Concurrent arsenic and microbe removal from groundwater using iron electro-coagulation: Mechanisms of E.coli attenuation

Around 60 million people in South Asia drink groundwater from arsenic contaminated shallow aquifers. Research over the last two decades has focused on arsenic removal alone to mitigate this problem, largely ignoring possible microbial contamination of shallow groundwater. However, diarrheal diseases are still prevalent in the region and recently, fecal indicators and pathogens were detected in shallow tubewells in Bangladesh. Comprehensive treatment technologies addressing both microbial and arsenic contamination are needed and may have a higher social acceptability, contributing to their sustainability in resource poor areas. Iron electro-coagulation (EC) is a low-cost and low-waste process using small amounts of electricity to produce Fe(III)-oxides that serve as an adsorbent for arsenic and a coagulant for microbes. Iron EC relies on the oxidative dissolution of a Fe(0) anode to produce Fe(II) ions that rapidly oxidize and precipitate in the presence of oxygen. In the process, strong oxidants generated by Fenton-like reactions convert As(III) into As(V), which is more amenable to adsorption. In this work, we demonstrate that iron EC can simultaneously remove arsenic and the model organism E.coli in South Asian synthetic groundwater. We find that E.coli is attenuated because it adheres to iron precipitates and is trapped in aggregates that settle out. Some inactivation (~20%, as probed by membrane permeability stains) also takes place, likely due to oxidative stress caused by strong oxidants produced in Fenton-like reactions. We find that pH has a significant effect on E.coli removal from South Asian synthetic groundwater. The iron dosages required to achieve 4-log attenuation (from an initial concentration of 10^6.4 CFU/mL) at pH 6.6. and 7.5 are 25 and 140 mg-Fe/L respectively, other parameters being equal. In this pH range, iron precipitates generated in synthetic groundwater have a negative surface charge, whose variation cannot entirely explain the sensitivity of bacterial attenuation to pH. We propose an alternative explanation involving Fe(II) oxidation rate. We use TEM and ATR-FTIR spectroscopy to investigate how E.coli binds to EC-precipitates. TEM enables identifying where iron particles are located with respect to the cell surface (e.g. in EPS at a distance from the cell, on the cell surface, or inside the periplasm). Analysis of ATR-FTIR spectra in the mid-IR region (800 to 1700 cm-1) allows detection of possible covalent bonds between carboxyl or phosphate residues on the cell wall and EC-precipitates. We build on these results to discuss the strength and robustness of attachment.