Escherichia coli Attenuation by Fe Electrocoagulation in Synthetic Bengal Groundwater: Effect of pH and Natural Organic Matter

Delaire, Caroline; van Genuchten, Case M.; Nelson, Kara L.; Amrose, Susan E.; Gadgil, Ashok J.

doi:10.1021/acs.est.5b01696

Title: Escherichia coli Attenuation by Fe Electrocoagulation in Synthetic Bengal Groundwater: Effect of pH and Natural Organic Matter

Journal Article · Tue Jul 14 00:00:00 EDT 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.5b01696· OSTI ID:1819440

Delaire, Caroline ^[1]; van Genuchten, Case M. ^[2]; Nelson, Kara L. ^[1]; Amrose, Susan E. ^[1]; Gadgil, Ashok J. ^[3]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Univ. of Lausanne (Switzerland)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Technologies addressing both arsenic and microbial contamination of Bengal groundwater are needed. Fe electrocoagulation (Fe-EC), a simple process relying on the dissolution of an Fe(0) anode to produce Fe(III) precipitates, has been shown to efficiently remove arsenic from groundwater at low cost. In this work, we investigated Escherichia coli (E. coli) attenuation by Fe-EC in synthetic Bengal groundwater as a function of Fe dosage rate, total Fe dosed, pH, and presence of natural organic matter (NOM). A 2.5 mM Fe dosage simultaneously achieved over 4-log E. coli attenuation and arsenic removal from 450 to below 10 μg/L. E. coli reduction was significantly enhanced at pH 6.6 compared to pH 7.5, which we linked to the decreased rate of Fe(II) oxidation at lower pH. 3 mg/L-C of NOM (Suwanee River fulvic acid) did not significantly affect E. coli attenuation. Live-dead staining and comparisons of Fe-EC with chemical coagulation controls showed that the primary mechanism of E. coli attenuation is physical removal with Fe(III) precipitates, with inactivation likely contributing as well at lower pH. Transmission electron microscopy showed that EC precipitates adhere to and bridge individual E. coli cells, resulting in large bacteria-Fe aggregates that can be removed by gravitational settling. Our results point to the promising ability of Fe-EC to treat arsenic and bacterial contamination simultaneously at low cost.

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Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USAID

Grant/Contract Number:: AC02-05CH11231; AID-OAA-A-13-00002

OSTI ID:: 1819440

Journal Information:: Environmental Science and Technology, Vol. 49, Issue 16; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (58)

Comparison of fecal indicators with pathogenic bacteria and rotavirus in groundwater Ferguson, Andrew S.; Layton, Alice C.; Mailloux, Brian J. Science of The Total Environment, Vol. 431 https://doi.org/10.1016/j.scitotenv.2012.05.060	journal	August 2012
Interactions between viruses and goethite during saturated flow: Effects of solution pH, carbonate, and phosphate Zhuang, Jie; Jin, Yan Journal of Contaminant Hydrology, Vol. 98, Issue 1-2 https://doi.org/10.1016/j.jconhyd.2008.02.002	journal	May 2008
Contrasting Influence of Geology on E. coli and Arsenic in Aquifers of Bangladesh Leber, Jessica; Rahman, M. Moshiur; Ahmed, Kazi M. Ground Water, Vol. 49, Issue 1 https://doi.org/10.1111/j.1745-6584.2010.00689.x	journal	December 2010
Virus removal by iron coagulation–microfiltration Zhu, Bintuan; Clifford, Dennis A.; Chellam, Shankar Water Research, Vol. 39, Issue 20 https://doi.org/10.1016/j.watres.2005.09.035	journal	December 2005
Comparison of electrocoagulation and chemical coagulation pretreatment for enhanced virus removal using microfiltration membranes Zhu, Bintuan; Clifford, Dennis A.; Chellam, Shankararaman Water Research, Vol. 39, Issue 13 https://doi.org/10.1016/j.watres.2005.05.020	journal	August 2005
Influence of organic matter on the transport of Cryptosporidium parvum oocysts in a ferric oxyhydroxide-coated quartz sand saturated porous medium Abudalo, R. A.; Ryan, J. N.; Harvey, R. W. Water Research, Vol. 44, Issue 4 https://doi.org/10.1016/j.watres.2009.09.039	journal	February 2010
Competitive adsorption of metal cations onto two gram positive bacteria: testing the chemical equilibrium model Fowle, David A.; Fein, Jeremy B. Geochimica et Cosmochimica Acta, Vol. 63, Issue 19-20 https://doi.org/10.1016/S0016-7037(99)00233-1	journal	October 1999
ATR-FTIR Spectroscopy Reveals Bond Formation During Bacterial Adhesion to Iron Oxide Parikh, Sanjai J.; Chorover, Jon Langmuir, Vol. 22, Issue 20 https://doi.org/10.1021/la061359p	journal	September 2006
Water Health Status in Lower Reaches of River Ganga, India Sengupta, Chitralekha; Sukumaran, Dipu; Barui, Dipanjali Applied Ecology and Environmental Sciences, Vol. 2, Issue 1 https://doi.org/10.12691/aees-2-1-3	journal	January 2014
Effects of water chemistry on arsenic removal from drinking water by electrocoagulation Wan, Wei; Pepping, Troy J.; Banerji, Tuhin Water Research, Vol. 45, Issue 1 https://doi.org/10.1016/j.watres.2010.08.016	journal	January 2011
Inactivation of Escherichia coli by Nanoparticulate Zerovalent Iron and Ferrous Ion Kim, Jee Yeon; Park, Hee-Jin; Lee, Changha Applied and Environmental Microbiology, Vol. 76, Issue 22 https://doi.org/10.1128/AEM.01009-10	journal	September 2010
Role of Cell Surface Lipopolysaccharides in Escherichia c oli K12 Adhesion and Transport Walker, Sharon L.; Redman, Jeremy A.; Elimelech, Menachem Langmuir, Vol. 20, Issue 18 https://doi.org/10.1021/la049511f	journal	August 2004
Characteristics and role of groundwater dissolved organic matter on arsenic mobilization and poisoning in Bangladesh Tareq, Shafi M.; Maruo, Masahiro; Ohta, Keiichi Physics and Chemistry of the Earth, Parts A/B/C, Vol. 58-60 https://doi.org/10.1016/j.pce.2013.04.014	journal	January 2013
Relative Insignificance of Virus Inactivation during Aluminum Electrocoagulation of Saline Waters Tanneru, Charan Tej; N., Jothikumar; Hill, Vincent R. Environmental Science & Technology, Vol. 48, Issue 24 https://doi.org/10.1021/es504381f	journal	November 2014
Precipitation of iron, silica, and sulfate on bacterial cell surfaces Fortin, D.; Ferris, F. G. Geomicrobiology Journal, Vol. 15, Issue 4 https://doi.org/10.1080/01490459809378085	journal	October 1998
Influence of Latrine Proximity and Type on Tubewell Water Quality and Diarrheal Disease in Bangladesh Escamilla, Veronica; Knappett, Peter S. K.; Yunus, Mohammad Annals of the Association of American Geographers, Vol. 103, Issue 2 https://doi.org/10.1080/00045608.2013.756257	journal	March 2013
Arsenic removal from groundwater using iron electrocoagulation: Effect of charge dosage rate Amrose, Susan; Gadgil, Ashok; Srinivasan, Venkat Journal of Environmental Science and Health, Part A, Vol. 48, Issue 9 https://doi.org/10.1080/10934529.2013.773215	journal	July 2013
Killing of microorganisms by pulsed electric fields Grahl, T.; Märkl, H. Applied Microbiology and Biotechnology, Vol. 45, Issue 1-2 https://doi.org/10.1007/s002530050663	journal	March 1996
Natural organic matter removal and enhanced coagulation as a link between coagulation and electrocoagulation Ghernaout, Djamel; Ghernaout, Badiaa; Kellil, Amara Desalination and Water Treatment, Vol. 2, Issue 1-3 https://doi.org/10.5004/dwt.2009.116	journal	February 2009
Tubewell water quality and predictors of contamination in three flood-prone areas in Bangladesh Luby, S. P.; Gupta, S. K.; Sheikh, M. A. Journal of Applied Microbiology, Vol. 105, Issue 4 https://doi.org/10.1111/j.1365-2672.2008.03826.x	journal	October 2008
Iron-silica crystallite nucleation by bacteria in a geothermal sediment Ferris, F. G.; Beveridge, T. J.; Fyfe, W. S. Nature, Vol. 320, Issue 6063 https://doi.org/10.1038/320609a0	journal	April 1986
Fe(III) Nucleation in the Presence of Bivalent Cations and Oxyanions Leads to Subnanoscale 7 Å Polymers van Genuchten, Case M.; Gadgil, Ashok J.; Peña, Jasquelin Environmental Science & Technology, Vol. 48, Issue 20 https://doi.org/10.1021/es503281a	journal	October 2014
Production and Transformation of Mixed-Valent Nanoparticles Generated by Fe(0) Electrocoagulation Dubrawski, Kristian L.; van Genuchten, Case M.; Delaire, Caroline Environmental Science & Technology, Vol. 49, Issue 4 https://doi.org/10.1021/es505059d	journal	February 2015
The isoelectric point of bacteria as an indicator for the presence of cell surface polymers that inhibit adhesion Rijnaarts, Huub H. M.; Norde, Willem; Lyklema, Johannes Colloids and Surfaces B: Biointerfaces, Vol. 4, Issue 4 https://doi.org/10.1016/0927-7765(94)01164-Z	journal	May 1995
Unsealed tubewells lead to increased fecal contamination of drinking water Knappett, Peter S. K.; McKay, Larry D.; Layton, Alice Journal of Water and Health, Vol. 10, Issue 4 https://doi.org/10.2166/wh.2012.102	journal	October 2012
Inactivation of Escherichia coli O157:H7 by the Combination of Organic Acids and Pulsed Electric Field Liu, Xia; Yousef, Ahmed E.; Chism, Grady W. Journal of Food Safety, Vol. 16, Issue 4 https://doi.org/10.1111/j.1745-4565.1997.tb00169.x	journal	April 1997
Sweep Flocculation and Adsorption of Viruses on Aluminum Flocs during Electrochemical Treatment Prior to Surface Water Microfiltration Tanneru, Charan Tej; Rimer, Jeffrey D.; Chellam, Shankararaman Environmental Science & Technology, Vol. 47, Issue 9 https://doi.org/10.1021/es400291e	journal	April 2013
Increase in Diarrheal Disease Associated with Arsenic Mitigation in Bangladesh Wu, Jianyong; van Geen, Alexander; Ahmed, Kazi Matin PLoS ONE, Vol. 6, Issue 12 https://doi.org/10.1371/journal.pone.0029593	journal	December 2011
The Capture and Destruction of Escherichia coli from Simulated Urban Runoff Using Conventional Bioretention Media and Iron Oxide-coated Sand Zhang, Lan; Seagren, Eric A.; Davis, Allen P. Water Environment Research, Vol. 82, Issue 8 https://doi.org/10.2175/106143010X12609736966441	journal	August 2010
Adsorbed Polymer and NOM Limits Adhesion and Toxicity of Nano Scale Zerovalent Iron to E. coli Li, Zhiqiang; Greden, Karl; Alvarez, Pedro J. J. Environmental Science & Technology, Vol. 44, Issue 9 https://doi.org/10.1021/es9031198	journal	May 2010
Fecal Contamination of Shallow Tubewells in Bangladesh Inversely Related to Arsenic van Geen, Alexander; Ahmed, Kazi Matin; Akita, Yasuyuki Environmental Science & Technology, Vol. 45, Issue 4 https://doi.org/10.1021/es103192b	journal	February 2011
Removing Arsenic from Synthetic Groundwater with Iron Electrocoagulation: An Fe and As K-Edge EXAFS Study van Genuchten, Case M.; Addy, Susan E. A.; Peña, Jasquelin Environmental Science & Technology, Vol. 46, Issue 2 https://doi.org/10.1021/es201913a	journal	December 2011
Adsorption of Humic Acid onto Nanoscale Zerovalent Iron and Its Effect on Arsenic Removal Giasuddin, Abul B. M.; Kanel, Sushil R.; Choi, Heechul Environmental Science & Technology, Vol. 41, Issue 6 https://doi.org/10.1021/es0616534	journal	March 2007
Sorption of humic acid on Fe oxides, bacteria, and Fe oxide-bacteria composites Jiang, Li; Zhu, Jun; Wang, Hui Journal of Soils and Sediments, Vol. 14, Issue 8 https://doi.org/10.1007/s11368-014-0897-1	journal	April 2014
Ferrous and Ferric Ion Generation During Iron Electrocoagulation Lakshmanan, Divagar; Clifford, Dennis A.; Samanta, Gautam Environmental Science & Technology, Vol. 43, Issue 10 https://doi.org/10.1021/es8036669	journal	April 2009
Use of fluorescent probes to assess physiological functions of bacteriaat single-cell level Joux, Fabien; Lebaron, Philippe Microbes and Infection, Vol. 2, Issue 12 https://doi.org/10.1016/S1286-4579(00)01307-1	journal	October 2000
Role of Carbonate Speciation on the Oxidation Rate of Fe(II) in Aquatic Systems King, D. Whitney Environmental Science & Technology, Vol. 32, Issue 19 https://doi.org/10.1021/es980206o	journal	October 1998
Measuring the mass, density, and size of particles and cells using a suspended microchannel resonator Godin, Michel; Bryan, Andrea K.; Burg, Thomas P. Applied Physics Letters, Vol. 91, Issue 12 https://doi.org/10.1063/1.2789694	journal	September 2007
Effect of high-voltage electric pulses on yeast cells: factors influencing the killing efficiency Gášková, D.; Sigler, K.; Janderová, B. Bioelectrochemistry and Bioenergetics, Vol. 39, Issue 2 https://doi.org/10.1016/0302-4598(95)01892-1	journal	March 1996
Modeling As(III) Oxidation and Removal with Iron Electrocoagulation in Groundwater Li, Lei; van Genuchten, Case M.; Addy, Susan E. A. Environmental Science & Technology, Vol. 46, Issue 21 https://doi.org/10.1021/es302456b	journal	October 2012
Ionic Strength Effects on Silicic Acid (H ₄ SiO ₄ ) Sorption and Oligomerization on an Iron Oxide Surface: An Interesting Interplay between Electrostatic and Chemical Forces Dol Hamid, Rossuriati; Swedlund, Peter J.; Song, Yantao Langmuir, Vol. 27, Issue 21 https://doi.org/10.1021/la201775c	journal	October 2011
Mechanisms of virus control during iron electrocoagulation – Microfiltration of surface water Tanneru, Charan Tej; Chellam, Shankararaman Water Research, Vol. 46, Issue 7 https://doi.org/10.1016/j.watres.2012.01.032	journal	May 2012
Influence of Phosphate on Bacterial Adhesion onto Iron Oxyhydroxide in Drinking Water Appenzeller, Brice M. R.; Duval, Yann B.; Thomas, Fabien Environmental Science & Technology, Vol. 36, Issue 4 https://doi.org/10.1021/es010155m	journal	February 2002
Structure of Fe(III) precipitates generated by the electrolytic dissolution of Fe(0) in the presence of groundwater ions van Genuchten, Case M.; Peña, Jasquelin; Amrose, Susan E. Geochimica et Cosmochimica Acta, Vol. 127 https://doi.org/10.1016/j.gca.2013.11.044	journal	February 2014
Inactivation of MS2 Coliphage by Ferrous Ion and Zero-Valent Iron Nanoparticles Kim, Jee Yeon; Lee, Changha; Love, David C. Environmental Science & Technology, Vol. 45, Issue 16 https://doi.org/10.1021/es201345y	journal	July 2011
Arsenic concentrations and bacterial contamination in a pilot shallow dugwell program in West Bengal, India Hira-Smith, Meera M.; Yuan, Yan; Savarimuthu, Xavier Journal of Environmental Science and Health, Part A, Vol. 42, Issue 1 https://doi.org/10.1080/10934520601015834	journal	May 2007
Application of electrocoagulation in Escherichia coli culture and two surface waters Ghernaout, D.; Badis, A.; Kellil, A. Desalination, Vol. 219, Issue 1-3 https://doi.org/10.1016/j.desal.2007.05.010	journal	January 2008
Enhanced coagulation: Us requirements and a broader view Edzwald, James K.; Tobiason, John E. Water Science and Technology, Vol. 40, Issue 9 https://doi.org/10.1016/S0273-1223(99)00641-1	journal	January 1999
Microbiological Analysis of Tube-Well Water in a Rural Area of Bangladesh Islam, M. S.; Siddika, A.; Khan, M. N. H. Applied and Environmental Microbiology, Vol. 67, Issue 7 https://doi.org/10.1128/AEM.67.7.3328-3330.2001	journal	July 2001
Arsenic contamination in groundwater in the Southeast Asia region Rahman, Mohammad Mahmudur; Naidu, R.; Bhattacharya, Prosun Environmental Geochemistry and Health, Vol. 31, Issue S1 https://doi.org/10.1007/s10653-008-9233-2	journal	January 2009
First Direct Imaging of Electrolyte-Induced Deswelling Behavior of pH-Responsive Microgels in Aqueous Media Using Scanning Transmission X-ray Microscopy Fujii, Syuji; Dupin, Damien; Araki, Tohru Langmuir, Vol. 25, Issue 5 https://doi.org/10.1021/la804212y	journal	March 2009
Metal deposits associated with bacteria: implications for Fe and Mn marine biogeochemistry Cowen, James P.; Bruland, Kenneth W. Deep Sea Research Part A. Oceanographic Research Papers, Vol. 32, Issue 3 https://doi.org/10.1016/0198-0149(85)90078-0	journal	March 1985
Arsenic Removal with Iron(II) and Iron(III) in Waters with High Silicate and Phosphate Concentrations Roberts, Linda C.; Hug, Stephan J.; Ruettimann, Thomas Environmental Science & Technology, Vol. 38, Issue 1 https://doi.org/10.1021/es0343205	journal	January 2004
Engineering Solutions to Improve the Removal of Fecal Indicator Bacteria by Bioinfiltration Systems during Intermittent Flow of Stormwater Mohanty, Sanjay K.; Torkelson, Andrew A.; Dodd, Hanna Environmental Science & Technology, Vol. 47, Issue 19 https://doi.org/10.1021/es305136b	journal	June 2013
Adsorption and desorption of natural organic matter on iron oxide: mechanisms and models Gu, Baohua.; Schmitt, Juergen.; Chen, Zhihong. Environmental Science & Technology, Vol. 28, Issue 1 https://doi.org/10.1021/es00050a007	journal	January 1994
The pH-Dependent Surface Charging and the Points of Zero Charge Kosmulski, Marek Journal of Colloid and Interface Science, Vol. 253, Issue 1 https://doi.org/10.1006/jcis.2002.8490	journal	September 2002
Electro-chemical arsenic remediation: Field trials in West Bengal Amrose, Susan E.; Bandaru, Siva R. S.; Delaire, Caroline Science of The Total Environment, Vol. 488-489 https://doi.org/10.1016/j.scitotenv.2013.11.074	journal	August 2014
Arsenic removal in synthetic ground water using iron electrolysis Li, Lei; Li, Jun; Shao, Chen Separation and Purification Technology, Vol. 122 https://doi.org/10.1016/j.seppur.2013.11.012	journal	February 2014

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