Susceptibility of Goethite to Fe2+-Catalyzed Recrystallization over Time

Recent work has shown that iron oxides, such as goethite and hematite, may recrystallize in the presence of aqueous Fe2+under anoxic conditions. This process, referred to as Fe2+-catalyzed recrystallization, can influence water quality by causing the incorporation/release of environmental contaminants and biological nutrients. Accounting for the effects of Fe2+-catalyzed recrystallization on water quality requires knowing the time scale over which recrystallization occurs. Here, we tested the hypothesis that nanoparticulate goethite becomes less susceptible to Fe2+-catalyzed recrystallization over time. We set up two batches of reactors in which 55Fe2+tracer was added at two different time points and tracked the 55Fe partitioning in the aqueous and goethite phases over 60 days. Less 55Fe uptake occurred between 30 and 60 days than between 0 and 30 days, suggesting goethite recrystallization slowed with time. Fitting the data with a box model indicated that 17% of the goethite recrystallized after 30 days of reaction, and an additional 2% recrystallized between 30 and 60 days. The decreasing susceptibility of goethite to recrystallize as it reacted with aqueous Fe2+suggested that recrystallization is likely only an important process over short time scales.