Green rusts, which are mixed ferrous/ferric hydroxides, are found in many suboxic environments and are believed to play a central role in the biogeochemistry of Fe. Analysis by U LIII-edge X-ray absorption near edge spectroscopy of aqueous green rust suspensions spiked with uranyl (U(VI)) showed that U(VI) was readily reduced to U(IV) by green rust The extended X-ray absorption fine structure (EXAFS) date for uranium reduced by green rust indicate the formation of a UO2 phase. A theoretical model based on the crystal structure of UO2 was generated by using FEFF7 and fitted to the data for the UO2 standard and the uranium in the green rust samples. The model fits indicate that the number of nearest-neighbor uranium atoms decreases from 12 for the UO2 structure to 5.4 forthe uranium-green rust sample. With an assumed four near-neighbor uranium atoms per uranium atom on the surface of UO2, the best-fit value for the average number of uranium atoms indicates UO2 particles with an average diameter of 1.7 +/- 0.6 nm. The formation of nanometer-scale particles of UO2, suggested by the modeling of the EXAFS data, was confirmed by high-resolution transmission electron microscopy, which showed discrete particles (approximately 2-9 nm in diameter) of crystalline UO2. Our results clearly indicate that U(VI) (as soluble uranyl ion) is readily reduced by green rust to U(IV) in the form of relatively insoluble UO2 nanoparticles, suggesting that the presence of green rusts in the subsurface may have significant effects on the mobility of uranium, particularly under iron-reducing conditions.
Microtubule-based transport by the kinesin motors, powered by ATP hydrolysis, is essential for a wide range of vital processes in eukaryotes. We obtained insight into this process by developing atomic models for no-nucleotide and ATP states of the monomeric kinesin motor domain on microtubules from cryo-EM reconstructions at 5–6 Å resolution. By comparing these models with existing X-ray structures of ADP-bound kinesin, we infer a mechanistic scheme in which microtubule attachment, mediated by a universally conserved ‘linchpin’ residue in kinesin (N255), triggers a clamshell opening of the nucleotide cleft and accompanying release of ADP. Binding of ATP re-closes the cleft in a manner that tightly couples to translocation of cargo, via kinesin's ‘neck linker’ element. These structural transitions are reminiscent of the analogous nucleotide-exchange steps in the myosin and F1-ATPase motors and inform how the two heads of a kinesin dimer ‘gate’ each other to promote coordinated stepping along microtubules.DOI: http://dx.doi.org/10.7554/eLife.04686.001
The structures of Fe 2 O 3 nanoparticles with different sizes were investigated using Fe K-edge X-ray absorption near-edge structure (XANES) and the FEFF calculations, as well as surface modification with enediol ligands. The studies not only revealed the existence of under-coordinated Fe sites in the nanoparticles but also confirmed that these under-coordinated sites were located on the surface. Upon binding of enediol ligands, surface sites were restructured to octahedral sites. In particular, the nature of the surface defects and their correlation with the unique properties of the nanoparticles were discussed. Model calculations were conducted for Fe m O n (m g 1, n g 4) clusters of various sizes centered at Fe sites with octahedral (O h ), distorted octahedral (C 3V ) and tetrahedral (T d ) coordination geometry using FEFF8.10 programs. The main features of the calculated spectra agree with the experimental results and were correlated to the density of states, the Fe coordination geometry, and the long-range order of the lattice.
Summary Magnetotactic bacteria (MTB) use magnetosomes, membrane bound crystals of magnetite or greigite, for navigation along geomagnetic fields. In Magnetospirillum magneticum sp. AMB-1, and other MTB, a magnetosome gene island (MAI) is essential for every step of magnetosome formation. An 8-gene region of the MAI encodes several factors implicated in control of crystal size and morphology in previous genetic and proteomic studies. We show that these factors play a minor role in magnetite biomineralization in vivo. In contrast, MmsF, a previously uncharacterized magnetosome membrane protein encoded within the same region plays a dominant role in defining crystal size and morphology and is sufficient for restoring magnetite synthesis in the absence of the other major biomineralization candidates. In addition, we show that the 18 genes of the mamAB gene cluster of the MAI are sufficient for the formation of an immature magnetosome organelle. Addition of MmsF to these 18 genes leads to a significant enhancement of magnetite biomineralization and an increase in the cellular magnetic response. These results define a new biomineralization protein and lay down the foundation for the design of autonomous gene cassettes for the transfer of the magnetic phenotype in other bacteria.
Single-crystal thin films of Pb(ZrxTi1−x)O3 (PZT) covering the full compositional range (0⩽x⩽1) were deposited by metal-organic chemical vapor deposition. Epitaxial SrRuO3(001) thin films grown on SrTiO3(001) substrates by rf-magnetron sputter deposition served as template electrode layers to promote the epitaxial growth of PZT. X-ray diffraction, energy-dispersive x-ray spectroscopy, atomic force microscopy, transmission electron microscopy, and optical waveguiding were used to characterize the crystalline structure, composition, surface morphology, microstructure, refractive index, and film thickness of the deposited films. The PZT films were single crystalline for all compositions exhibiting cube-on-cube growth epitaxy with the substrate and showed very high degrees of crystallinity and orientation. The films exhibited typical root mean square surface roughness of ∼1.0–2.5 nm. For tetragonal films, the surface morphology was dominated by grain tilting resulting from ferroelectric domain formation. We report the systematic compositional variation of the optical, dielectric, polarization, and electronic transport properties of these single-crystalline PZT thin films. We show that the solid-solution phase diagram of the PZT system for thin films differs from the bulk due to epitaxy-induced strains and interfacial defect formation. High values of remanant polarization (30–55 μC/cm2) were observed for ferroelectric compositions in the range of 0.8⩽x⩽0.2. Unlike previous studies, the dielectric constant exhibited a clear dependence on composition with values ranging from 225 to 650. The coercive fields decreased with increasing Zr concentration to a minimum of 20 kV/cm for x=0.8. The undoped films exhibited both high resistivity and dielectric-breakdown strength (1013–1014 Ω cm at 100 kV/cm and 300–700 kV/cm, respectively).
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