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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.

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