DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Bacteria attenuation by iron electrocoagulation governed by interactions between bacterial phosphate groups and Fe(III) precipitates

Abstract

Iron electrocoagulation (Fe-EC) is a low-cost process in which Fe(II) generated from an Fe(0) anode reacts with dissolved O2 to form (1) Fe(III) precipitates with an affinity for bacterial cell walls and (2) bactericidal reactive oxidants. Previous work suggests that Fe-EC is a promising treatment option for groundwater containing arsenic and bacterial contamination. However, the mechanisms of bacteria attenuation and the impact of major groundwater ions are not well understood. In this work, using the model indicator Escherichia coli (E. coli), we show that physical removal via enmeshment in EC precipitate flocs is the primary process of bacteria attenuation in the presence of HCO3-, which significantly inhibits inactivation, possibly due to a reduction in the lifetime of reactive oxidants. Here, we demonstrate that the adhesion of EC precipitates to cell walls, which results in bacteria encapsulation in flocs, is driven primarily by interactions between EC precipitates and phosphate functional groups on bacteria surfaces. In single solute electrolytes, both P (0.4 mM) and Ca/Mg (1-13 mM) inhibited the adhesion of EC precipitates to bacterial cell walls, whereas Si (0.4 mM) and ionic strength (2-200 mM) did not impact E. coli attenuation. Interestingly, P (0.4 mM) did not affect E. coli attenuationmore » in electrolytes containing Ca/Mg, consistent with bivalent cation bridging between bacterial phosphate groups and inorganic P sorbed to EC precipitates. Finally, we found that EC precipitate adhesion is largely independent of cell wall composition, consistent with comparable densities of phosphate functional groups on Gram-positive and Gram-negative cells. Our results are critical to predict the performance of Fe-EC to eliminate bacterial contaminants from waters with diverse chemical compositions.« less

Authors:
 [1];  [2];  [1];  [3]
  1. Univ. of California, Berkeley, CA (United States)
  2. Univ. of Utrecht (Netherlands)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); United States Agency for International Development (USAID)
OSTI Identifier:
1828154
Alternate Identifier(s):
OSTI ID: 1397363
Grant/Contract Number:  
AC02-05CH11231; AID-OAA-A-13-00002
Resource Type:
Accepted Manuscript
Journal Name:
Water Research
Additional Journal Information:
Journal Volume: 103; Journal ID: ISSN 0043-1354
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; Iron electrocoagulation; Bacteria attenuation; Bacterial surface functional groups; Specific interactions; Bivalent cations; Oxyanions

Citation Formats

Delaire, Caroline, van Genuchten, Case M., Amrose, Susan E., and Gadgil, Ashok J. Bacteria attenuation by iron electrocoagulation governed by interactions between bacterial phosphate groups and Fe(III) precipitates. United States: N. p., 2016. Web. doi:10.1016/j.watres.2016.07.020.
Delaire, Caroline, van Genuchten, Case M., Amrose, Susan E., & Gadgil, Ashok J. Bacteria attenuation by iron electrocoagulation governed by interactions between bacterial phosphate groups and Fe(III) precipitates. United States. https://doi.org/10.1016/j.watres.2016.07.020
Delaire, Caroline, van Genuchten, Case M., Amrose, Susan E., and Gadgil, Ashok J. Mon . "Bacteria attenuation by iron electrocoagulation governed by interactions between bacterial phosphate groups and Fe(III) precipitates". United States. https://doi.org/10.1016/j.watres.2016.07.020. https://www.osti.gov/servlets/purl/1828154.
@article{osti_1828154,
title = {Bacteria attenuation by iron electrocoagulation governed by interactions between bacterial phosphate groups and Fe(III) precipitates},
author = {Delaire, Caroline and van Genuchten, Case M. and Amrose, Susan E. and Gadgil, Ashok J.},
abstractNote = {Iron electrocoagulation (Fe-EC) is a low-cost process in which Fe(II) generated from an Fe(0) anode reacts with dissolved O2 to form (1) Fe(III) precipitates with an affinity for bacterial cell walls and (2) bactericidal reactive oxidants. Previous work suggests that Fe-EC is a promising treatment option for groundwater containing arsenic and bacterial contamination. However, the mechanisms of bacteria attenuation and the impact of major groundwater ions are not well understood. In this work, using the model indicator Escherichia coli (E. coli), we show that physical removal via enmeshment in EC precipitate flocs is the primary process of bacteria attenuation in the presence of HCO3-, which significantly inhibits inactivation, possibly due to a reduction in the lifetime of reactive oxidants. Here, we demonstrate that the adhesion of EC precipitates to cell walls, which results in bacteria encapsulation in flocs, is driven primarily by interactions between EC precipitates and phosphate functional groups on bacteria surfaces. In single solute electrolytes, both P (0.4 mM) and Ca/Mg (1-13 mM) inhibited the adhesion of EC precipitates to bacterial cell walls, whereas Si (0.4 mM) and ionic strength (2-200 mM) did not impact E. coli attenuation. Interestingly, P (0.4 mM) did not affect E. coli attenuation in electrolytes containing Ca/Mg, consistent with bivalent cation bridging between bacterial phosphate groups and inorganic P sorbed to EC precipitates. Finally, we found that EC precipitate adhesion is largely independent of cell wall composition, consistent with comparable densities of phosphate functional groups on Gram-positive and Gram-negative cells. Our results are critical to predict the performance of Fe-EC to eliminate bacterial contaminants from waters with diverse chemical compositions.},
doi = {10.1016/j.watres.2016.07.020},
journal = {Water Research},
number = ,
volume = 103,
place = {United States},
year = {Mon Jul 11 00:00:00 EDT 2016},
month = {Mon Jul 11 00:00:00 EDT 2016}
}

Journal Article:

Citation Metrics:
Cited by: 31 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Iron-Catalyzed Oxidation of Arsenic(III) by Oxygen and by Hydrogen Peroxide:  pH-Dependent Formation of Oxidants in the Fenton Reaction
journal, June 2003

  • Hug, Stephan J.; Leupin, Olivier
  • Environmental Science & Technology, Vol. 37, Issue 12
  • DOI: 10.1021/es026208x

Iron oxyhydroxide mineralization on microbial extracellular polysaccharides
journal, July 2009

  • Chan, Clara S.; Fakra, Sirine C.; Edwards, David C.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 13
  • DOI: 10.1016/j.gca.2009.02.036

Effect of phosphate, silicate, and Ca on Fe(III)-precipitates formed in aerated Fe(II)- and As(III)-containing water studied by X-ray absorption spectroscopy
journal, January 2010

  • Voegelin, Andreas; Kaegi, Ralf; Frommer, Jakob
  • Geochimica et Cosmochimica Acta, Vol. 74, Issue 1
  • DOI: 10.1016/j.gca.2009.09.020

Multi-competitive interaction of As(III) and As(V) oxyanions with Ca2+, Mg2+, PO3−4, and CO2−3 ions on goethite
journal, April 2008

  • Stachowicz, Monika; Hiemstra, Tjisse; van Riemsdijk, Willem H.
  • Journal of Colloid and Interface Science, Vol. 320, Issue 2
  • DOI: 10.1016/j.jcis.2008.01.007

ATR–FTIR Spectroscopic Investigation on Phosphate Adsorption Mechanisms at the Ferrihydrite–Water Interface
journal, September 2001

  • Arai, Yuji; Sparks, D. L.
  • Journal of Colloid and Interface Science, Vol. 241, Issue 2
  • DOI: 10.1006/jcis.2001.7773

ATR-FTIR Spectroscopy Study of the Influence of pH and Contact Time on the Adhesion of Shewanella putrefaciens Bacterial Cells to the Surface of Hematite
journal, November 2012

  • Elzinga, Evert J.; Huang, Jen-How; Chorover, Jon
  • Environmental Science & Technology, Vol. 46, Issue 23
  • DOI: 10.1021/es303318y

Adsorption of phenol and substituted phenols by iron oxides
journal, April 1991

  • McBride, M. B.; Kung, King-Hsi
  • Environmental Toxicology and Chemistry, Vol. 10, Issue 4
  • DOI: 10.1002/etc.5620100403

ATR-FTIR Spectroscopy Reveals Bond Formation During Bacterial Adhesion to Iron Oxide
journal, September 2006

  • Parikh, Sanjai J.; Chorover, Jon
  • Langmuir, Vol. 22, Issue 20
  • DOI: 10.1021/la061359p

Adhesion of Bacterial Exopolymers to α-FeOOH:  Inner-Sphere Complexation of Phosphodiester Groups
journal, November 2004

  • Omoike, Anselm; Chorover, Jon; Kwon, Kideok D.
  • Langmuir, Vol. 20, Issue 25
  • DOI: 10.1021/la048597+

Inactivation of Escherichia coli by Nanoparticulate Zerovalent Iron and Ferrous Ion
journal, September 2010

  • Kim, Jee Yeon; Park, Hee-Jin; Lee, Changha
  • Applied and Environmental Microbiology, Vol. 76, Issue 22
  • DOI: 10.1128/AEM.01009-10

Role of Cell Surface Lipopolysaccharides in Escherichia c oli K12 Adhesion and Transport
journal, August 2004

  • Walker, Sharon L.; Redman, Jeremy A.; Elimelech, Menachem
  • Langmuir, Vol. 20, Issue 18
  • DOI: 10.1021/la049511f

Adhesion of Shewanella oneidensis MR-1 to Goethite: A Two-Dimensional Correlation Spectroscopic Study
journal, April 2016

  • Yan, Wei; Wang, Hongbo; Jing, Chuanyong
  • Environmental Science & Technology, Vol. 50, Issue 8
  • DOI: 10.1021/acs.est.6b00066

ATR–FTIR spectroscopic evidence for biomolecular phosphorus and carboxyl groups facilitating bacterial adhesion to iron oxides
journal, July 2014


Hydrogen peroxide for prevention of bacterial growth on polymer biomaterials
journal, December 1999


Fecal Indicator Bacteria Transport and Deposition in Saturated and Unsaturated Porous Media
journal, July 2012

  • Chen, Gexin; Walker, Sharon L.
  • Environmental Science & Technology, Vol. 46, Issue 16
  • DOI: 10.1021/es301378q

Composition and structure of Fe(III)-precipitates formed by Fe(II) oxidation in water at near-neutral pH: Interdependent effects of phosphate, silicate and Ca
journal, August 2015


Fe(III) Nucleation in the Presence of Bivalent Cations and Oxyanions Leads to Subnanoscale 7 Å Polymers
journal, October 2014

  • van Genuchten, Case M.; Gadgil, Ashok J.; Peña, Jasquelin
  • Environmental Science & Technology, Vol. 48, Issue 20
  • DOI: 10.1021/es503281a

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

Adsorption of alpha amino acids at the water/goethite interface
journal, March 2008

  • Norén, Katarina; Loring, John S.; Persson, Per
  • Journal of Colloid and Interface Science, Vol. 319, Issue 2
  • DOI: 10.1016/j.jcis.2007.11.046

Spectroscopic characterization of the structural and functional properties of natural organic matter fractions
journal, July 2002


Rate Constants for Reactions of Inorganic Radicals in Aqueous Solution
journal, July 1988

  • Neta, P.; Huie, Robert E.; Ross, Alberta B.
  • Journal of Physical and Chemical Reference Data, Vol. 17, Issue 3
  • DOI: 10.1063/1.555808

Structure of the O antigen of Escherichia coli K-12 and the sequence of its rfb gene cluster
journal, July 1994


Removing Arsenic from Synthetic Groundwater with Iron Electrocoagulation: An Fe and As K-Edge EXAFS Study
journal, December 2011

  • van Genuchten, Case M.; Addy, Susan E. A.; Peña, Jasquelin
  • Environmental Science & Technology, Vol. 46, Issue 2
  • DOI: 10.1021/es201913a

A combined electrochemical-irradiation treatment of highly colored and polluted industrial wastewater
journal, July 2003


Lipopolysaccharide Density and Structure Govern the Extent and Distance of Nanoparticle Interaction with Actual and Model Bacterial Outer Membranes
journal, August 2015

  • Jacobson, Kurt H.; Gunsolus, Ian L.; Kuech, Thomas R.
  • Environmental Science & Technology, Vol. 49, Issue 17
  • DOI: 10.1021/acs.est.5b01841

Analysis of Bacterial Deposition on Metal (Hydr)oxide-Coated Sand Filter Media
journal, July 1998

  • Truesdail, S. E.; Lukasik, J.; Farrah, S. R.
  • Journal of Colloid and Interface Science, Vol. 203, Issue 2
  • DOI: 10.1006/jcis.1998.5541

Proton and metal adsorption onto bacterial consortia: Stability constants for metal–bacterial surface complexes
journal, April 2007


The carbonate radical and related oxidants derived from bicarbonate buffer
journal, January 2007


Virulence and Immunogenic Activities of B. Typhosus in Relation to its Antigenic Constituents
journal, August 1935


The future for electrocoagulation as a localised water treatment technology
journal, April 2005


Modeling As(III) Oxidation and Removal with Iron Electrocoagulation in Groundwater
journal, October 2012

  • Li, Lei; van Genuchten, Case M.; Addy, Susan E. A.
  • Environmental Science & Technology, Vol. 46, Issue 21
  • DOI: 10.1021/es302456b

Influence of Phosphate on Bacterial Adhesion onto Iron Oxyhydroxide in Drinking Water
journal, February 2002

  • Appenzeller, Brice M. R.; Duval, Yann B.; Thomas, Fabien
  • Environmental Science & Technology, Vol. 36, Issue 4
  • DOI: 10.1021/es010155m

Mechanisms of virus control during iron electrocoagulation – Microfiltration of surface water
journal, May 2012


Structure of Fe(III) precipitates generated by the electrolytic dissolution of Fe(0) in the presence of groundwater ions
journal, February 2014

  • van Genuchten, Case M.; Peña, Jasquelin; Amrose, Susan E.
  • Geochimica et Cosmochimica Acta, Vol. 127
  • DOI: 10.1016/j.gca.2013.11.044

Application of electrocoagulation in Escherichia coli culture and two surface waters
journal, January 2008


Reactions of the ferryl ion with some compounds found in cloud water
journal, January 1998


Chemical Force Spectroscopy Evidence Supporting the Layer-by-Layer Model of Organic Matter Binding to Iron (oxy)Hydroxide Mineral Surfaces
journal, August 2015

  • Chassé, Alexander W.; Ohno, Tsutomu; Higgins, Steven R.
  • Environmental Science & Technology, Vol. 49, Issue 16
  • DOI: 10.1021/acs.est.5b01877

Arsenic Removal with Iron(II) and Iron(III) in Waters with High Silicate and Phosphate Concentrations
journal, January 2004

  • Roberts, Linda C.; Hug, Stephan J.; Ruettimann, Thomas
  • Environmental Science & Technology, Vol. 38, Issue 1
  • DOI: 10.1021/es0343205

Engineering Solutions to Improve the Removal of Fecal Indicator Bacteria by Bioinfiltration Systems during Intermittent Flow of Stormwater
journal, June 2013

  • Mohanty, Sanjay K.; Torkelson, Andrew A.; Dodd, Hanna
  • Environmental Science & Technology, Vol. 47, Issue 19
  • DOI: 10.1021/es305136b

Factors Affecting the Yield of Oxidants from the Reaction of Nanoparticulate Zero-Valent Iron and Oxygen
journal, February 2008

  • Keenan, Christina R.; Sedlak, David L.
  • Environmental Science & Technology, Vol. 42, Issue 4
  • DOI: 10.1021/es7025664

Comparison of the acid-base behaviour and metal adsorption characteristics of a gram-negative bacterium with other strains
journal, April 2003


Electro-chemical arsenic remediation: Field trials in West Bengal
journal, August 2014


Arsenic removal in synthetic ground water using iron electrolysis
journal, February 2014


Works referencing / citing this record:

Bacterial bioreporter detection of arsenic associated with iron oxides
journal, January 2018

  • van Genuchten, Case M.; Finger, Amanda; van der Meer, Jan R.
  • Environmental Science: Processes & Impacts, Vol. 20, Issue 6
  • DOI: 10.1039/c8em00071a

Electrocoagulation as a Pretreatment for Electroxidation of E. coli
journal, November 2019

  • Lynn, William; Heffron, Joe; Mayer, Brooke K.
  • Water, Vol. 11, Issue 12
  • DOI: 10.3390/w11122509

Electrodisinfection of real swine wastewater for water reuse
journal, July 2018

  • Simas, Angélica; Mores, Rúbia; Steffens, Juliana
  • Environmental Chemistry Letters, Vol. 17, Issue 1
  • DOI: 10.1007/s10311-018-0782-z