Dual-Functional Nanofiltration and Adsorptive Membranes for PFAS and Organics Separation from Water

Francisco Léniz-Pizarro; Ronald J. Vogler; Phillip Sandman; Natalie Harris; Lindell E. Ormsbee; Chunqing Liu; Dibakar Bhattacharyya

doi:10.1021/acsestwater.2c00043

Dual-Functional Nanofiltration and Adsorptive Membranes for PFAS and Organics Separation from Water

Francisco Léniz-Pizarro, Ronald J. Vogler, Phillip Sandman, Natalie Harris, Lindell E. Ormsbee, Chunqing Liu, Dibakar Bhattacharyya

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

Challenges associated with water separation technologies for per- and polyfluoroalkyl substances (PFASs) require efficient and sustainable processes supported by a proper understanding of the separation mechanisms. The solute rejections by nanofiltration (NF) at pH values near the membrane isoelectric point were compared to the size- and mass-transfer-dependent modeled rejection rates of these compounds in an ionized state. We find that the low pKa value of perfluorooctanoic acid (PFOA) relates to enhanced solute exclusions by minimizing the presence and partitioning of the protonated organic compound into the membrane domain. The effects of Donnan exclusion are moderate, and co-ion transport also contributes to the PFAS rejection rates. An additional support barrier with thermo-responsive (quantified by water permeance variation) adsorption/desorption properties allows for enhanced separations of PFAS. This was possible by successfully synthesizing an NF layer on top of a poly-N-isopropylacrylamide (PNIPAm) pore-functionalized microfiltration support structure. The support layer adsorbs organics (178 mg PFOA adsorbed/m2 membrane at an equilibrium concentration of 70 mg/L), and the simultaneous exclusion from the NF layer allows separations of PFOA and the smaller sized heptafluorobutyric acid from solutions containing 70 μg/L of these compounds at a high water flux of 100 L/m2-h at 7 bar.

Original language	English
Journal	ACS Environmental Science and Technology Water
DOIs	https://doi.org/10.1021/acsestwater.2c00043
State	Accepted/In press - 2022

Bibliographical note

Funding Information:
Research reported in this publication was supported by the National Institute of Environmental Health Sciences of the National Institutes of Health under Award Number P42ES007380. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. Partial support was also provided by Honeywell UOP. The authors would like to thank Dr. Andrew Morris, Dr. Abigail Burrows, Dr. Scott Stanley, and Michael Hedge for the time, assistance, and analytical support on LC-MS/MS analysis. Additionally, thanks to Benjamin Weaver and Solecta for providing technical expertise and the PVDF400 membranes. Also, thanks to Dr. Nicolas Briot for SEM assistance and Nicholas Cprek for helping to create the crossflow membrane testing unit.

Publisher Copyright:
© 2022 American Chemical Society.

Keywords

PFAS
organic anions
responsive materials
water treatment

ASJC Scopus subject areas

Chemical Engineering (miscellaneous)
Chemistry (miscellaneous)
Environmental Chemistry
Water Science and Technology

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10.1021/acsestwater.2c00043

Cite this

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title = "Dual-Functional Nanofiltration and Adsorptive Membranes for PFAS and Organics Separation from Water",

abstract = "Challenges associated with water separation technologies for per- and polyfluoroalkyl substances (PFASs) require efficient and sustainable processes supported by a proper understanding of the separation mechanisms. The solute rejections by nanofiltration (NF) at pH values near the membrane isoelectric point were compared to the size- and mass-transfer-dependent modeled rejection rates of these compounds in an ionized state. We find that the low pKa value of perfluorooctanoic acid (PFOA) relates to enhanced solute exclusions by minimizing the presence and partitioning of the protonated organic compound into the membrane domain. The effects of Donnan exclusion are moderate, and co-ion transport also contributes to the PFAS rejection rates. An additional support barrier with thermo-responsive (quantified by water permeance variation) adsorption/desorption properties allows for enhanced separations of PFAS. This was possible by successfully synthesizing an NF layer on top of a poly-N-isopropylacrylamide (PNIPAm) pore-functionalized microfiltration support structure. The support layer adsorbs organics (178 mg PFOA adsorbed/m2 membrane at an equilibrium concentration of 70 mg/L), and the simultaneous exclusion from the NF layer allows separations of PFOA and the smaller sized heptafluorobutyric acid from solutions containing 70 μg/L of these compounds at a high water flux of 100 L/m2-h at 7 bar.",

keywords = "PFAS, organic anions, responsive materials, water treatment",

author = "Francisco L{\'e}niz-Pizarro and Vogler, {Ronald J.} and Phillip Sandman and Natalie Harris and Ormsbee, {Lindell E.} and Chunqing Liu and Dibakar Bhattacharyya",

note = "Funding Information: Research reported in this publication was supported by the National Institute of Environmental Health Sciences of the National Institutes of Health under Award Number P42ES007380. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. Partial support was also provided by Honeywell UOP. The authors would like to thank Dr. Andrew Morris, Dr. Abigail Burrows, Dr. Scott Stanley, and Michael Hedge for the time, assistance, and analytical support on LC-MS/MS analysis. Additionally, thanks to Benjamin Weaver and Solecta for providing technical expertise and the PVDF400 membranes. Also, thanks to Dr. Nicolas Briot for SEM assistance and Nicholas Cprek for helping to create the crossflow membrane testing unit. Publisher Copyright: {\textcopyright} 2022 American Chemical Society.",

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TY - JOUR

T1 - Dual-Functional Nanofiltration and Adsorptive Membranes for PFAS and Organics Separation from Water

AU - Léniz-Pizarro, Francisco

AU - Vogler, Ronald J.

AU - Sandman, Phillip

AU - Harris, Natalie

AU - Ormsbee, Lindell E.

AU - Liu, Chunqing

AU - Bhattacharyya, Dibakar

N1 - Funding Information: Research reported in this publication was supported by the National Institute of Environmental Health Sciences of the National Institutes of Health under Award Number P42ES007380. The content is solely the responsibility of the authors and does not necessarily represent the official views of the National Institutes of Health. Partial support was also provided by Honeywell UOP. The authors would like to thank Dr. Andrew Morris, Dr. Abigail Burrows, Dr. Scott Stanley, and Michael Hedge for the time, assistance, and analytical support on LC-MS/MS analysis. Additionally, thanks to Benjamin Weaver and Solecta for providing technical expertise and the PVDF400 membranes. Also, thanks to Dr. Nicolas Briot for SEM assistance and Nicholas Cprek for helping to create the crossflow membrane testing unit. Publisher Copyright: © 2022 American Chemical Society.

PY - 2022

Y1 - 2022

N2 - Challenges associated with water separation technologies for per- and polyfluoroalkyl substances (PFASs) require efficient and sustainable processes supported by a proper understanding of the separation mechanisms. The solute rejections by nanofiltration (NF) at pH values near the membrane isoelectric point were compared to the size- and mass-transfer-dependent modeled rejection rates of these compounds in an ionized state. We find that the low pKa value of perfluorooctanoic acid (PFOA) relates to enhanced solute exclusions by minimizing the presence and partitioning of the protonated organic compound into the membrane domain. The effects of Donnan exclusion are moderate, and co-ion transport also contributes to the PFAS rejection rates. An additional support barrier with thermo-responsive (quantified by water permeance variation) adsorption/desorption properties allows for enhanced separations of PFAS. This was possible by successfully synthesizing an NF layer on top of a poly-N-isopropylacrylamide (PNIPAm) pore-functionalized microfiltration support structure. The support layer adsorbs organics (178 mg PFOA adsorbed/m2 membrane at an equilibrium concentration of 70 mg/L), and the simultaneous exclusion from the NF layer allows separations of PFOA and the smaller sized heptafluorobutyric acid from solutions containing 70 μg/L of these compounds at a high water flux of 100 L/m2-h at 7 bar.

AB - Challenges associated with water separation technologies for per- and polyfluoroalkyl substances (PFASs) require efficient and sustainable processes supported by a proper understanding of the separation mechanisms. The solute rejections by nanofiltration (NF) at pH values near the membrane isoelectric point were compared to the size- and mass-transfer-dependent modeled rejection rates of these compounds in an ionized state. We find that the low pKa value of perfluorooctanoic acid (PFOA) relates to enhanced solute exclusions by minimizing the presence and partitioning of the protonated organic compound into the membrane domain. The effects of Donnan exclusion are moderate, and co-ion transport also contributes to the PFAS rejection rates. An additional support barrier with thermo-responsive (quantified by water permeance variation) adsorption/desorption properties allows for enhanced separations of PFAS. This was possible by successfully synthesizing an NF layer on top of a poly-N-isopropylacrylamide (PNIPAm) pore-functionalized microfiltration support structure. The support layer adsorbs organics (178 mg PFOA adsorbed/m2 membrane at an equilibrium concentration of 70 mg/L), and the simultaneous exclusion from the NF layer allows separations of PFOA and the smaller sized heptafluorobutyric acid from solutions containing 70 μg/L of these compounds at a high water flux of 100 L/m2-h at 7 bar.

KW - PFAS

KW - organic anions

KW - responsive materials

KW - water treatment

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DO - 10.1021/acsestwater.2c00043

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Dual-Functional Nanofiltration and Adsorptive Membranes for PFAS and Organics Separation from Water

Abstract

Bibliographical note

Keywords

ASJC Scopus subject areas

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