.…”

Section: Methodsmentioning

confidence: 99%

“…Integrative samplers report time-weighted averages of water concentrations that can give a more representative depiction of surface water contamination across diurnal, tidal, and seasonal trends than discrete grab sampling . ,,− Other passive sampler designs such as the diffusive gradient in thin film (DGT) samplers have been investigated for PFAS in surface waters. − Recently, an equilibrium-based sampler for PFAS was investigated using modified nanographene hydrogel to create a water-based sampler as opposed to sorbent-based sampler . This study was hence performed to calibrate and validate an integrative passive sampler based on a microporous polyethylene tube sampler filled with sorbent for the accumulated of dissolved PFAS in surface waters.…”

Section: Introductionmentioning

confidence: 99%

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Calibration of Perfluorinated Alkyl Acid Uptake Rates by a Tube Passive Sampler in Water

et al. 2023

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Per- and polyfluoroalkyl substances (PFAS) are a group of 4000+ man-made compounds of great concern due to their environmental ubiquity and adverse effects. Despite general interest, few reliable detection tools for integrative passive sampling of PFAS in water are available. A microporous polyethylene tube with a hydrophilic–lipophilic balance sorbent could serve as a flow-resistant passive sampler for PFAS. The tube’s sampling rate, R s, was predicted based on either partitioning and diffusion or solely diffusion. At 15 °C, the laboratory-measured R s for perfluorohexanoic acid of 100 ± 81 mL day–1 was better predicted by a partitioning and diffusion model (48 ± 1.8 mL day–1) across 10–60 cm s–1 water flow speeds (15 ± 4.2 mL day–1 diffusion only). For perfluorohexane sulfonate, R s at 15 °C were similarly different (110 ± 60 mL day–1 measured, 120 ± 63 versus 12 ± 3.4 mL day–1 in respective models). R s values from field deployments were in between these estimates (46 ± 40 mL day–1 for perfluorohexanoic acid). PFAS uptake was not different for previously biofouled membranes in the laboratory, suggesting the general applicability of the sampler in environmental conditions. This research demonstrates that the polyethylene tube’s sampling rates are sensitive to the parameterization of the models used here and partitioning-derived values should be used.

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Section: Methodsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Calibration of Perfluorinated Alkyl Acid Uptake Rates by a Tube Passive Sampler in Water

et al. 2023

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“…One possible explanation could be attributed to the higher hydrophobicity of PFOS, which has previously been observed to adsorb more strongly than PFOA onto single- and multiwalled carbon nanotubes. , Other possibilities are the lower pKa of PFOS and the higher number of hydrogen-bonding sites per molecule of PFOS. A possible solution to enhance PFOA adsorption would be functionalization of graphene with positively charged functional groups like amine-functionalized graphene . Such approaches could enhance selectivity for certain PFAS molecules and could be implemented as strategies for multiplexed printed SERS patches.…”

Section: Resultsmentioning

confidence: 99%

“…A possible solution to enhance PFOA adsorption would be functionalization of graphene with positively charged functional groups like amine-functionalized graphene. 50 Such approaches could enhance selectivity for certain PFAS molecules and could be implemented as strategies for multiplexed printed SERS patches. This will be important for future SERS measurements of real-world contaminated water and surfaces, which are expected to contain a variety of PFAS molecules among other possible contaminants.…”

Section: Resultsmentioning

confidence: 99%

Aerosol Jet Printed Surface-Enhanced Raman Substrates: Application for High-Sensitivity Detection of Perfluoroalkyl Substances

et al. 2022

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Printing technologies offer an attractive means for producing low-cost surface-enhanced Raman spectroscopy (SERS) substrates with high-throughput methods. The development of these substrates is especially important for field-deployable detection of environmental contaminants. Toward this end, we demonstrate SERS-based substrates fabricated through aerosol jet printing of silver nanoparticles and graphene inks on Kapton films. Our printed arrays exhibited measurable intensities for fluorescein and rhodamine dyes down to concentrations of 10–7 M, with the highest SERS intensities obtained for four print passes of Ag nanoparticles. The substrates also exhibited an excellent shelf life, with little reduction in fluorescein intensities after 9 months of shelf storage. We also demonstrated the capability of our substrates to sense perfluoroalkyl substances (PFAS), the so-called forever chemicals that resist degradation due to their strong C–F bonds and persist in the environment. Interestingly, the addition of graphene to the Ag nanoparticles greatly enhanced the SERS intensity of the perfluorooctanoic acid (PFOA) and perfluorooctanesulfonic acid (PFOS) molecules under basic conditions (pH ∼ 9) compared to that of fluorescein and rhodamine. We were able to successfully detect SERS spectra from nano- and picomolar (∼0.4 ppt) concentrations of PFOA and PFOS, respectively, demonstrating the viability of deploying our SERS sensors in the environment for the ultrasensitive detection of contaminants.

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“…Some passive samplers are designed to equilibrate with resident concentrations (Becanova et al 2021;Britt et al 2010) while others are more "integrative," representing a time-weighted average concentration (Kaserzon et al 2014(Kaserzon et al , 2019Cao et al 2018;Dixon-Anderson and Lohmann 2018;Guan et al 2018;Hartmann et al 2021). To date, only a few field studies have been published comparing the results of passive and no-purge sampling to conventional methods for PFAS sampling.…”

Section: Passive and No-purge Samplingmentioning

confidence: 99%

Where Is the PFAS? Innovations in PFAS Detection and Characterization

Horst¹,

Divine²,

Quinnan³

et al. 2022

Groundwater Monitoring Rem

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This column reviews the general features of PHT3D Version 2, a reactive multicomponent transport model that couples the geochemical modeling software PHREEQC-2 (Parkhurst and Appelo 1999) with three-dimensional groundwater flow and transport simulators MODFLOW-2000 and MT3DMS (Zheng and Wang 1999). The original version of PHT3D was developed by Henning Prommer and Version 2 by Henning Prommer and Vincent Post (Prommer and Post 2010). More detailed information about PHT3D is available at the website http://www.pht3d.org.The review was conducted separately by two reviewers. This column is presented in two parts.

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A graphene-based hydrogel monolith with tailored surface chemistry for PFAS passive sampling

Abstract: Aquatic contamination by per- and polyfluorinated alkyl substances (PFAS) has attracted global attention due to their environmental and health concerns. Current health advisories and surface water regulatory limits require PFAS...

Cited by 25 publications

References 62 publications

Calibration of Perfluorinated Alkyl Acid Uptake Rates by a Tube Passive Sampler in Water

Calibration of Perfluorinated Alkyl Acid Uptake Rates by a Tube Passive Sampler in Water

Aerosol Jet Printed Surface-Enhanced Raman Substrates: Application for High-Sensitivity Detection of Perfluoroalkyl Substances

Where Is the PFAS? Innovations in PFAS Detection and Characterization

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