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Published online by Cambridge University Press: 23 May 2012
Uranyl adsorption/reduction by Fe2+ on hematite and pyrite has been studied at neutral pH under anoxic and CO2-free conditions. XPS results confirm that more U3O8 precipitates on hematite than on pyrite reacted for 24 h in 160 μM uranyl nitrate and 160 μM Fe2+ solution at initial pH 7.3. These results are explained in terms of co-adsorption energy and U atom Mulliken charge transfer by quantum mechanical calculations. Moreover, in situ fluid tapping-mode AFM experiments on hematite indicate a deceleration of the U reduction rate within 24 h due to the passivation of the surface caused by the formation of orthorhombic U3O8 crystals. In addition, crystals observed using AFM show morphologies of orthorhombic schoepite appearing on hematite after 5 h.