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Title: Trace Adsorptive Removal of PFAS from Water by Optimizing the UiO‐66 MOF Interface

Journal Article · · Advanced Materials
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [5]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [3]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [8]
  1. Chair of Urban Water Systems Engineering Technical University of Munich Am Coulombwall 3 85748 Garching Germany
  2. Department of Chemistry University of North Texas 1155 Union Cir Denton TX 76203 USA
  3. Chair of Simulation of Nanosystems for Energy Conversion, Department of Electrical Engineering, TUM School of Computation, Information and Technology Technical University of Munich Hans‐Piloty‐Straße 1 85748 Garching Germany
  4. Chair of Inorganic and Metal‐Organic Chemistry, Catalysis Research Center School of Natural Sciences Technical University of Munich 85748 Garching Germany
  5. Chair of Urban Water Systems Engineering Technical University of Munich Am Coulombwall 3 85748 Garching Germany, Xylem Services GmbH Boschstraße 4–14 32051 Herford Germany
  6. Bernal Institute, Department of Chemical Sciences University of Limerick Limerick V94 T9PX Ireland
  7. Inorganic Chemistry I Technische Universität Dresden Bergstraße 66 01069 Dresden Germany
  8. Chair of Inorganic and Metal‐Organic Chemistry, Catalysis Research Center School of Natural Sciences Technical University of Munich 85748 Garching Germany, Bernal Institute, Department of Chemical Sciences University of Limerick Limerick V94 T9PX Ireland

Abstract The confluence of pervasiveness, bioaccumulation, and toxicity in freshwater contaminants presents an environmental threat second to none. Exemplifying this trifecta, per‐ and polyfluoroalkyl substances (PFAS) present an alarming hazard among the emerging contaminants. State‐of‐the‐art PFAS adsorbents used in drinking water treatment, namely, activated carbons and ion‐exchange resins, are handicapped by low adsorption capacity, competitive adsorption, and/or slow kinetics. To overcome these shortcomings, metal–organic frameworks (MOFs) with tailored pore size, surface, and pore chemistry are promising alternatives. Thanks to the compositional modularity of MOFs and polymer–MOF composites, herein we report on a series of water‐stable zirconium carboxylate MOFs and their low‐cost polymer‐grafted composites as C 8 –PFAS adsorbents with benchmark kinetics and “parts per billion” removal efficiencies. Bespoke insights into the structure–function relationships of PFAS adsorbents are obtained by leveraging interfacial design principles on solid sorbents, creating a synergy between the extrinsic particle surfaces and intrinsic molecular building blocks.

Sponsoring Organization:
USDOE
Grant/Contract Number:
SC0019902
OSTI ID:
2478547
Journal Information:
Advanced Materials, Journal Name: Advanced Materials Journal Issue: 6 Vol. 37; ISSN 0935-9648
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English

References (53)

Stable Metal-Organic Frameworks: Design, Synthesis, and Applications journal February 2018
Metal–Organic Framework Materials for the Separation and Purification of Light Hydrocarbons journal May 2019
Hydrophobic Metal–Organic Frameworks journal June 2019
Hydrophobic Metal–Organic Frameworks: Assessment, Construction, and Diverse Applications journal January 2020
Thermodynamics of mixed-gas adsorption journal January 1965
Perfluoroalkyl and polyfluoroalkyl substances in the environment: Terminology, classification, and origins journal September 2011
Rational design and synthesis of ultramicroporous metal-organic frameworks for gas separation journal November 2020
Adsorption behavior and mechanism of emerging perfluoro-2-propoxypropanoic acid (GenX) on activated carbons and resins journal May 2019
Regulation and synthesis of metal–organic frameworks through mixed-ligand strategy: A pathway to enhance adsorption of perfluoroalkyl acids journal September 2024
Treatment technologies for aqueous perfluorooctanesulfonate (PFOS) and perfluorooctanoate (PFOA): A critical review with an emphasis on field testing journal October 2015
An Encapsulation-Rearrangement Strategy to Integrate Superhydrophobicity into Mesoporous Metal-Organic Frameworks journal April 2020
Metal-organic frameworks as platforms for the removal of per- and polyfluoroalkyl substances from contaminated waters journal October 2022
Influence of crystal topology and interior surface functionality of metal-organic frameworks on PFOA sorption performance journal December 2016
Is sorption technology fit for the removal of persistent and mobile organic contaminants from water? journal July 2023
GROMACS: High performance molecular simulations through multi-level parallelism from laptops to supercomputers journal September 2015
Hydrophobicity: a key factor en route to applications of metal–organic frameworks journal November 2021
Fate of Perfluorooctanesulfonate and perfluorooctanoate in drinking water treatment processes journal July 2011
Behaviour and fate of perfluoroalkyl and polyfluoroalkyl substances (PFASs) in drinking water treatment: A review journal March 2014
Treatment of poly- and perfluoroalkyl substances in U.S. full-scale water treatment systems journal March 2014
Life cycle assessment and life cycle cost analysis of anion exchange and granular activated carbon systems for remediation of groundwater contaminated by per- and polyfluoroalkyl substances (PFASs) journal September 2023
Efficient Removal of Per- and Polyfluoroalkyl Substances from Water with Zirconium-Based Metal–Organic Frameworks journal April 2021
Functionalizing the Defects: Postsynthetic Ligand Exchange in the Metal Organic Framework UiO-66 journal October 2016
Room-Temperature Synthesis of UiO-66 and Thermal Modulation of Densities of Defect Sites journal January 2017
MOF-Polymer Hybrid Materials: From Simple Composites to Tailored Architectures journal January 2020
Understanding the Adsorption of PFOA on MIL-101(Cr)-Based Anionic-Exchange Metal–Organic Frameworks: Comparing DFT Calculations with Aqueous Sorption Experiments journal July 2015
Detection of Poly- and Perfluoroalkyl Substances (PFASs) in U.S. Drinking Water Linked to Industrial Sites, Military Fire Training Areas, and Wastewater Treatment Plants journal August 2016
Efficient PFAS Removal by Amine-Functionalized Sorbents: Critical Review of the Current Literature journal October 2019
Tailoring the Properties of UiO-66 through Defect Engineering: A Review journal August 2019
A Modulated Hydrothermal (MHT) Approach for the Facile Synthesis of UiO-66-Type MOFs journal April 2015
Computational Investigation of Structure–Function Relationship in Fluorine-Functionalized MOFs for PFOA Capture from Water journal February 2023
Electrodeposition of Ag/ZIF-8-Modified Membrane for Water Remediation journal January 2023
Separation of Perfluorooctanoic Acid from Water Using Meso- and Macroporous Syndiotactic Polystyrene Gels journal May 2024
The Price of Really Clean Water: Combining Nanofiltration with Granular Activated Carbon and Anion Exchange Resins for the Removal of Per- And Polyfluoralkyl Substances (PFASs) in Drinking Water Production journal January 2021
Accurate Enthalpies of Formation for PFAS from First-Principles: Combining Different Levels of Theory in a Generalized Thermochemical Hierarchy journal February 2024
Highly Defective UiO-66 Materials for the Adsorptive Removal of Perfluorooctanesulfonate journal March 2019
Detailed Structure Analysis of Atomic Positions and Defects in Zirconium Metal–Organic Frameworks journal October 2014
Synthesis and Stability of Tagged UiO-66 Zr-MOFs journal December 2010
Perfluorooctanesulfonate and Related Fluorochemicals in Human Blood from Several Countries journal September 2004
A Facile and General Coating Approach to Moisture/Water-Resistant Metal–Organic Frameworks with Intact Porosity journal November 2014
A New Zirconium Inorganic Building Brick Forming Metal Organic Frameworks with Exceptional Stability
  • Cavka, Jasmina Hafizovic; Jakobsen, Søren; Olsbye, Unni
  • Journal of the American Chemical Society, Vol. 130, Issue 42, p. 13850-13851 https://doi.org/10.1021/ja8057953
journal October 2008
Exceptionally High Perfluorooctanoic Acid Uptake in Water by a Zirconium-Based Metal–Organic Framework through Synergistic Chemical and Physical Adsorption journal March 2024
Chemical, thermal and mechanical stabilities of metal–organic frameworks journal February 2016
A mesoporous cationic thorium-organic framework that rapidly traps anionic persistent organic pollutants journal November 2017
Imaging defects and their evolution in a metal–organic framework at sub-unit-cell resolution journal May 2019
Water adsorption in UiO-66: the importance of defects journal January 2014
Vacancy defect configurations in the metal–organic framework UiO-66: energetics and electronic structure journal January 2018
Metal–organic framework sorbents for the removal of perfluorinated compounds in an aqueous environment journal January 2018
A new post-synthetic polymerization strategy makes metal–organic frameworks more stable journal January 2019
A switchable sensor and scavenger: detection and removal of fluorinated chemical species by a luminescent metal–organic framework journal January 2021
Hydrophobicity and dielectric properties across an isostructural family of MOFs: a duet or a duel? journal January 2022
Adsorption as a remediation technology for short-chain per- and polyfluoroalkyl substances (PFAS) from water – a critical review journal January 2023
Superhydrophobic perfluorinated metal–organic frameworks journal January 2013
Water Treatment Technologies for PFAS: The Next Generation journal April 2018