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The biomineralization of intracellular magnetite in magnetotactic bacteria (MTB) is an area of active investigation. Previous work has provided evidence that magnetite biomineralization begins with the formation of an amorphous phosphate-rich ferric hydroxide precursor phase followed by the eventual formation of magnetite within specialized vesicles (magnetosomes) through redox chemical reactions. Although important progress has been made in elucidating the different steps and possible precursor phases involved in the biomineralization process, many questions still remain. Here, we present a novel in vitro method to form magnetite directly from a mixed valence iron phosphate precursor, without the involvement of other known iron hydroxide precursors such as ferrihydrite. Our results corroborate the idea that phosphate containing phases likely play an iron storage role during magnetite biomineralization. Further, our results help elucidate the influence of phosphate ions on iron chemistry in groundwater and wastewater treatment. 

Engineering structures that bridge between elements with disparate mechanical properties are a significant challenge. Organisms reap synergy by creating complex shapes that are intricately graded. For instance, the wear-resistant cusp of the chiton radula tooth works in concert with progressively softer microarchitectural units as the mollusk grazes on and erodes rock. Herein, we focus on the stylus that connects the ultrahard and stiff tooth head to the flexible radula membrane. Using techniques that are especially suited to probe the rich chemistry of iron at high spatial resolution, in particular synchrotron Mössbauer and X-ray absorption spectroscopy, we find that the upper stylus ofCryptochiton stelleriis in fact a mineralized tissue. Remarkably, the inorganic phase is nano disperse santabarbaraite, an amorphous ferric hydroxyphosphate that has not been observed as a biomineral. The presence of two persistent polyamorphic phases, amorphous ferric phosphate and santabarbaraite, in close proximity, is a unique aspect that demonstrates the level of control over phase transformations inC. stelleridentition. The stylus is a highly graded material in that its mineral content and mechanical properties vary by a factor of 3 to 8 over distances of a few hundred micrometers, seamlessly bridging between the soft radula and the hard tooth head. The use of amorphous phases that are low in iron and high in water content may be key to increasing the specific strength of the stylus. Finally, we show that we can distill these insights into design criteria for inks for additive manufacturing of highly tunable chitosan-based composites.