Long-term consumption of groundwater containing elevated levels of arsenic (As) can have severe health consequences, including cancer. To effectively remove As, conventional treatment technologies require expensive chemical oxidants to oxidise neutral arsenite (As(III)) in groundwater to negatively charged arsenate (As(V)), which is more easily removed. Rapid sand filter beds used in conventional aeration-filtration to treat anaerobic groundwater can naturally oxidise As(III) through biological processes but require an additional step to remove the generated As(V), adding complexity and cost. This study introduces a novel approach where As(V), produced through biological As(III) oxidation in a sand filter, is effectively removed within the same filter by embedding and operating an iron electrocoagulation (FeEC) system inside the filter. Operating FeEC within the biological filter achieved higher As(III) removal (81 %) compared to operating FeEC in the filter supernatant (67 %). This performance was similar to an analogous embedded-FeEC system treating As(V)-contaminated water (85 %), confirming the benefits of incorporating FeEC in a biological bed for comparable As(III) and As(V) removal. However, operating FeEC in the sand matrix consumed more energy (14 Wh/m³) compared to FeEC operated in a water matrix (7 Wh/m³). The efficiency of As removal increased and energy requirements decreased in such embedded-FeEC systems by deep-bed infiltration of Fe(III)-precipitates, which can be controlled by adjusting flow rate and pH. This study is one of the first to demonstrate the feasibility of embedding FeEC systems in sand filters for groundwater arsenic removal. Such systems capitalise on biological As(III) oxidation in aeration-filtration, effectively eliminating As(V) within the same setup without the need for chemicals or major modifications.

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In the top layer of aerated rapid sand filtration systems, uncharged As(III) is biologically converted to charged As(V). Subsequently, the main removal mechanism for As(V) is adsorption onto oxidised, flocculated Fe(III) (hydrous ferric hydroxides; HFO). The aim of this research was to understand the interactions between As and Fe in biologically active rapid filter columns and investigate the effect of different operational modes on Fe removal to subsequently promote As removal. For this purpose, different filter media column experiments were performed using natural, aerated groundwater containing 3.4 μg/l As(III). Results show that independent of the filter media size, complete (biological) conversion of As(III), manganese, ammonium and nitrite was achieved in approximately 70 days. After ripening, enhanced As removal was achieved with a top layer of coarse media or by dosing additional Fe(III). Addition of Fe(II) did not have the same effect on As removal, potentially due to heterogeneous Fe(II) oxidation in the upper layer of the filter, attaching rapidly to the filter grain surface and thereby preventing HFO flocs to penetrate deeper into the bed. Increasing the flow rate from 1 to 4 m/h did not improve As removal and lowering the pH from 8 to 7.4, resulted in an 55% increased removal of dissolved As. Altogether it is concluded that As removal in biologically active rapid sand filters can be improved by applying coarser filter media on top, in combination with dosing Fe(III) and/or pH correction.

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The objective of this study was to investigate whether arsenic-oxidising bacteria (AsOB) will grow and survive in rapid sand filters. Additionally, the interdependence of other groundwater constituents (Fe(II), Mn(II), NH₄) with biological As(III) oxidation was investigated. For this purpose As(III) oxidation was monitored in pilot-scale filter sand columns fed with raw groundwater, as well as treated groundwater (drinking water) with spikes of either As(III), Mn(II) or NH₄. It was concluded that biological As(III) oxidation rapidly developed in the rapid sand filter columns. With a typical lag and log phase, decreasing As(III) and increasing As(V) concentrations in the effluent of the sand columns were observed in a timeframe of weeks. The growth of biomass in the sand columns was confirmed with ATP analysis. ATP concentrations on the sand grains increased from 0.7 ng/g to 16, 8 and 2 ng/g filter sand stratified from the top of the sand filter to the bottom, respectively. Additionally, a microbial community analysis (16S rRNA) showed a high relative abundance of α- and β-Proteobacteria; the same classes where most AsOB are phylogenetically placed. This study establishes that AsOB are able to grow and maintain their population on low As(III) concentrations, either in presence, or absence, of other common groundwater bacteria and mineral precipitates, directly leading to an increased As removal in the filter bed.

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Current groundwater treatment facilities, mostly relying on aeration-filtration configurations, aim at the removal of iron (Fe), ammonia (NH 4 + ) and manganese (Mn). However, recently water companies expressed the ambition to also reduce arsenic (As) concentrations in these rapid sand filters. The aim of this study was to investigate the effect of the Fe oxidation state entering a biological filter bed on As removal. By varying supernatant water level, either Fe(II) or Fe(III) in the form of hydrous ferric oxides (HFO) could be stimulated to enter the filter bed at alkaline groundwater pH (7.6). The experimental pilot column filters showed that once the As(III) oxidation stabilised in the top layer of the filter sand, As removal reached its maximum (±75% at 120 cm supernatant level and 1.5 m/h filtration velocity). The increase in supernatant level from 5 to 120 cm resulted in additional HFO production prior to rapid filtration (1.5, 5 and 10 m/h), i.e. homogeneous Fe(II) oxidation and flocculation, and subsequently, HFO ending up deeper into the filter bed (120 cm filter depth). At a low supernatant water level of 5 cm, Fe(II) oxidised heterogeneously and was removed within the top 20 cm of the filter bed. Consequently, filters with high supernatant levels removed As to lower levels (by 20%) than in filters with low supernatant water levels. The benefits of Fe(II) oxidation prior to filtration for As removal was confirmed by comparing Fe(III) to Fe(II) additions in the supernatant water or in the filter bed. Overall it is concluded that in biological groundwater filters, the combination of a higher supernatant level and/or Fe(III) addition with biological As(III) oxidation in the top of the filter bed promotes As removal. @en

Arsenic (As) mobility in water is worldwide studied since its toxicity was proven in 1888. Intake of As can lead to skin disease, cancer, kidney and heart failure, diabetes and paralysis. In the Netherlands, groundwater used for drinking water production contains As in the range from 0 – 70 μg/L. Currently, all groundwater treatment plants reduce As in drinking water below the WHO standard of 10 μg/L. However, to ensure no adverse health effects occur by the intake of drinking water, Dutch drinking water companies investigate implications of distributing water with As concentrations below 1 μg/L. The new target value causes 58% of the treatment plants with measurable As in the raw water (19% of all total groundwater treatment plants) to need some sort of adjustment to their treatment scheme to comply with the new As target value...@en

The top layer of natural rapid sand filtration was found to effectively oxidise arsenite (As(III)) in groundwater treatment. However, the oxidation pathway has not yet been identified. The aim of this study was to investigate whether naturally formed manganese oxide (MnO₂), present on filter grains, could abiotically be responsible for As(III) oxidation in the top of a rapid sand filter. For this purpose As(III) oxidation with two MnO₂ containing powders was investigated in aerobic water containing manganese(II) (Mn(II)), iron(II) (Fe(II)) and/or iron(III) (Fe(III)). The first MnO₂ powder was a very pure - commercially available - natural MnO₂ powder. The second originated from a filter sand coating, produced over 22 years in a rapid filter during aeration and filtration. Jar test experiments showed that both powders oxidised As(III). However, when applying the MnO₂ in aerated, raw groundwater, As(III) removal was not enhanced compared to aeration alone. It was found that the presence of Fe(II)) and Mn(II) inhibited As(III) oxidation, as Fe(II) and Mn(II) adsorption and oxidation were preferred over As(III) on the MnO₂ surface (at pH 7). Therefore it is concluded that just because MnO₂ is present in a filter bed, it does not necessarily mean that MnO₂ will be available to oxidise As(III). However, unlike Fe(II), the addition of Fe(III) did not hinder As(III) oxidation on the MnO₂ surface; resulting in subsequent effective As(V) removal by the flocculating hydrous ferric oxides.

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Arsenic (As) mobility during full-scale aeration and rapid filtration was investigated. As(III) remained largely mobile during aeration and as supernatant water and was not efficiently immobilized. In the filter bed however, oxidation of As(III) was complete within 2 min of contact time and As removal efficiency improved. Therefore, the overall conclusion is that not aeration and supernatant storage, but the filter bed is the crucial treatment step for rapid As(III) removal, indicating the importance to control the oxidation sequence of Fe and As for achieving improved As removal efficiencies.@en