Rechargeable battery technologies have ignited major breakthroughs in contemporary society, including but not limited to revolutions in transportation, electronics, and grid energy storage The remarkable development of rechargeable batteries is largely attributed to in-depth efforts to improve battery electrode and electrolyte materials There are, however, still intimidating challenges of lower cost, longer cycle and calendar life, higher energy density, and better safety for large scale energy storage and vehicular applications Further progress with rechargeable batteries may require new chemistries (lithium ion batteries and beyond) and better understanding of materials electrochemistry in the various battery technologies In the past decade, advancement of battery materials has been complemented by new analytical techniques that are capable of probing battery chemistries at various length and time scales Synchrotron X-ray techniques stand out as one of the most effective methods that allow for near

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Synchrotron X-ray Analytical Techniques for Studying Materials Electrochemistry in Rechargeable Batteries

The effect of interstitial carbon on the mechanical properties and dislocation substructure evolution in Fe40.4Ni11.3Mn34.8Al7.5Cr6 high entropy alloys

Modern approaches for bioremediation of radionuclide contaminated environments are based on the ability of microorganisms to effectively catalyze changes in the oxidation states of metals that in turn influence their solubility. Although microbial metal reduction has been identified as an effective means for immobilizing highly-soluble uranium(VI) complexes in situ, the biomolecular mechanisms of U(VI) reduction are not well understood. Here, we show that c-type cytochromes of a dissimilatory metal-reducing bacterium, Shewanella oneidensis MR-1, are essential for the reduction of U(VI) and formation of extracelluar UO 2 nanoparticles. In particular, the outer membrane (OM) decaheme cytochrome MtrC (metal reduction), previously implicated in Mn(IV) and Fe(III) reduction, directly transferred electrons to U(VI). Additionally, deletions of mtrC and/or omcA significantly affected the in vivo U(VI) reduction rate relative to wild-type MR-1. Similar to the wild-type, the mutants accumulated UO 2 nanoparticles extracellularly to high densities in association with an extracellular polymeric substance (EPS). In wild-type cells, this UO 2-EPS matrix exhibited glycocalyx-like properties and contained multiple elements of the OM, polysaccharide, and heme-containing proteins. Using a novel combination of methods including synchrotron-based X-ray fluorescence microscopy and high-resolution immune-electron microscopy, we demonstrate a close association of the extracellular UO 2 nanoparticles with MtrC and OmcA (outer membrane cytochrome). This is the first study to our knowledge to directly localize the OM-associated cytochromes with EPS, which contains biogenic UO 2 nanoparticles. In the environment, such association of UO 2 nanoparticles with biopolymers may exert a strong influence on subsequent behavior including susceptibility to oxidation by O 2 or transport in soils and sediments.

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c-Type cytochrome-dependent formation of U(IV) nanoparticles by Shewanella oneidensis.

The ability to alter nutrient partitioning within plants cells is poorly understood. In Arabidopsis (Arabidopsis thaliana), a family of endomembrane cation exchangers (CAXs) transports Ca2+ and other cations. However, experiments have not focused on how the distribution and partitioning of calcium (Ca) and other elements within seeds are altered by perturbed CAX activity. Here, we investigate Ca distribution and abundance in Arabidopsis seed from cax1 and cax3 loss-of-function lines and lines expressing deregulated CAX1 using synchrotron x-ray fluorescence microscopy. We conducted 7- to 10-μm resolution in vivo x-ray microtomography on dry mature seed and 0.2-μm resolution x-ray microscopy on embryos from lines overexpressing deregulated CAX1 (35S-sCAX1) and cax1cax3 double mutants only. Tomograms showed an increased concentration of Ca in both the seed coat and the embryo in cax1, cax3, and cax1cax3 lines compared with the wild type. High-resolution elemental images of the mutants showed that perturbed CAX activity altered Ca partitioning within cells, reducing Ca partitioning into organelles and/or increasing Ca in the cytosol and abolishing tissue-level Ca gradients. In comparison with traditional volume-averaged metal analysis, which confirmed subtle changes in seed elemental composition, the collection of spatially resolved data at varying resolutions provides insight into the impact of altered CAX activity on seed metal distribution and indicates a cell type-specific function of CAX1 and CAX3 in partitioning Ca into organelles. This work highlights a powerful technology for inferring transport function and quantifying nutrient changes.

The role of CAX1 and CAX3 in elemental distribution and abundance in Arabidopsis seed

The structures of oxides formed in water and lithiated water on three Zr-based alloys with varied corrosion behavior were studied with micro-beam synchrotron radiation and optical microscopy. Micro-beam synchrotron radiation (0.2 µm spot) has a unique combination of high elemental sensitivity (ppm level) and fine spatial resolution that allowed the determination of various oxide characteristics such as phase content, texture, grain size, and composition as a function of distance from the oxide-metal interface. Micro-beam X-ray fluorescence shows that the oxides formed in lithiated water have increased levels of Fe absorbed from the autoclave environment indicating greater oxide porosity in these oxides. The phase content, texture, and grain size of oxides were studied in detail using synchrotron radiation micro-beam diffraction for samples corroded in water and lithiated water. A remarkable periodicity was observed in the oxide structures using various techniques including X-ray peak intensities for both monoclinic and tetragonal zirconia, texture, and optical microscopy. The periods were similar to the transition period and were less visible in the oxides that behaved worse in lithiated water. These results are discussed in terms of models of oxide growth and of the differences between alloys.

Microstructure and growth mechanism of oxide layers formed on Zr alloys studied with micro-beam synchrotron radiation

A hard x-ray scanning microprobe based on zone plate optics and undulator radiation, in the energy region from 6 to 20 keV, has reached a focal spot size (FWHM) of 0.15 μm(v)×0.6 μm(h), and a photon flux of 4×109 photons/sec/0.01%BW. Using a slit 44 meters upstream to create a virtual source, a circular beam spot of 0.15 μm in diameter can be obtained with a photon flux of one order of magnitude less. During fluorescence mapping of trace elements in a single human ovarian cell, the microprobe exhibited an imaging sensitivity for Pt (Lα line) of 80 attograms/μm2 for a count rate of 10 counts per second. The x-ray microprobe has been used to map crystallographic strain and multiquantum well thickness in micro-optoelectronic devices produced with the selective area growth technique.

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A hard x-ray scanning microprobe for fluorescence imaging and microdiffraction at the advanced photon source

A hard x-ray scanning microprobe based on zone plate optics and undulator radiation, in the energy region from 6 to 20 keV, has reached a focal spot size (FWHM) of 0.15 {micro}m (v) x 0.6 {micro}m (h), and a photon flux of 4 x 10{sup 9} photons/sec/0.01%BW. Using a slit 44 meters upstream to create a virtual source, a circular beam spot of 0.15 {micro}m in diameter can be obtained with a photon flux of one order of magnitude less. During fluorescence mapping of trace elements in a single human ovarian cell, the microprobe exhibited an imaging sensitivity for Pt (L{sub a} line) of 80 attograms/{micro}m{sup 2} for a count rate of 10 counts per second. The x-ray microprobe has been used to map crystallographic strain and multiquantum well thickness in micro-optoelectronic devices produced with the selective area growth technique.

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A hard x-ray scanning microprobe for fluorescence imaging and microdiffraction at the Advanced Photon Source

Lithographic techniques for fabrication of hard X-ray Fresnel Zone Plates are discussed. Practical results achieved at the center for X-ray Lithography of the University of Wisconsin-Madison are presented. Fabrication technology includes replication of an e-beam written master mask into a thick photoresist by synchrotron radiation X-ray lithography, and subsequent electroplating of a metal zone plate structure using photoresist pattern as a mold.

Microfocusing optics for hard x-rays fabricated by x-ray lithography

Fresnel zone plates have been highly successful as focusing and imaging optics for soft x-ray microscopes and microprobe. More recently, with the advent of third-generation high-energy storage rings, zone plates for the hard x-ray regime have been put to use as well. The performance of zone plates manufactured using a combination of electron-beam lithography and x-ray lithography is described.

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B. Lai

Papers

A hard x-ray scanning microprobe for fluorescence imaging and microdiffraction at the advanced photon source

A hard x-ray scanning microprobe for fluorescence imaging and microdiffraction at the Advanced Photon Source

Microfocusing optics for hard x-rays fabricated by x-ray lithography

Performance of hard X-ray zone plates at the Advanced Photon Source