Despite the significance of surface absorbed proteins in determining the biological identity of nanoparticles (NPs) entering the human body, little is known about the surface corona and factors that shape their formation on dietary particles used as food additives. In this study, food grade NPs of silica and titania and their food additive counterparts (E551 and E171) were interacted with milk proteins or with skimmed milk and the levels of protein adsorption were quantified. Characteristics of proteins correlating with their level of adsorption to NPs were determined using partial least squares regression analysis.
View Article and Find Full Text PDFSolid-state C Nuclear Magnetic Resonance (NMR) and synchrotron-based X-ray Absorption Near-Edge Structure (XANES) have applications for determining the relative proportions of organic C functional groups in materials. Spectral data obtained by NMR is typically processed using integration (INTEG) whereas XANES spectral data is typically processed using deconvolution (DECONV). The objective of this study was to examine the impact of spectral data collection and processing on the estimated relative proportions of organic C functional groups in biochars.
View Article and Find Full Text PDFMine tailings exposed to water and oxygen generate acid mine drainage (AMD) when the neutralizing minerals are insufficient to buffer the acid produced by sulfide oxidation. Mineral reactivity, such as sulfide oxidation and carbonate dissolution, leads to several changes within mine tailings in terms of their physical, mineralogical, and geochemical properties, which may lead to the release of metal(oid)s (e.g.
View Article and Find Full Text PDFThe amine-rich surfaces of pyrolyzed human solid waste (py-HSW) can be "primed" or "regenerated" with carbon dioxide (CO) to enhance their adsorption of ammonia (NH) for use as a soil amendment. To better understand the mechanism by which CO exposure facilitates NH adsorption to py-HSW, we artificially enriched a model sorbent, pyrolyzed, oxidized wood (py-ox wood) with amine functional groups through exposure to NH. We then exposed these N-enriched materials to CO and then resorbed NH.
View Article and Find Full Text PDFVegetation fires are known to have broad geochemical effects on carbon (C) cycles in the Earth system, yet limited information is available for nitrogen (N). In this study, we evaluated how charring organic matter (OM) to pyrogenic OM (PyOM) altered the N molecular structure and affected subsequent C and N mineralization. Nitrogen near-edge X-ray absorption fine structure (NEXAFS) of uncharred OM, PyOM, PyOM toluene extract, and PyOM after toluene extraction were used to predict PyOM-C and -N mineralization potentials.
View Article and Find Full Text PDFManufactured Zn oxide nanoparticle (ZnO-NP) are extensively used world-wide in personal care and industrial products and are important contaminants of aquatic environments. To understand the overall impact of ZnO-NP contamination on aquatic ecosystems, investigation of their toxicity on aquatic biofilms is of particular consequence, given biofilms are known sinks for NP contaminants. In order to assess alterations in the functional activity of river microbial biofilm communities as a result of environmentally-relevant ZnO-NP exposure, biofilms were exposed to ionic zinc salt or ZnOPs that were uncoated (hydrophilic), coated with silane (hydrophobic) or stearic acid (lipophilic), at a total concentration of 188 μg l Zn.
View Article and Find Full Text PDFUsing Canadian (CMZ), Bear River (BRZ), and St. Cloud (SCZ) zeolites, this study investigates the application of natural and pre-treated zeolites for Na removal from salinised groundwater. Natural BRZ achieved better Na removal for initial concentrations of 250-10,000 mg Na/L and had the highest maximum adsorption capacity (14.
View Article and Find Full Text PDFAluminium (Al) K- and L-edge X-ray absorption near-edge structure (XANES) has been used to examine Al speciation in minerals but it remains unclear whether it is suitable for in situ analyses of Al speciation within plants. The XANES analyses for nine standard compounds and root tissues from soybean (Glycine max), buckwheat (Fagopyrum tataricum), and Arabidopsis (Arabidopsis thaliana) were conducted in situ. It was found that K-edge XANES is suitable for differentiating between tetrahedral coordination (peak of 1566 eV) and octahedral coordination (peak of 1568 to 1571 eV) Al, but not suitable for separating Al binding to some of the common physiologically relevant compounds in plant tissues.
View Article and Find Full Text PDFCerium oxide (CeO) nanoparticles are used as in-fuel catalysts and in manufacturing processes, creating a potential for release to aquatic environments. Exposures at 1 and 10 μg/L CeO-nanoparticles were made to assess effects during the development of river biofilm communities. Scanning transmission x-ray microscopy (STXM) indicated extensive sorption of nanoparticles to the community and co-localization with lipid moieties.
View Article and Find Full Text PDFPreserved labile tissues (e.g., skin, muscle) in the fossil record of terrestrial vertebrates are increasingly becoming recognized as an important source of biological and taphonomic information.
View Article and Find Full Text PDFSynergistic catalysis occurring in an enzyme pocket shows enhanced performance through supramolecular recognition and flexibility. This study presents an aerogel capable of similar function by fabricating a gel catalyst with hierarchical porosity. Here, the as-prepared Co-MMPG, a Co(II) metal-metalloporphyrin gel, maintains enough conformational flexibility and features a binding pocket formed from the co-facial arrangement of the porphyrin rings, as elucidated through the combined studies of solid-state NMR and X-ray absorption near-edge structure (XANES).
View Article and Find Full Text PDFFire-derived organic matter, often referred to as pyrogenic organic matter (PyOM), is present in the Earth's soil, sediment, atmosphere, and water. We investigated interactions of PyOM with ammonia (NH) gas, which makes up much of the Earth's reactive nitrogen (N) pool. Here we show that PyOM's NH retention capacity under ambient conditions can exceed 180 mg N g PyOM-carbon, resulting in a material with a higher N content than any unprocessed plant material and most animal manures.
View Article and Find Full Text PDFDirect evidence-based approaches are vital to evaluating newly proposed theories on the persistence of soil organic carbon and establishing the contributions of abiotic and biotic controls. Our primary goal was to directly identify the mechanisms of organic carbon stabilization in native-state, free soil microaggregates without disrupting the aggregate microstructure using scanning transmission x-ray microscopy coupled with near edge x-ray absorption fine structure spectroscopy (STXM-NEXAFS). The influence of soil management practices on microaggregate associated-carbon was also assessed.
View Article and Find Full Text PDFThis study focused on advancing the dual-adsorbent desalination technique that sequentially combines calcined layered double hydroxide (CLDH) and acid-treated zeolites (H-form zeolite) using groundwater spiked with potash mining effluent (brine). In sequential batch experiments, the CLDH adsorbent first reduced the high Cl concentration (4600 mg/L) of saline groundwater by 96%, the Ca by 90%, and the Mg by 92%, while transiently raising the pH to 12.80.
View Article and Find Full Text PDFThe efficiency with which renewable fuels and feedstocks are synthesized from electrical sources is limited at present by the sluggish oxygen evolution reaction (OER) in pH-neutral media. We took the view that generating transition-metal sites with high valence at low applied bias should improve the activity of neutral OER catalysts. Here, using density functional theory, we find that the formation energy of desired Ni sites is systematically modulated by incorporating judicious combinations of Co, Fe and non-metal P.
View Article and Find Full Text PDFManganese (Mn)-based antiperovskite structures (MnAX, where A and X represent the 3d transition-metal elements and N or C atoms, respectively) have attracted growing attention because of their novel electronic and magnetic properties. However, the lack of an effective approach to regulate the magnetic coupling in MnAX crystal structure, particularly in antiferromagnetic ground states, hinders their further design and applications. Herein, robust high-temperature ferrimagnetic order with a Curie temperature ( ) in the range of ~390-420 K was successfully achieved in ( , 0.
View Article and Find Full Text PDFThe emergence of multidrug resistance in bacteria has reached alarming levels. To solve this growing problem, discovery of novel cellular targets or pathways important for antimicrobial resistance is urgently needed. In this study, we explored how the alternative sigma factor, RpoE, protects Escherichia coli O157 against the toxic effects of the polycationic antimicrobial agent, chlorhexidine (CHX).
View Article and Find Full Text PDFIn wheat (), it is commonly assumed that Al is detoxified by the release of organic anions into the rhizosphere, but it is also possible that detoxification occurs within the apoplast and symplast of the root itself. Using Al-resistant (ET8) and Al-sensitive (ES8) near-isogenic lines of wheat, we utilized traditional and synchrotron-based approaches to provide analyses of the distribution and speciation of Al within root tissues. Some Al appeared to be complexed external to the root, in agreement with the common assumption.
View Article and Find Full Text PDFSci Total Environ
September 2017
The impact of saline mining effluent has been a significant environmental concern. Natural and modified clay-mineral adsorbents have been receiving increasing attention for salinity reduction of brine-impacted water, especially for natural resource extraction sites and surrounding environments. In this study, a dual-adsorbent treatment based on the sequential application of calcined layered double hydroxide (CLDH) and acid-treated zeolite was developed, evaluated and characterized for the desalination of potash brine-impacted groundwater.
View Article and Find Full Text PDFExposure of coal waste rock to atmospheric oxygen can result in the oxidation of sulfide minerals and the release of sulfate (SO) and associated trace elements (e.g., Se, As, Cd, and Zn) to groundwaters and surface waters.
View Article and Find Full Text PDFProc Natl Acad Sci U S A
January 2017
Uranium is an important carbon-free fuel source and environmental contaminant that accumulates in the tetravalent state, U(IV), in anoxic sediments, such as ore deposits, marine basins, and contaminated aquifers. However, little is known about the speciation of U(IV) in low-temperature geochemical environments, inhibiting the development of a conceptual model of U behavior. Until recently, U(IV) was assumed to exist predominantly as the sparingly soluble mineral uraninite (UO) in anoxic sediments; however, studies now show that this is not often the case.
View Article and Find Full Text PDFDiacetylene-bridged periodic mesoporous organosilicas (DAPMOs) with aggregates were synthesized and characterized. The DAPMO-based donor-acceptor charge-transfer (CT) system was prepared under ambient conditions, in which the diacetylenic groups in the pore walls were the electron donors and the decylviologen molecules acted as electron acceptors in the pore channels. The UV/Vis diffuse reflectance spectra and soft X-ray absorption near-edge structure (XANES) spectroscopy showed the formation of the CT complex.
View Article and Find Full Text PDFSelenium (Se) is an element of growing environmental concern, because low aqueous concentrations can lead to biomagnification through the aquatic food web. Biofilms, naturally occurring microbial consortia, play numerous important roles in the environment, especially in biogeochemical cycling of toxic elements in aquatic systems. The complexity of naturally forming multispecies biofilms presents challenges for characterization because conventional microscopic techniques require chemical and physical modifications of the sample.
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