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Metallic iron (Fe0) is a reactive material for treating polluted water. The effect of water salinity on the efficiency of Fe0-based remediation systems is not yet established. This work aims to clarify the reasons why Cl− ions are often reported to improve the efficiency of Fe0/H2O remediation systems. Quiescent batch experiments were carried out to characterize the effect of chloride (Cl−) ions on the efficiency of methylene blue (MB) discoloration in the presence of Fe0. Cl− was used in the form of NaCl at concentrations ranging from 0 to 40 g L−1. The MB concentration was 10 mg L−1, the Fe0 loading was 5 g L−1, and the duration of the experiment varied from 2 to 46 days. Four different Fe0 materials were tested in parallel experiments. Tests with different NaCl levels were performed in parallel with three other organic dyes: Methyl orange (MO), orange II (OII), and reactive red 120 (RR 120). The results clearly show that the presence of Cl− reduces the extent of dye discoloration in all systems investigated. The efficiency of the dyes increased in the order MB < MO < RR 120 < OII. In systems with varying NaCl concentrations, dye discoloration initially decreases with increasing NaCl and slightly increases for [NaCl] > 30 g L−1. However, the extent of dye discoloration for [NaCl] = 40 g L−1 remains much lower than for the system with [NaCl] = 0 g L−1. The results clearly demonstrate that the presence of Cl− fundamentally delays the process of contaminant removal in Fe0/H2O systems, thus improving the understanding of the contaminant interactions in Fe0-based remediation systems. These results also suggest that the effects of other inorganic anions on the efficiency of Fe0/H2O systems should be revisited for the design of field applications.

Granular metallic iron (gFe0) materials have been widely used for eliminating a wide range of pollutants from aqueous solutions over the past three decades. However, the intrinsic reactivity of gFe0 is rarely evaluated and existing methods for such evaluations have not been standardized. The aim of the present study was to develop a simple spectrophotometric method to characterize the intrinsic reactivity of gFe0 based on the extent of iron dissolution in an ascorbic acid (AA—0.002 M or 2 mM) solution. A modification of the ethylenediaminetetraacetic acid method (EDTA method) is suggested for this purpose. Being an excellent chelating agent for FeII and a reducing agent for FeIII, AA sustains the oxidative dissolution of Fe0 and the reductive dissolution of FeIII oxides from gFe0 specimens. In other words, Fe0 dissolution to FeII ions is promoted while the further oxidation to FeIII ions is blocked. Thus, unlike the EDTA method that promotes Fe0 oxidation to FeIII ions, the AA method promotes only the formation of FeII species, despite the presence of dissolved O2. The AA test is more accurate than the EDTA test and is considerably less expensive. Eight selected gFe0 specimens (ZVI1 through ZVI8) with established diversity in intrinsic reactivity were tested in parallel batch experiments (for 6 days) and three of these specimens (ZVI1, ZVI3, ZVI5) were further tested for iron leaching in column experiments (for 150 days). Results confirmed the better suitability (e.g., accuracy in assessing Fe0 dissolution) of the AA test relative to the EDTA test as a powerful screening tool to select materials for various field applications. Thus, the AA test should be routinely used to characterize and rationalize the selection of gFe0 in individual studies.

The whole population of Feutap still collects drinking water from two protected springs, some 1 km away from this small rural agglomeration. For many generations, the only improvement has been the protection of the springs during the 1980s. The resulting high incidence of gastrointestinal infections continues to hinder the socioeconomic development of this mountain community. This dynamic wherein “poverty begets disease, and disease begets poverty” seems endless given the number of water improvement programs and other health-focused campaigns in rural areas of Cameroon since the 1960s. Fortunately, the hydrographic regime of Feutap and its geographical situation enable the implementation of the Kilimanjaro Concept (KC), wherein rainwater is quantitatively harvested, partly infiltrated, and largely stored to (i) meet the whole-year water needs of the population, (ii) create new ecosystems, and (iii) enable irrigated agriculture. This communication prepares the implementation of the KC in Feutap, including the creation of irrigation ponds for agriculture and small farm animals (e.g., goats and sheep). The view is promoted that Feutap is a potential viable space in which life and work are possible, using the existing rainfall and the few natural springs in a sustainable manner. The presented concept can be extended to other hilly small communities with similar hydraulic regimes.

Science denial relates to rejecting well-established views that are no longer questioned by scientists within a given community. This expression is frequently connected with climate change and evolution. In such cases, prevailing views are built on historical facts and consensus. For water remediation using metallic iron (Fe0), also known as the remediation Fe0/H2O system, a consensus on electro-chemical contaminant reduction was established during the 1990s and still prevails. Arguments against the reductive transformation concept have been regarded for more than a decade as ‘science denial’. However, is it the prevailing concept that denies the science of aqueous iron corrosion? This article retraces the path taken by our research group to question the reductive transformation concept. It is shown that the validity of the following has been questioned: (i) analytical applications of the arsenazo III method for the determination of uranium, (ii) molecular diffusion as sole relevant mass-transport process in the vicinity of the Fe0 surface in filtration systems, and (iii) the volumetric expansive nature of iron corrosion at pH > 4.5. Item (i) questions the capability of Fe0 to serve as an electron donor for UVI reduction under environmental conditions. Items (ii) and (iii) are inter-related, as the Fe0 surface is permanently shielded by a non-conductive oxide scale acting as a diffusion barrier to dissolved species and a barrier to electrons from Fe0. The net result is that no electron transfer from Fe0 to contaminants is possible under environmental conditions. This conclusion refutes the validity of the reductive transformation concept and calls for alternative theories.

This article critically evaluates the conventional Kanchan Arsenic Filter (KAF) in order to determine the main reasons for its reported poor performance. The KAF was introduced in 2004 in Nepal and makes use of non-galvanized nails as a Fe0 source for As removal. As early as 2009, the KAF was demonstrated to be ineffective for As removal in many cases. This was unambiguously attributed to the Fe0 layer which is placed on top of a sand filter instead of being incorporated into a sand matrix. Despite this conceptual mistake, the conventional KAF has been largely distributed in Asia, and recent articles have assessed its sustainability. This study reiterates that the suitability of the technology, rather than its sustainability, should be addressed. Evidence shows that the KAF has the following design limitations: (i) uses iron nails of unknown reactivity, and (ii) operates on the principle of a wet/dry cycle. The latter causes a decrease in the corrosion rate of the used nails, thereby limiting the availability of the iron corrosion products which act as contaminant scavengers. Taken together, these results confirm the unsuitability of the conventional KAF. Besides correcting the design mistakes, more attention should be paid to the intrinsic reactivity of the used iron nails, including using alternative Fe0 materials (e.g., iron filings, steel wool) for filters lasting for just 6 or 18 months. Specific design considerations to be addressed in the future are highlighted.

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Results from different research suggest that metallic iron (Fe0) materials enhance anaerobic digestion (AD) systems to remove organics (chemical oxygen demand (COD)), phosphorus and nitrogen from polluted water. However, the available results are difficult to compare because they are derived from different experimental conditions. This research characterises the effects of Fe0 type and dosage in AD systems to simultaneously remove COD and nutrients (orthophosphate (PO43−), ammonium (NH4+), and nitrate (NO3−)) Lab-scale reactors containing domestic sewage (DS) were fed with various Fe0 dosages (0 to 30 g/L). Batch AD experiments were operated at 37 ± 0.5 °C for 76 days; the initial pH value was 7.5. Scrap iron (SI) and steel wool (SW) were used as Fe0 sources. Results show that: (i) SW performed better than SI on COD and PO43− removal (ii) optimum dosage for the organics and nutrients removal was 10 g/L SI (iii) (NO3− + NH4+) was the least removed pollutant (iv) maximum observed COD, PO43− and NO3− + NH4+ removal efficiencies were 88.0%, 98.0% and 40.0% for 10 g/L SI, 88.2%, 99.9%, 25.1% for 10 g/L SW, and 68.9%, 7.3% and 0.7% for the reference system. Fe0-supported AD significantly removed the organics and nutrients from DS.

Scientific collaboration among various geographically scattered research groups on the broad topic of “metallic iron (Fe0) for water remediation” has evolved greatly over the past three decades. This collaboration has involved different kinds of research partners, including researchers from the same organization and domestic researchers from non-academic organizations as well as international partners. The present analysis of recent publications by some leading scientists shows that after a decade of frank collaboration in search of ways to improve the efficiency of Fe0/H2O systems, the research community has divided itself into two schools of thought since about 2007. Since then, progress in knowledge has stagnated. The first school maintains that Fe0 is a reducing agent for some relevant contaminants. The second school argues that Fe0 in-situ generates flocculants (iron hydroxides) for contaminant scavenging and reducing species (e.g., FeII, H2, and Fe3O4), but reductive transformation is not a relevant contaminant removal mechanism. The problem encountered in assessing the validity of the views of both schools arises from the quantitative dominance of the supporters of the first school, who mostly ignore the second school in their presentations. The net result is that the various derivations of the original Fe0 remediation technology may be collectively flawed by the same mistake. While recognizing that the whole research community strives for the success of a very promising but unestablished technology, annual review articles are suggested as an ingredient for successful collaboration.

Metallic iron (Fe0) corrosion under immersed conditions (Fe0/H2O system) has been used for water treatment for the past 170 years. Fe0 generates solid iron corrosion products (FeCPs) which are known to in situ coat the surface of aggregates, including granular activated carbon (GAC), gravel, lapillus, manganese oxide (MnO2), pyrite (FeS2), and sand. While admixing Fe0 and reactive aggregates to build hybrid systems (e.g., Fe0/FeS2, Fe0/MnO2, Fe0/sand) for water treatment, it has been largely overlooked that these materials would experience reactivity loss upon coating. This communication clarifies the relationships between aggregate addition and the sustainability of Fe0/H2O filtration systems. It is shown that any enhanced contaminant removal efficiency in Fe0/aggregate/H2O systems relative to the Fe0/H2O system is related to the avoidance/delay of particle cementation by virtue of the non-expansive nature of the aggregates. The argument that aggregate addition sustains any reductive transformation of contaminants mediated by electrons from Fe0 is disproved by the evidence that Fe0/sand systems are equally more efficient than pure Fe0 systems. This demonstration corroborates the concept that aqueous contaminant removal in iron/water systems is not a process mediated by electrons from Fe0. This communication reiterates that only hybrid Fe0/H2O filtration systems are sustainable.

Providing everyone with safe drinking water is a moral imperative. Yet, sub-Saharan Africa seems unable to achieve “safe drinking water for all” by 2030. This sad situation calls for a closer examination of the water supply options for both rural and urban populations. Commonly, two main aspects are considered: (1) behavioural responses to available or potential water supply options, and (2) socio-economic acceptability. These aspects determine the feasibility and the affordability of bringing safe drinking water as a basic good and human right to everyone. There is a broad consensus that achieving the UN Sustainable Development Goal 6.1 is mostly a financial issue, especially in low-income settings. This communication challenges this view as water is available everywhere and affordable treatment options are well-known. It considers the decentralized water supply model as a reference or standard approach in low-income settings rather than as an alternative. Here, the medium-sized city of Bangangté in the western region of Cameroon is used to demonstrate that universal safe drinking water will soon be possible. In fact, during the colonial period, the residences of the elite and the main institutions, including the administrative quarter, churches, and hospital, have been supplied with clean water from various local sources. All that is needed is to consider everyone as important or accept safe drinking water as human right. First, we present a historical background on water supply in the colonial period up to 1980. Second, the drinking water supply systems and water demand driven by population growth are discussed. Finally, a hybrid model for the achieving of universal access to clean drinking water, and preconditions for its successful implementation, are presented. Overall, this communication calls for a shift from safe drinking water supply approaches dominated by centralized systems, and presents a transferable hybrid model to achieve universal clean drinking water.

There is escalating salinity levels on small islands due to uncontrolled groundwater extraction. Conventionally, this challenge is addressed by adopting optimal groundwater pumping strategies. Currently, on Unguja Island (Zanzibar), urban freshwater is supplied by desalination, which is expensive and energy-intensive. Hence, desalinization cannot be afforded by rural communities. This study demonstrates that the innovative Kilimanjaro Concept (KC), based on rainwater harvesting (RWH) can remediate seawater intrusion in Unguja, while enabling a universal safe drinking water supply. The reasoning is rooted in the water balance of the whole island. It is shown that if rainwater is systematically harvested, quantitatively stored, and partly infiltrated, seawater intrusion will be reversed, and a universal safe drinking water supply will be secured. Water treatment with affordable technologies (e.g., filtration and adsorption) is suggested. The universality of KC and its suitability for small islands is demonstrated. Future research should focus on pilot testing of this concept on Unguja Island and other island nations.

Since the realization in the 1930s that elevated fluoride concentrations in drinking water can have detrimental effects on human health, new methods have been progressively developed in order to reduce fluoride to acceptable levels. In the developing world the necessity for filtration media that are both low-cost and sourced from locally available materials has resulted in the widespread use of bone char. Since the early 1990s metallic iron (Fe0) has received widespread use as both an adsorbent and a reducing agent for the removal of a wide range of contaminant species from water. The ion-selectivity of Fe0 is dictated by the positively charged surface of iron (hydr)oxides at circumneutral pH. This suggests that Fe0 could potentially be applied as suitable filter media for the negatively charged fluoride ion. This communication seeks to demonstrate from a theoretical basis and using empirical data from the literature the suitability of Fe0 filters for fluoride removal. The work concludes that Fe0-bearing materials, such as steel wool, hold good promise as low-cost, readily available and highly effective decentralized fluoride treatment materials.

Metallic iron (Fe0) has been demonstrated as an excellent material for decentralized safe drinking water provision, wastewater treatment and environmental remediation. An open issue for all these applications is the rational material selection or quality assurance. Several methods for assessing Fe0 quality have been presented, but all of them are limited to characterizing its initial reactivity. The present study investigates H2 evolution in an acidic solution (pH 2.0) as an alternative method, while comparing achieved results to those of uranium removal in quiescent batch experiments at neutral pH values. The unique feature of the H2 evolution experiment is that quantitative H2 production ceased when the pH reached a value of 3.1. A total of twelve Fe0 specimens were tested. The volume of molecular H2 produced by 2.0 g of each Fe0 specimen in 560 mL H2SO4 (0.01 M) was monitored for 24 h. Additionally, the extent of U(VI) (0.084 mM) removal from an aqueous solution (20.0 mL) by 0.1 g of Fe0 was characterized. All U removal experiments were performed at room temperature (22 ± 2 °C) for 14 days. Results demonstrated the difficulty of comparing Fe0 specimens from different sources and confirmed that the elemental composition of Fe0 is not a stand-alone determining factor for reactivity. The time-dependent changes of H2 evolution in H2SO4 confirmed that tests in the neutral pH range just address the initial reactivity of Fe0 materials. In particular, materials initially reacting very fast would experience a decrease in reactivity in the long-term, and this aspect must be incorporated in designing novel materials and sustainable remediation systems. An idea is proposed that could enable the manufacturing of intrinsically long-term efficient Fe0 materials for targeted operations as a function of the geochemistry.

A critical survey of the abundant literature on environmental remediation and water treatment using metallic iron (Fe0) as reactive agent raises two major concerns: (i) the peculiar properties of the used materials are not properly considered and characterized, and, (ii) the literature review in individual publications is very selective, thereby excluding some fundamental principles. Fe0 specimens for water treatment are typically small in size. Before the advent of this technology and its application for environmental remediation, such small Fe0 particles have never been allowed to freely corrode for the long-term spanning several years. As concerning the selective literature review, the root cause is that Fe0 was considered as a (strong) reducing agent under environmental conditions. Subsequent interpretation of research results was mainly directed at supporting this mistaken view. The net result is that, within three decades, the Fe0 research community has developed itself to a sort of modern knowledge system. This communication is a further attempt to bring Fe0 research back to the highway of mainstream corrosion science, where the fundamentals of Fe0 technology are rooted. The inherent errors of selected approaches, currently considered as countermeasures to address the inherent limitations of the Fe0 technology are demonstrated. The misuse of the terms “reactivity”, and “efficiency”, and adsorption kinetics and isotherm models for Fe0 systems is also elucidated. The immense importance of Fe0/H2O systems in solving the long-lasting issue of universal safe drinking water provision and wastewater treatment calls for a science-based system design.

There are many factors to consider for the design of appropriate water treatment systems including: cost, the concentration and type of biological and/or chemical contamination, concentration limits at which contaminant(s) are required to be removed, required flow rate, level of local expertise for on-going maintenance, and social acceptance. An ideal technology should be effective at producing clean, potable water; however it must also be low-cost, low-energy (ideally energy-free) and require low-maintenance. The use of packed beds containing metallic iron (Fe0 filters) has the potential to become a cheap widespread technology for both safe drinking water provision and wastewater treatment. Fe0 filters have been intensively investigated over the past two decades, however, sound design criteria are still lacking. This article presents an overview of the design of Fe0 filters for decentralized water treatment particularly in the developing world. A design for safe drinking water to a community of 100 people is also discussed as starting module. It is suggested that Fe0 filters have the potential for significant worldwide applicability, but particularly in the developing world. The appropriate design of Fe0 filters, however, is site-specific and dependent upon the availability of local expertise/materials.

Slow sand filters were first used for safe drinking water provision during the 19th century. The technology has been gradually improved and utilized at several scales. Based on their intrinsic limitations other filtration systems have been developed, including membrane technologies. The universal applicability of filtration in drinking water supply makes filters a device of choice to facilitate the achievement of the UN Sustainable Development Goals (‘drinking water for all by 2030’). Available strategies to rationally design efficient and sustainable water filters are scattered in the literature and are difficult to access and evaluate by starting researchers. The present Special Issue summarizes knowledge on two key filtration systems for drinking water supply: (i) membrane technology and (ii) metallic iron based filters. The five (5) accepted articles are being briefly presented herein.

Inadequate access to safe drinking water is one of the most pervasive problems currently afflicting the developing world. Scientists and engineers are called to present affordable but efficient solutions, particularly applicable to small communities. Filtration systems based on metallic iron (Fe0) are discussed in the literature as one such viable solution, whether as a stand-alone system or as a complement to slow sand filters (SSFs). Fe0 filters can also be improved by incorporating biochar to form Fe0-biochar filtration systems with potentially higher contaminant removal efficiencies than those based on Fe0 or biochar alone. These three low-cost and chemical-free systems (Fe0, biochar, SSFs) have the potential to provide universal access to safe drinking water. However, a well-structured systematic research is needed to design robust and efficient water treatment systems based on these affordable filter materials. This communication highlights the technology being developed to use Fe0-based systems for decentralized safe drinking water provision. Future research directions for the design of the next generation Fe0-based systems are highlighted. It is shown that Fe0 enhances the efficiency of SSFs, while biochar has the potential to alleviate the loss of porosity and uncertainties arising from the non-linear kinetics of iron corrosion. Fe0-based systems are an affordable and applicable technology for small communities in low-income countries, which could contribute to attaining self-reliance in clean water supply and universal public health.

Fluorosis has been prevalent in the great East African Rift Valley (EARV) since before this region was given a name. In the Tanganyika days, Germans reported elevated fluoride concentrations in natural waters. In the 1930s, the clear relationship between high fluoride level and mottling of teeth was established. Since then, the global research community has engaged in the battle to provide fluoride-free drinking water, and the battle is not yet won for low-income communities. An applicable concept for fluoride-free drinking water in the EARV was recently presented, using the Kilimanjaro as a rainwater harvesting park. The Kilimanjaro concept implies that rainwater is harvested, stored on the Kilimanjaro mountains, gravity-transported to the point of use, eventually blended with natural water and treated for distribution. This article provides a roadmap for the implementation of the Kilimanjaro concept in Tanzania. Specifically, the current paper addresses the following: (i) presents updated nationwide information on fluoride contaminated areas, (ii) discusses the quality and quantity of rainwater, and current rainwater harvesting practices in Tanzania, (iii) highlights how low-cost water filters based on Fe0/biochar can be integrating into rainwater harvesting (RWH) systems to provide clean drinking water, and (iv) discusses the need for strict regulation of RWH practices to optimize water collection and storage, while simplifying the water treatment chain, and recommends strict analytical monitoring of water quality and public education to sustain public health in the EARV. In summary, it is demonstrated that, by combining rainwater harvesting and low-cots water treatment methods, the Kilimanjaro concept has the potential to provide clean drinking water, and overcome fluorosis on a long-term basis. However, a detailed design process is required to determine: (i) institutional roles, and community contributions and participation, (ii) optimal location and sizing of conveyance and storage facilities to avoid excessive pumping costs, and (iii) project funding mechanisms, including prospects for government subsidy. By drawing attention to the Kilimanjaro concept, the article calls for African engineers and scientists to take the lead in translating this concept into reality for the benefit of public health, while simultaneously increasing their self-confidence to address other developmental challenges pervasive in Africa.

Elemental iron (Fe0) has been widely used in groundwater/soil remediation, safe drinking water provision, and wastewater treatment. It is still mostly reported that a surface-mediated reductive transformation (direct reduction) is a dominant decontamination mechanism. Thus, the expressions “contaminant removal„ and “contaminant reduction„ are interchangeably used in the literature for reducible species (contaminants). This contribution reviews the scientific literature leading to the advent of the Fe0 technology and shows clearly that reductive transformations in Fe0/H2O systems are mostly driven by secondary (FeII, H/H2) and tertiary/quaternary (e.g., Fe3O4, green rust) reducing agents. The incidence of this original mistake on the Fe0 technology and some consequences for its further development are discussed. It is shown, in particular, that characterizing the intrinsic reactivity of Fe0 materials should be the main focus of future research.

Efficient but affordable water treatment technologies are currently sought to solve the prevalent shortage of safe drinking water. Adsorption-based technologies are in the front-line of these efforts. Upon proper design, universally applied materials (e.g., activated carbons, bone chars, metal oxides) are able to quantitatively remove inorganic and organic pollutants as well as pathogens from water. Each water filter has a defined removal capacity and must be replaced when this capacity is exhausted. Operational experience has shown that it may be difficult to convince some low-skilled users to buy new filters after a predicted service life. This communication describes the quest to develop a filter-clock to encourage all users to change their filters after the designed service life. A brief discussion on such a filter-clock based on rusting of metallic iron (Fe0) is presented. Integrating such filter-clocks in the design of water filters is regarded as essential for safeguarding public health.

Continuous gravity-fed column experiments using the methylene blue (MB) discoloration method were performed to characterize the suitability of a pozzolan (PZ) specimen as alternative admixing aggregate for metallic iron filters (Fe0-filters). Investigated systems were: (i) pure sand, (ii) pure PZ, (iii) pure Fe0, (iv) Fe0/sand, (v) Fe0/PZ, and (vi) Fe0/sand/PZ. The volumetric proportion of Fe0 was 25%. The volumetric proportions of the Fe0/sand/PZ system was 25/45/30. The initial MB concentration was 2.0 mg·L−1, 6.0 g of Fe0 was used, and the experiments lasted for 46 days. The individual systems were fed with 3.9 to 8.4 L (7.80 to 16.69 mg of MB) and were characterized by the time-dependent changes of: (i) the pH value, (ii) the iron breakthrough, (iii) the MB breakthrough, and (iv) the hydraulic conductivity. Results showed that the Fe0/sand/PZ system was the most efficient. This ternary system was also the most permeable and therefore the most sustainable. The suitability of MB as a powerful operative indicator for the characterization of processes in the Fe0/H2O system was confirmed. The tested PZ is recommended as an alternative material for efficient but sustainable Fe0 filters.

Since its introduction about 25 years ago, metallic iron (Fe0) has shown its potential as the key component of reactive filtration systems for contaminant removal in polluted waters. Technical applications of such systems can be enhanced by numerical simulation of a filter design to improve, e.g., the service time or the minimum permeability of a prospected system to warrant the required output water quality. This communication discusses the relevant input quantities into such a simulation model, illustrates the possible simplifications and identifies the lack of relevant thermodynamic and kinetic data. As a result, necessary steps are outlined that may improve the numerical simulation and, consequently, the technical design of Fe0 filters. Following a general overview on the key reactions in a Fe0 system, the importance of iron corrosion kinetics is illustrated. Iron corrosion kinetics, expressed as a rate constant kiron, determines both the removal rate of contaminants and the average permeability loss of the filter system. While the relevance of a reasonable estimate of kiron is thus obvious, information is scarce. As a conclusion, systematic experiments for the determination of kiron values are suggested to improve the database of this key input parameter to Fe0 filters.