Metallic iron (Fe0) materials have been industrially used for water treatment since the 1850s. There are still many fundamental challenges in affordably and reliably characterizing the Fe0 intrinsic reactivity. From the available methods, the one using Fe0 dissolution in ethylenediaminetetraacetic acid (EDTA—2 mM) was demonstrated the most applicable as it uses only four affordable chemicals: Ascorbic acid, an ascorbate salt, EDTA and 1,10-Phenanthroline (Phen). A careful look at these chemicals reveals that EDTA and Phen are complexing agents for dissolved iron species. Fe3-EDTA is very stable and difficult to destabilize; ascorbic acid is one of the few appropriate reducing agents, therefore. On the other hand, the Fe2-Phen complex is so stable that oxidation by dissolved O2 is not possible. This article positively tests Fe0 (0.1 g) dissolution in 2 mM Phen (50 mL) as a characterization tool for the intrinsic reactivity, using 9 commercial steel wool (Fe0 SW) specimens as probe materials. The results are compared with those obtained by the EDTA method. The apparent iron dissolution rate in EDTA (kEDTA) and in Phen (kPhen) were such that 0.53 ≤ kEDTA (μg h−1) ≤ 4.81 and 0.07 ≤ kPhen (μg h−1) ≤ 1.30. Higher kEDTA values, relative to kPhen, are a reflection of disturbing Fe3 species originating from Fe2 oxidation by dissolved O2 and dissolution of iron corrosion products. It appears that the Phen method considers only the forward dissolution of Fe0. The Phen method is reliable and represents the most affordable approach for characterizing the suitability of Fe0 for water treatment.

The high availability of fluoride in surface and groundwater in the East African Rift Valley was documented during the colonial period. Since the early 1960s, many studies have been conducted to solve the fluorosis crisis in this region. At present, no cost-effective solution to mitigate fluoride contamination is available for the large majority of the population. This situation prompted a process analysis of commonly used technologies. Results revealed that the geochemistry of fluoride is the main problem. Fluoride is very difficult to remove from the aqueous phase. Thus, eliminating the need for technical water defluoridation is an excellent way out of the fluorosis crisis. This goal can be achieved by harvesting fluoride-free rainwater. Harvested rainwater can be mixed with naturally polluted waters in calculated proportions to obtain safe drinking water (blending). This paper presents a concept to transform the Kilimanjaro Mountains into a huge rainwater harvesting park for drinking water supply for the whole East African Rift Valley. However, blended water may contain other pollutants including pathogens that are easy to treat using low-cost methods such as metallic iron based-filters (Fe 0 filters). The proposed concept is transferable to other parts of the world still enduring fluoride pollution.

Studies were undertaken to determine the reasons why published information regarding the efficiency of metallic iron (Fe 0 ) for water treatment is conflicting and even confusing. The reactivity of eight Fe 0 materials was characterized by Fe dissolution in a dilute solution of ethylenediaminetetraacetate (Na 2 -EDTA; 2 mM). Both batch (4 days) and column (100 days) experiments were used. A total of 30 different systems were characterized for the extent of Fe release in EDTA. The effects of Fe 0 type (granular iron, iron nails and steel wool) and pretreatment procedure (socking in acetone, EDTA, H 2 O, HCl and NaCl for 17 h) were assessed. The results roughly show an increased iron dissolution with increasing reactive sites (decreasing particle size: wool > filings > nails), but there were large differences between materials from the same group. The main output of this work is that available results are hardly comparable as they were achieved under very different experimental conditions. A conceptual framework is presented for future research directed towards a more processed understanding.Sustainability 2019, 11, 671 2 of 20 organic [27,28], fluoride [29][30][31], heavy metals [32,33], nitrate [34,35], pathogens [36][37][38] and radionuclides [32,39]. The desalination of water using Fe 0 has also been reported [40][41][42][43]. The two key advantages of Fe 0 are its affordability and its universal availability (iron nails, scrap iron and steel wool) [9,10,44,45]. It is commonly reported that the major drawback of Fe 0 -based technologies for water treatment is the low intrinsic reactivity of granular materials [28,33,46]. This situation is said to be aggravated by the inherent generation of an oxide scale at the Fe 0 surface (passivation). Countermeasures to overcome Fe 0 passivation were recently reviewed by Guan et al. [28] and further discussed by Noubactep [47]. It is recalled that, considering passivation as a "curse" contradicts the evidence that Fe 0 -based subsurface permeable barriers have been successfully working for more than one decade [48][49][50]. On the other hand, increased "passivation" should have occurred in the spongy iron filters in Antwerpen as well [2,19]. Clarifying this contradiction is certainly a progress for the whole Fe 0 technology. Clearly, an understanding of the role of "passivation" in the process of decontamination using Fe 0 should be useful for enhancing the system's efficiency in practice [30,31,47].There is an agreement on the evidence that using Fe 0 for water treatment and environmental remediation is "putting corrosion to use" [51][52][53]. There is otherwise a contradiction on practically any other aspect concerning the Fe 0 /H 2 O system, including the reaction mechanisms and factors determining the long-term efficiency of such systems [9,28,47,[54][55][56][57][58]. A key reason for this is the large variability of experimental conditions used in testing Fe 0 materials [58][59][60][61][62]. The main influencing operational parameter seems to be Fe 0 itself [58,61,63,6...

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.

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.