Zoltan Imre Balogh

Characterization of Eyjafjallajökull volcanic ash particles and a protocol for rapid risk assessment

On April 14, 2010, when meltwaters from the Eyjafjallajökull glacier mixed with hot magma, an explosive eruption sent unusually fine-grained ash into the jet stream. It quickly dispersed over Europe. Previous airplane encounters with ash resulted in sandblasted windows and particles melted inside jet engines, causing them to fail. Therefore, air traffic was grounded for several days. Concerns also arose about health risks from fallout, because ash can transport acids as well as toxic compounds, such as fluoride, aluminum, and arsenic. Studies on ash are usually made on material collected far from the source, where it could have mixed with other atmospheric particles, or after exposure to water as rain or fog, which would alter surface composition. For this study, a unique set of dry ash samples was collected immediately after the explosive event and compared with fresh ash from a later, more typical eruption. Using nanotechniques, custom-designed for studying natural materials, we explored the physical and chemical nature of the ash to determine if fears about health and safety were justified and we developed a protocol that will serve for assessing risks during a future event. On single particles, we identified the composition of nanometer scale salt coatings and measured the mass of adsorbed salts with picogram resolution. The particles of explosive ash that reached Europe in the jet stream were especially sharp and abrasive over their entire size range, from submillimeter to tens of nanometers. Edges remained sharp even after a couple of weeks of abrasion in stirred water suspensions.

Creation of High Mobility Two-Dimensional Electron Gases via Strain Induced Polarization at an Otherwise Nonpolar Complex Oxide Interface

The discovery of two-dimensional electron gases (2DEGs) in SrTiO3-based heterostructures provides new opportunities for nanoelectronics. Herein, we create a new type of oxide 2DEG by the epitaxial-strain-induced polarization at an otherwise nonpolar perovskite-type interface of CaZrO3/SrTiO3. Remarkably, this heterointerface is atomically sharp and exhibits a high electron mobility exceeding 60,000 cm(2) V(-1) s(-1) at low temperatures. The 2DEG carrier density exhibits a critical dependence on the film thickness, in good agreement with the polarization induced 2DEG scheme.

Triple junction transport and the impact of grain boundary width in nanocrystalline Cu.

Triple junctions (TJ), singular topological defects of the grain boundary (GB) structure, get a dominant role for grain growth and atomic transport in nanocrystalline matter. Here, we present detailed measurements by atom probe tomography, even of the temperature dependence of TJ transport of Ni in nanocrystalline Cu in the chemical regime of interdiffusion. An unexpected variation of the effective width of merging GBs with temperature is detected. It is demonstrated that proper measurement of TJ transport requires taking into account this remarkable effect. TJ diffusion is found to be a factor of about 200 faster than GB diffusion. Its activation energy amounts to only two-thirds of that of the GB.

Mapping the evolution of hierarchical microstructures in a Ni-based superalloy

Phase separation of γ precipitates determines the microstructure and mechanical properties of nickel-based superalloys. In the course of ageing, disordered γ spheres form inside ordered (L12) γ precipitates, undergo a morphological change to plates and finally split the γ precipitates. The presence of γ particles inside γ affects coarsening kinetics and increases alloy hardness. Here we use atom probe tomography to visualize phase separation in a Ni86.1Al8.5Ti5.4 alloy in three dimensions and to quantify the composition of all the phases with near-atomic resolution. We find that γ precipitates are supersaturated in nickel, thereby driving the formation of γ particles and observe a compositional evolution of the γ particles, which accompanies their morphological change. Our results suggest that by controlling nickel supersaturation we can tailor the phase separation and thereby the properties of nickel-based superalloys.

Nano-analysis of grain boundary and triple junction transport in nanocrystalline Ni/Cu.

Nanocrystalline materials are distinguished by a high density of structural defects and grain boundaries. Due to the small grain size, a particular defect of the grain boundary topology, the so-called triple junction takes a dominant role for grain growth and atomic transport. We demonstrate by atom probe tomography that triple junctions in nanocrystalline Cu have 100-300 times higher diffusivity of Ni than standard high angle grain boundaries. Also, a previously unexpected systematic variation of the grain boundary width with temperature is detected. The impurity segregation layer at the grain boundaries grows from the 0.7 nm at 563 K to 2.5 nm at 643 K. This variation is clearly not controlled by simple bulk diffusion. Taking this effect into consideration, the activation energies for Ni diffusion in triple junctions and grain boundaries in Cu can be determined to be (83 ± 10) and (120 ± 15) kJ/mol, respectively. Thus, triple junctions are distinguished by considerably lower activation energy with respect to grain boundaries.

Stability of a Bifunctional Cu-Based Core@Zeolite Shell Catalyst for Dimethyl Ether Synthesis Under Redox Conditions Studied by Environmental Transmission Electron Microscopy and In Situ X-Ray Ptychography

When using bifunctional core@shell catalysts, the stability of both the shell and core-shell interface is crucial for catalytic applications. In the present study, we elucidate the stability of a CuO/ZnO/Al2O3@ZSM-5 core@shell material, used for one-stage synthesis of dimethyl ether from synthesis gas. The catalyst stability was studied in a hierarchical manner by complementary environmental transmission electron microscopy (ETEM), scanning electron microscopy (SEM) and in situ hard X-ray ptychography with a specially designed in situ cell. Both reductive activation and reoxidation were applied. The core-shell interface was found to be stable during reducing and oxidizing treatment at 250°C as observed by ETEM and in situ X-ray ptychography, although strong changes occurred in the core on a 10 nm scale due to the reduction of copper oxide to metallic copper particles. At 350°C, in situ X-ray ptychography indicated the occurrence of structural changes also on the µm scale, i.e. the core material and parts of the shell undergo restructuring. Nevertheless, the crucial core-shell interface required for full bifunctionality appeared to remain stable. This study demonstrates the potential of these correlative in situ microscopy techniques for hierarchically designed catalysts.

Evolution of nanoscale clusters in γ′ precipitates of a Ni–Al–Ti model alloy

The evolution of phase separation and ordering processes determines the structure and properties of Ni-based superalloys. Here we use atom probe tomography to clarify the origin of γ particles occurring in ordered (L12) γ precipitates in a Ni86.1Al8.5Ti5.4 alloy. Particularly, we elucidate the evolution from nanoscaled Ni-rich heterogeneities (Ni-rich clusters) to γ spheres and then γ plates inside γ precipitates from the compositional and the thermodynamic point of view. We find that Ni supersaturation of γ precipitates is relieved by formation of Ni-rich clusters, which results in an energetically more favorable state. Subsequently, coalescence introduces necking between the Ni-rich clusters and leads to the formation of γ particles. Our results demonstrate that phase separation of γ precipitates is characterized by different stages with various governing driving forces.

Defect analysis by statistical fitting to 3D atomicmaps

In this article we present a statistical fitting method for evaluation of atomic reconstructions which does not require a coarse-graining step. The fitting compares different models of chemical structure in their capability to explain the measured data set by a least square type merit function. Only preliminary qualitative assumptions about the possible chemical structure are required, while accurate quantitative parameters of the chosen model are delivered by fitting. The technique is particularly useful for singular defect structures with very high composition gradients, for which iso-concentration surfaces determined by coarse-graining become questionable or impossible. We demonstrate that particularly detailed information can be gained from triple junctions and grain boundaries.

Reactive nanoparticles in chalk: Implications for sequestration of metals from groundwater

Abstract Water supplies from chalk aquifers in northern Europe can be contaminated by semi-metals such as As and metals such as Cr, Ni and many more, as a result of leaks from landfills, industrial sites and from natural oxidation of pyrite in the chalk, releasing trace elements. Chalk, which is predominantly calcite (CaCO3), has the ability to immobilize Ni, but its uptake by chalk is sometimes greater than expected. In an attempt to identify the controls on metal uptake, chalk samples from Klintholm I/S (Fyn, Denmark) were decalcified in EDTA solution and the residue was examined with transmission electron microscopy (TEM) for morphology and composition. Energy dispersive X-ray spectrometry (EDXS) revealed minor Si and Al (probably clay) and major Mn and Fe as (hydr)oxides. These natural nanoparticles have very large surface areas contributing to chalk’s uptake capacity for Ni and other metals from groundwater.

More oil from Chalk: Studying the holes - and the borders of the holes, the particle interfaces

General information State: Published Organisations: Theoretical Atomic-scale Physics, Department of Physics Contributors: Stipp, S. L. S., West, K., Dideriksen, K., Lakshtanov, L., Yang, M. J., Bohr, J., Belova, D., Pasarin, I. S., Johnson, A., Pedersen, C. S., Balogh, Z., Nissenbaum, J., Wang, X. Z., Jensen, T. H., Feidenhansl, R., Engstrøm, F., Bechgaard, K., Bjørnholm, T. Publication date: 2008