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Impact of organic phosphates on the structure and composition of short-range ordered iron nanophases

Urheber*innen
/persons/resource/zhchen

Chen,  Zhengzheng
3.5 Interface Geochemistry, 3.0 Geochemistry, Departments, GFZ Publication Database, Deutsches GeoForschungsZentrum;

/persons/resource/jpperez

Perez,  J.P.H.
3.5 Interface Geochemistry, 3.0 Geochemistry, Departments, GFZ Publication Database, Deutsches GeoForschungsZentrum;

Smales,  Glen J.
External Organizations;

/persons/resource/rblukis

Blukis,  Roberts
3.5 Interface Geochemistry, 3.0 Geochemistry, Departments, GFZ Publication Database, Deutsches GeoForschungsZentrum;

Pauw,  Brian R.
External Organizations;

/persons/resource/jessi

Stammeier,  Jessica Alexandra
3.1 Inorganic and Isotope Geochemistry, 3.0 Geochemistry, Departments, GFZ Publication Database, Deutsches GeoForschungsZentrum;

Radnik,  Jörg
External Organizations;

Smith,  Andrew J.
External Organizations;

/persons/resource/benning

Benning,  Liane G.
3.5 Interface Geochemistry, 3.0 Geochemistry, Departments, GFZ Publication Database, Deutsches GeoForschungsZentrum;

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5025723.pdf
(Verlagsversion), 3MB

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Zitation

Chen, Z., Perez, J., Smales, G. J., Blukis, R., Pauw, B. R., Stammeier, J. A., Radnik, J., Smith, A. J., Benning, L. G. (2024): Impact of organic phosphates on the structure and composition of short-range ordered iron nanophases. - Nanoscale Advances, 6, 2656-2668.
https://doi.org/10.1039/D3NA01045G


Zitierlink: https://gfzpublic.gfz-potsdam.de/pubman/item/item_5025723
Zusammenfassung
Organic phosphates (OP) are important nutrient components for living cells in natural environments, where they readily interact with ubiquitous iron phases such as hydrous ferric oxide, ferrihydrite (FHY). FHY partakes in many key bio(geo)chemical reactions including iron-mediated carbon storage in soils, or iron-storage in living organisms. However, it is still unknown how OP affects the formation, structure and properties of FHY. Here, we document how β-glycerophosphate (GP), a model OP ligand, affects the structure and properties of GP–FHY nanoparticles synthesized by coprecipitation at variable nominal molar P/Fe ratios (0.01 to 0.5). All GP–FHY precipitates were characterized by a maximum solid P/Fe ratio of 0.22, irrespective of the nominal P/Fe ratio. With increasing nominal P/Fe ratio, the specific surface area of the GP–FHY precipitates decreased sharply from 290 to 3 m2 g−1, accompanied by the collapse of their pore structure. The Fe–P local bonding environment gradually transitioned from a bidentate binuclear geometry at low P/Fe ratios to monodentate mononuclear geometry at high P/Fe ratios. This transition was accompanied by a decrease in coordination number of edge-sharing Fe polyhedra, and the loss of the corner-sharing Fe polyhedra. We show that Fe(III) polymerization is impeded by GP, and that the GP–FHY structure is highly dependent on the P/Fe ratio. We discuss the role that natural OP-bearing Fe(III) nanophases have in biogeochemical reactions between Fe–P and C species in aquatic systems.