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Palaeoecological evidence for sustained change in a shallow Murray River (Australia) floodplain lake: regime shift or press response
No full textPaleolimnological techniques can reveal long-term perturbations and associated stable state transitions of lake ecosystems. However, such transitions are difficult to predict since changes to lake ecosystems can be abrupt or gradual. This study examined whether there were past transitions in the ecological regime of Kings Billabong, a shallow River Murray wetland in southeast Australia. A 94-cm-long core, covering c. 90 years of age, was analysed at 1 cm resolution for subfossil cladocerans, diatoms and other proxies. Prior to river regulation (c. 1930), the littoral to planktonic ratios of cladocerans and diatoms, and bulk sediment δ13C values were high, while the period from c. 1930 to c. 1970 experienced considerable changes to the wetland ecosystem. The abrupt nature of changes of planktonic cladocerans and diatoms, particularly after the onset of river regulation (1930s), was triggered by inundation, high rates of sedimentation and shifts in bulk sediment δ15N values. However, the transition of a once littoral-dominated community, to one favouring an increasingly turbid, plankton-dominated trophic condition following river regulation was relatively slow and lasted for decades. The progression to a new regime was likely delayed by the partial recovery of submerged plant communities and related internal dynamics.© 2016, Springer International Publishing Switzerland
Plasma Polymer-Functionalized Silica Particles for Heavy Metals Removal.
No full textHighly negatively charged particles were fabricated via an innovative plasma-assisted approach for the removal of heavy metal ions. Thiophene plasma polymerization was used to deposit sulfur-rich films onto silica particles followed by the introduction of oxidized sulfur functionalities, such as sulfonate and sulfonic acid, via water–plasma treatments. Surface chemistry analyses were conducted by X-ray photoelectron spectroscopy and time-of-flight secondary ion mass spectroscopy. Electrokinetic measurements quantified the zeta potentials and isoelectric points (IEPs) of modified particles and indicated significant decreases of zeta potentials and IEPs upon plasma modification of particles. Plasma polymerized thiophene-coated particles treated with water plasma for 10 min exhibited an IEP of less than 3.5. The effectiveness of developed surfaces in the adsorption of heavy metal ions was demonstrated through copper (Cu) and zinc (Zn) removal experiments. The removal of metal ions was examined through changing initial pH of solution, removal time, and mass of particles. Increasing the water plasma treatment time to 20 min significantly increased the metal removal efficiency (MRE) of modified particles, whereas further increasing the plasma treatment time reduced the MRE due to the influence of an ablation mechanism. The developed particulate surfaces were capable of removing more than 96.7% of both Cu and Zn ions in 1 h. The combination of plasma polymerization and oxidative plasma treatment is an effective method for the fabrication of new adsorbents for the removal of heavy metals. © 2015 American Chemical Societ
Development of negatively charged particulate surfaces through a dry plasma-assisted approach
No full textA dry two-step plasma process is introduced for the fabrication of particulate surfaces showing negative charges over a wide range of pH. Plasma polymerized thiophene (PPT) was initially deposited onto silica particles using an inductively coupled plasma polymerization reactor fitted with a rotating barrel. Sulfur-functionalized particles were further chemically modified through an oxidative air or water plasma treatment. Wide ranges of plasma specific energies (0.06–2.4 kJ cm−3) and treatment times (5–60 minutes) were employed to manipulate the surface chemistry, hydrophobicity and surface charge of the silica particles. Surface chemistry of the modified silica particles was studied using X-ray photoelectron spectroscopy (XPS) and time of flight secondary ion mass spectroscopy (ToF-SIMS). Changes in hydrophobicity and surface charge of the modified particles were quantified via Washburn capillary rise measurements and electrokinetic analysis, respectively. Plasma treatment of PPT coated particles resulted in homogenous formation of –SOx(H) functionalities such as sulfonate (SO3−), sulfonic acid (SO3H), and sulfate (SO42−) on surfaces. Such changes in surface chemistry significantly decreased the zeta potential and isoelectric point of the particles as well as their degree of hydrophobicity. In comparison to air plasma, water plasma was found to be a better candidate for the treatment of PPT coated particles as it produced surfaces with lower zeta potentials and isoelectric points. Our introduced solvent-free approach is applicable for the modification of almost any other particles regardless of their shape and surface chemistry. Such surface engineered particles could be utilized as protein detectors/adsorbents, solid-state catalysts, and heavy metal removal agents. © Royal Society of Chemistry 201
Synthesis of titanium dioxide nanoparticles: phase, morphology and size control
No full textTitanium dioxide is a well-studied and popular photocatalyst, but a number of factors still prevent its widespread use in a number of commercial applications. In this thesis we explored the synthesis of titanium dioxide nanoparticles via the sol-gel method, with the goal of creating a viable catalyst for the visible-light degradation of wastewater dyes. A number of different synthetic pathways were explored and developed, and the products categorised with respect to nanoparticle size, shape and crystallinity as well as electronic and photocatalytic properties
Characterization of complex carbide–silicide precipitates in a Ni–Cr–Mo–Fe–Si alloy modified by welding
No full textNickel based alloys of the type Hastelloy-N™ are ideal candidate materials for molten salt reactors, as well as for applications such as pressure vessels, due to their excellent resistance to creep, oxidation and corrosion. In this work, the authors have attempted to understand the effects of welding on the morphology, chemistry and crystal structure of the precipitates in the heat affected zone (HAZ) and the weld zone of a Ni–Cr–Mo–Fe–Si alloy similar to Hastelloy-N™ in composition, by using characterization techniques such as scanning and transmission electron microscopy. Two plates of a Ni–Cr–Mo–Fe–Si alloy GH-3535 were welded together using a TiG welding process without filler material to achieve a joint with a curved molten zone with dendritic structure. It is evident that the primary precipitates have melted in the HAZ and re-solidified in a eutectic-like morphology, with a chemistry and crystal structure only slightly different from the pre-existing precipitates, while the surrounding matrix grains remained unmelted, except for the zones immediately adjacent to the precipitates. In the molten zone, the primary precipitates were fully melted and dissolved in the matrix, and there was enrichment of Mo and Si in the dendrite boundaries after solidification, and re-precipitation of the complex carbides/silicides at some grain boundaries and triple points. The nature of the precipitates in the molten zone varied according to the local chemical composition.© 2015, Elsevier Inc
Quantifying the influences of atmospheric stability on air pollution in Lanzhou, China, using a radon-based stability monitor
No full textCommercially-available “stability monitors” based on in situ atmospheric radon progeny measurements remain underutilised as a tool for urban pollution studies, due in part to difficulties experienced in relating their standard output directly to the atmospheric mixing state in a consistent manner. The main confounding factor has been a lack of attention to the fact that the observed near-surface atmospheric radon concentration includes large synoptic and fetch-related components in addition to the local stability influence. Here, a technique recently developed for stability classification using a research-quality dual-flow-loop two-filter radon detector is adapted for use with a commercially-available radon-based stability monitor. Performance of the classification scheme is then tested in Lanzhou, China, a topographically-complex region renowned for low mean annual wind speeds (0.8 m s−1) and winter stagnation episodes. Based on an 11-month composite, a factor of seven difference is estimated between peak NOx concentrations in the city's industrial region and a rural background location under stable conditions. The radon-based scheme is evaluated against the Pasquil-Gifford “radiation” (PGR) scheme, and assigns pollutant concentrations more consistently between defined atmospheric stability states than the PGR scheme. Furthermore, the PGR scheme consistently underestimates all peak pollutant concentrations under stable conditions compared with the radon-based scheme, in some cases (e.g. CO in the industrial region) by 25%. © 2015, Elsevier Ltd
Temperature- and pH-Responsive Micelles with Collapsible Poly(N-isopropylacrylamide) Headgroups
No full textWe have studied the micelle formation and phase behavior of a series of temperature- and pH-responsive surfactants prepared by controlled radical (RAFT) polymerization. These C12NIPAMm surfactants consist of a dodecyl tail, a poly(N-isopropylacrylamide) (polyNIPAM) headgroup with average degrees of polymerization of between 7 and 96, and an ionizable carboxylate group. In the un-ionized state, these surfactants phase separate on warming toward a lower critical solution temperature (LCST), which decreases as the length of the NIPAM group is decreased. This is in agreement with the behavior of conventional nonionic poly(ethylene oxide)-based surfactants but is very different from that of polyNIPAM oligomer solutions. Small angle neutron scattering (SANS) shows that these surfactants self-assemble into micelles consisting of a nearly spherical hydrophobic core surrounded by a “hairy” polyNIPAM shell far below their LCST. Upon warming, the micelles undergo a sphere-to-rod transition induced by the collapse of the polyNIPAM shell, causing a reduction in the headgroup area. In the un-ionized state the demixing follows at the LCST, but a single charge on the free polymer end completely suppresses phase separation, allowing micelles to undergo a shape change but remain dissolved. © 2014, American Chemical Society
Hydrogen accommodation in αα-iron and nickel
No full textAb initio calculations have been used to study the effects of hydrogen on vacancy concentrations in αα-Fe and Ni. The presence of H interstitials aided vacancy formation in both metals but via two different mechanisms. In αα-Fe, trapping of H by a vacancy is favourable. However binding of further hydrogen atoms was not predicted to proceed. The thermal equilibrium concentration of H interstitials in comparison to vacancies in αα-Fe is many orders of magnitude higher over a wide temperature range. Excessive H interstitials in solid solution facilitate vacancy formation, lowering the required energy by 0.79 eV (down to 1.41 eV). In Ni, a single H interstitial is not expected to have an impact on the vacancy population, increasing the vacancy formation energy by 0.32 eV. Two bound H interstitials however are predicted to decrease the vacancy formation energy by 0.52 eV with expected arrangement along a 〈〈1 1 1〉〉 direction around the vacancy. The calculations show reasonable agreement with experimental data when comparing crystal lattice contractions of the pure metals and predicted melting temperature of the Me–H alloys. © 2013, Elsevier B.V
10Be in late deglacial climate simulated by ECHAM5-HAM – Part 2: Isolating the solar signal from 10Be deposition
Get PDFThis study investigates the effect of deglacial climate on the deposition of the solar proxy 10Be globally, and at two specific locations, the GRIP site at Summit, Central Greenland, and the Law Dome site in coastal Antarctica. The deglacial climate is represented by three 30 year time slice simulations of 10 000 BP (years before present = 1950 CE), 11 000 and 12 000 BP, compared with a preindustrial control simulation. The model used is the ECHAM5-HAM atmospheric aerosol–climate model, driven with sea-surface temperatures and sea ice cover simulated using the CSIRO Mk3L coupled climate system model. The focus is on isolating the 10Be production signal, driven by solar variability, from the weather- or climate-driven noise in the 10Be deposition flux during different stages of climate. The production signal varies at lower frequencies, dominated by the 11 year solar cycle within the 30 year timescale of these experiments. The climatic noise is of higher frequencies than 11 years during the 30 year period studied. We first apply empirical orthogonal function (EOF) analysis to global 10Be deposition on the annual scale and find that the first principal component, consisting of the spatial pattern of mean 10Be deposition and the temporally varying solar signal, explains 64% of the variability. The following principal components are closely related to those of precipitation. Then, we apply ensemble empirical decomposition (EEMD) analysis to the time series of 10Be deposition at GRIP and at Law Dome, which is an effective method for adaptively decomposing the time series into different frequency components. The low-frequency components and the long-term trend represent production and have reduced noise compared to the entire frequency spectrum of the deposition. The high-frequency components represent climate-driven noise related to the seasonal cycle of e.g. precipitation and are closely connected to high frequencies of precipitation. These results firstly show that the 10Be atmospheric production signal is preserved in the deposition flux to surface even during climates very different from today's both in global data and at two specific locations. Secondly, noise can be effectively reduced from 10Be deposition data by simply applying the EOF analysis in the case of a reasonably large number of available data sets, or by decomposing the individual data sets to filter out high-frequency fluctuations. © Author(s) 2014
Domination of second-sphere shrinkage effect to improve photoluminescence of red nitride phosphors
No full textRed Ca0.99Al1–4δ/3–xSi1+δ+xN3–xCx:Eu2+0.01 (δ = 0.345; x = 0–0.2) nitride phosphors exhibit a blue-shifted emission with increased eye sensitivity function and excellent thermal stability. The variations in the photoluminescence in the Ca0.99Al1–4δ/3–xSi1+δ+xN3–xCx:Eu2+0.01 (δ = 0.345; x = 0–0.2) system are thoroughly investigated. The enhanced emission energy and the improved thermal stability with increasing x are dominated by the second-sphere shrinkage effect via the substitution of small Si4+ for large Al3+ with simultaneous charge compensation. Related proofs of the second-sphere shrinkage effect control for photoluminescence are confirmed via high-resolution neutron powder diffraction, EXAFS, and 29Si solid-state NMR techniques. © 2014, American Chemical Society