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Title: Iron detection and remediation with a functionalized porous polymer applied to environmental water samples

Abstract

Iron is one of the most abundant elements in the environment and in the human body. As an essential nutrient, iron homeostasis is tightly regulated, and iron dysregulation is implicated in numerous pathologies, including neuro-degenerative diseases, atherosclerosis, and diabetes. Endogenous iron pool concentrations are directly linked to iron ion uptake from environmental sources such as drinking water, providing motivation for developing new technologies for assessing iron(II) and iron(III) levels in water. However, conventional methods for measuring aqueous iron pools remain laborious and costly and often require sophisticated equipment and/or additional processing steps to remove the iron ions from the original environmental source. We now report a simplified and accurate chemical platform for capturing and quantifying the iron present in aqueous samples through use of a post-synthetically modified porous aromatic framework (PAF). The ether/thioether-functionalized network polymer, PAF-1–ET, exhibits high selectivity for the uptake of iron(II) and iron(III) over other physiologically and environmentally relevant metal ions. Mössbauer spectroscopy, XANES, and EXAFS measurements provide evidence to support iron(III) coordination to oxygen-based ligands within the material. The polymer is further successfully employed to adsorb and remove iron ions from groundwater, including field sources in West Bengal, India. Combined with an 8-hydroxyquinoline colorimetric indicator, PAF-1–ETmore » enables the simple and direct determination of the iron(II) and iron(III) ion concentrations in these samples, providing a starting point for the design and use of molecularly-functionalized porous materials for potential dual detection and remediation applications.« less

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [1];  [1];  [3];  [4]; ORCiD logo [2];  [1];  [4]; ORCiD logo [1]; ORCiD logo [5];  [4];  [3]; ORCiD logo [6]; ORCiD logo [6]; ORCiD logo [7]; ORCiD logo [8]
  1. Department of Chemistry, University of California, Berkeley, USA
  2. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, USA
  3. Department of Civil and Environmental Engineering, University of California, Berkeley, USA
  4. Molecular Biophysics and Integrated Bioimaging Division, Lawrence Berkeley National Laboratory, Berkeley, USA
  5. Department of Chemical and Biomolecular Engineering, University of California, Berkeley, USA, Materials Sciences Division
  6. Department of Chemistry, Missouri University of Science and Technology, University of Missouri, Rolla, USA
  7. Department of Chemistry, University of California, Berkeley, USA, Department of Chemical and Biomolecular Engineering
  8. Department of Chemistry, University of California, Berkeley, USA, Department of Molecular and Cell Biology
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Gas Separations Relevant to Clean Energy Technologies (CGS); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1524484
Alternate Identifier(s):
OSTI ID: 1559810
Grant/Contract Number:  
AC02-05CH11231; SC0001015
Resource Type:
Published Article
Journal Name:
Chemical Science
Additional Journal Information:
Journal Name: Chemical Science Journal Volume: 10 Journal Issue: 27; Journal ID: ISSN 2041-6520
Publisher:
Royal Society of Chemistry (RSC)
Country of Publication:
United Kingdom
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Lee, Sumin, Uliana, Adam, Taylor, Mercedes K., Chakarawet, Khetpakorn, Bandaru, Siva Rama Satyam, Gul, Sheraz, Xu, Jun, Ackerman, Cheri M., Chatterjee, Ruchira, Furukawa, Hiroyasu, Reimer, Jeffrey A., Yano, Junko, Gadgil, Ashok, Long, Gary J., Grandjean, Fernande, Long, Jeffrey R., and Chang, Christopher J.. Iron detection and remediation with a functionalized porous polymer applied to environmental water samples. United Kingdom: N. p., 2019. Web. doi:10.1039/C9SC01441A.
Lee, Sumin, Uliana, Adam, Taylor, Mercedes K., Chakarawet, Khetpakorn, Bandaru, Siva Rama Satyam, Gul, Sheraz, Xu, Jun, Ackerman, Cheri M., Chatterjee, Ruchira, Furukawa, Hiroyasu, Reimer, Jeffrey A., Yano, Junko, Gadgil, Ashok, Long, Gary J., Grandjean, Fernande, Long, Jeffrey R., & Chang, Christopher J.. Iron detection and remediation with a functionalized porous polymer applied to environmental water samples. United Kingdom. https://doi.org/10.1039/C9SC01441A
Lee, Sumin, Uliana, Adam, Taylor, Mercedes K., Chakarawet, Khetpakorn, Bandaru, Siva Rama Satyam, Gul, Sheraz, Xu, Jun, Ackerman, Cheri M., Chatterjee, Ruchira, Furukawa, Hiroyasu, Reimer, Jeffrey A., Yano, Junko, Gadgil, Ashok, Long, Gary J., Grandjean, Fernande, Long, Jeffrey R., and Chang, Christopher J.. Wed . "Iron detection and remediation with a functionalized porous polymer applied to environmental water samples". United Kingdom. https://doi.org/10.1039/C9SC01441A.
@article{osti_1524484,
title = {Iron detection and remediation with a functionalized porous polymer applied to environmental water samples},
author = {Lee, Sumin and Uliana, Adam and Taylor, Mercedes K. and Chakarawet, Khetpakorn and Bandaru, Siva Rama Satyam and Gul, Sheraz and Xu, Jun and Ackerman, Cheri M. and Chatterjee, Ruchira and Furukawa, Hiroyasu and Reimer, Jeffrey A. and Yano, Junko and Gadgil, Ashok and Long, Gary J. and Grandjean, Fernande and Long, Jeffrey R. and Chang, Christopher J.},
abstractNote = {Iron is one of the most abundant elements in the environment and in the human body. As an essential nutrient, iron homeostasis is tightly regulated, and iron dysregulation is implicated in numerous pathologies, including neuro-degenerative diseases, atherosclerosis, and diabetes. Endogenous iron pool concentrations are directly linked to iron ion uptake from environmental sources such as drinking water, providing motivation for developing new technologies for assessing iron(II) and iron(III) levels in water. However, conventional methods for measuring aqueous iron pools remain laborious and costly and often require sophisticated equipment and/or additional processing steps to remove the iron ions from the original environmental source. We now report a simplified and accurate chemical platform for capturing and quantifying the iron present in aqueous samples through use of a post-synthetically modified porous aromatic framework (PAF). The ether/thioether-functionalized network polymer, PAF-1–ET, exhibits high selectivity for the uptake of iron(II) and iron(III) over other physiologically and environmentally relevant metal ions. Mössbauer spectroscopy, XANES, and EXAFS measurements provide evidence to support iron(III) coordination to oxygen-based ligands within the material. The polymer is further successfully employed to adsorb and remove iron ions from groundwater, including field sources in West Bengal, India. Combined with an 8-hydroxyquinoline colorimetric indicator, PAF-1–ET enables the simple and direct determination of the iron(II) and iron(III) ion concentrations in these samples, providing a starting point for the design and use of molecularly-functionalized porous materials for potential dual detection and remediation applications.},
doi = {10.1039/C9SC01441A},
journal = {Chemical Science},
number = 27,
volume = 10,
place = {United Kingdom},
year = {2019},
month = {7}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/C9SC01441A

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Cited by: 23 works
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Works referencing / citing this record:

Functionalized Porous Aromatic Frameworks as High‐Performance Adsorbents for the Rapid Removal of Boric Acid from Water
journal, February 2019

  • Kamcev, Jovan; Taylor, Mercedes K.; Shin, Dong‐Myeong
  • Advanced Materials, Vol. 31, Issue 18
  • DOI: 10.1002/adma.201808027

Conjugated Microporous Poly(aryleneethynylene) Networks
journal, September 2007

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Targeted Synthesis of a Porous Aromatic Framework with High Stability and Exceptionally High Surface Area
journal, November 2009

  • Ben, Teng; Ren, Hao; Ma, Shengqian
  • Angewandte Chemie International Edition, Vol. 48, Issue 50, p. 9457-9460
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Polyamine-Tethered Porous Polymer Networks for Carbon Dioxide Capture from Flue Gas
journal, June 2012

  • Lu, Weigang; Sculley, Julian P.; Yuan, Daqiang
  • Angewandte Chemie International Edition, Vol. 51, Issue 30, p. 7480-7484
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A Ratiometric Fluorescent Probe for Rapid Detection of Hydrogen Sulfide in Mitochondria
journal, January 2013

  • Chen, Yuncong; Zhu, Chengcheng; Yang, Zhenghao
  • Angewandte Chemie International Edition, Vol. 52, Issue 6
  • DOI: 10.1002/anie.201207701

Iron(III), cobalt(II) and copper(II) complexes bearing 8-quinolinol encapsulated in zeoliteY for the aerobic oxidation of styrene
journal, March 2011

  • Yang, Ying; Ding, Hong; Hao, Shijie
  • Applied Organometallic Chemistry, Vol. 25, Issue 4
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A Cryptand Metal-Organic Framework as a Platform for the Selective Uptake and Detection of Group I Metal Cations
journal, January 2017

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Occurrence and characteristics of inorganic ions and microorganisms in potable water from Jamaica
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The role of lysosomes in iron metabolism and recycling
journal, December 2011

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Activity-based sensing fluorescent probes for iron in biological systems
journal, April 2018

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  • DOI: 10.1016/j.cbpa.2017.12.010

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journal, May 2011


Contamination of drinking water resources in the Mekong delta floodplains: Arsenic and other trace metals pose serious health risks to population
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Paramagnetic NMR in solution and the solid state
journal, April 2019

  • Pell, Andrew J.; Pintacuda, Guido; Grey, Clare P.
  • Progress in Nuclear Magnetic Resonance Spectroscopy, Vol. 111
  • DOI: 10.1016/j.pnmrs.2018.05.001

Electro-chemical arsenic remediation: Field trials in West Bengal
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Recognition- and Reactivity-Based Fluorescent Probes for Studying Transition Metal Signaling in Living Systems
journal, July 2015

  • Aron, Allegra T.; Ramos-Torres, Karla M.; Cotruvo, Joseph A.
  • Accounts of Chemical Research, Vol. 48, Issue 8
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Escherichia coli Attenuation by Fe Electrocoagulation in Synthetic Bengal Groundwater: Effect of pH and Natural Organic Matter
journal, July 2015

  • Delaire, Caroline; van Genuchten, Case M.; Nelson, Kara L.
  • Environmental Science & Technology, Vol. 49, Issue 16
  • DOI: 10.1021/acs.est.5b01696

Functionalized Porous Aromatic Framework for Efficient Uranium Adsorption from Aqueous Solutions
journal, March 2017

  • Li, Baiyan; Sun, Qi; Zhang, Yiming
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 14
  • DOI: 10.1021/acsami.7b01711

Extraction of Lanthanide and Actinide Ions from Aqueous Mixtures Using a Carboxylic Acid-Functionalized Porous Aromatic Framework
journal, April 2016


Rapid, Selective Heavy Metal Removal from Water by a Metal–Organic Framework/Polydopamine Composite
journal, March 2018


Porous Aromatic Frameworks as a Platform for Multifunctional Applications
journal, February 2019


NMR Studies of Cathode Materials for Lithium-Ion Rechargeable Batteries
journal, October 2004

  • Grey, Clare P.; Dupré, Nicolas
  • Chemical Reviews, Vol. 104, Issue 10
  • DOI: 10.1021/cr020734p

Living with Iron (and Oxygen): Questions and Answers about Iron Homeostasis
journal, October 2009

  • Theil, Elizabeth C.; Goss, Dixie J.
  • Chemical Reviews, Vol. 109, Issue 10
  • DOI: 10.1021/cr900052g

O-TRENSOX, a New Tripodal Iron Chelator Based on 8-Hydroxyquinoline Subunits:  Thermodynamic and Kinetic Studies
journal, August 1997

  • Serratrice, Guy; Boukhalfa, Hakim; Béguin, Claude
  • Inorganic Chemistry, Vol. 36, Issue 18
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High-field cross polarization NMR from laser-polarized xenon to a polymer surface
journal, September 1993

  • Long, H. W.; Gaede, H. C.; Shore, J.
  • Journal of the American Chemical Society, Vol. 115, Issue 18
  • DOI: 10.1021/ja00071a086

Sulfonate-Grafted Porous Polymer Networks for Preferential CO2 Adsorption at Low Pressure
journal, November 2011

  • Lu, Weigang; Yuan, Daqiang; Sculley, Julian
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