4 Material und Umwelt
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Paper des Monats
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The present work demonstrates a sustainable approach of using relatively coarser iron ore particles for ironmaking. The motivation is to reduce the energy consumption in the milling of the iron ore by utilizing coarser iron ore particles (+0.05 mm) and to select a suitable binder for improving pellet properties. Iron ore fines in the range of 0.05–0.25 mm was selected and classified into three size ranges. Fluxed iron ore pellets were prepared using lime as a binder for the basicity of 0, 1, and 2. Reduction of these pellets with a packed bed of coal fines was performed in the temperature range of 900–1200 °C for a duration of 30–120 min. The direct reduction kinetics of the iron ore pellets were studied by employing diffusion and chemical reaction control models to the experimental data. The results show that pellets made with coarser iron ore particles have improved reduction behavior and kinetics. The reduction reaction is found to be a mixed control. The activation energy for the reduction reaction varies from 44.3 to 74.76 kJ mol−1 as iron ore particle size decreases from 0.25 to 0.05 mm and basicity increases from 0 to 2.
AbstractRed mud is the waste of bauxite refinement into alumina, the feedstock for aluminium production1. With about 180 million tonnes produced per year1, red mud has amassed to one of the largest environmentally hazardous waste products, with the staggering amount of 4 billion tonnes accumulated on a global scale1. Here we present how this red mud can be turned into valuable and sustainable feedstock for ironmaking using fossil-free hydrogen-plasma-based reduction, thus mitigating a part of the steel-related carbon dioxide emissions by making it available for the production of several hundred million tonnes of green steel. The process proceeds through rapid liquid-state reduction, chemical partitioning, as well as density-driven and viscosity-driven separation between metal and oxides. We show the underlying chemical reactions, pH-neutralization processes and phase transformations during this surprisingly simple and fast reduction method. The approach establishes a sustainable toxic-waste treatment from aluminium production through using red mud as feedstock to mitigate greenhouse gas emissions from steelmaking.
Microbially induced carbonate precipitation (MICP), a widespread phenomenon in nature, is gaining attention as a low-carbon alternative to ordinary Portland cement (OPC) in geotechnical engineering and the construction industry for sustainable development. In the Philippines, however, very few works have been conducted to isolate and identify indigenous, urease-producing (ureolytic) bacteria suitable for MICP. In this study, we isolated seven, ureolytic and potentially useful bacteria for MICP from marine sediments in Iligan City. DNA barcoding using 16s rDNA identified six of them as Pseudomonas stutzeri, Pseudomonas pseudoalcaligenes, Bacillus paralicheniformis, Bacillus altitudinis, Bacillus aryabhattai, and Stutzerimonas stutzeri but the seventh was not identified since it was a bacterial consortium. Bio-cementation assay experiments showed negligible precipitation in the control (without bacteria) at pH 7, 8, and 9. However, precipitates were formed in all seven bacterial isolates, especially between pH 7 and 8 (0.7–4 g). Among the six identified bacterial species, more extensive precipitation (2.3–4 g) and higher final pH were observed in S. stutzeri, and B. aryabhattai, which indicate better urease production and decomposition, higher CO2 generation, and more favorable CaCO3 formation. Characterization of the precipitates by scanning electron microscopy with energy dispersive X-ray spectroscopy (SEM-EDS) and attenuated total reflectance Fourier transform spectroscopy (ATR-FTIR) confirmed the formation of three carbonate minerals: calcite, aragonite, and vaterite. Based on these results, all six identified indigenous, ureolytic bacterial species from Iligan City are suitable for MICP provided that the pH is controlled between 7 and 8. To the best of our knowledge, this is the first report of the urease-producing ability and potential for MICP of P. stutzeri, P. pseudoalcaligenes, S. stutzeri, and B. aryabhattai.
Maintaining and modulating mechanical anisotropy is essential for biological processes. However, how this is achieved at the microscopic scale in living soft matter is not always clear. Although Brillouin light scattering (BLS) spectroscopy can probe the mechanical properties of materials, spatiotemporal mapping of mechanical anisotropies in living matter with BLS microscopy has been complicated by the need for sequential measurements with tilted excitation and detection angles. Here we introduce Brillouin light scattering anisotropy microscopy (BLAM) for mapping high-frequency viscoelastic anisotropy inside living cells. BLAM employs a radial virtually imaged phased array that enables the collection of angle-resolved dispersion in a single shot, thus enabling us to probe phonon modes in living matter along different directions simultaneously. We demonstrate a precision of 10 MHz in the determination of the Brillouin frequency shift, at a spatial resolution of 2 µm. Following proof-of-principle experiments on muscle myofibres, we apply BLAM to the study of two fundamental biological processes. In plant cell walls, we observe a switch from anisotropic to isotropic wall properties that may lead to asymmetric growth. In mammalian cell nuclei, we uncover a spatiotemporally oscillating elastic anisotropy correlated to chromatin condensation. Our results highlight the role that high-frequency mechanics can play in the regulation of diverse fundamental processes in biological systems. We expect BLAM to find diverse applications in biomedical imaging and material characterization.
Here, we show that calcium sulfate dihydrate (gypsum) can be directly, rapidly and reversibly converted to calcium sulfate hemihydrate (bassanite) in high salinity solutions (brines). The optimum conditions for the efficient production of bassanite in a short time (<5 min) involve the use of brines with c(NaCl) > 4 M and maintaining a temperature, T > 80 °C. When the solution containing bassanite crystals is cooled down to around room temperature, eventually gypsum is formed. When the temperature is raised again to T > 80 °C, bassanite is rapidly re-precipitated. This contrasts with the better-known behaviour of the bassanite phase in low-salt environments. In low-salinity aqueous solutions, bassanite is considered to be metastable with respect to gypsum and anhydrite, and therefore gypsum-to-bassanite conversion does not occur in pure water. Interestingly, the high-salinity transformation of gypsum-to-bassanite has been reported by many authors and used in practice for several decades, although its very occurrence actually contradicts numerical thermodynamic predictions regarding solubility of calcium sulfate phases. By following the evolution of crystalline phases with in situ and time-resolved X-ray diffraction/scattering and Raman spectroscopy, we demonstrated that the phase stability in brines at elevated temperatures was inaccurately represented in the thermodynamic databases. Most notably for c(NaCl) > 4 M, and T > 80 °C gypsum becomes readily more soluble than bassanite, which induces the direct precipitation of the latter from gypsum. The fact that these transformations are controlled by the solution provides extensive opportunities for precise manipulation of crystal formation. Our experiments confirmed that bassanite remained the sole crystalline phase for many hours before reverting into gypsum. This property is extremely advantageous for practical processing and efficient crystal extraction in industrial scenarios.
Reliable measurement of the size of polydisperse, complex-shaped commercial nanopowders is a difficult but necessary task, e.g., for regulatory requirements and toxicity risk assessment. Suitable methods exist for the accurate characterization of the size of non-aggregated, stabilized, spherical and monodisperse nanoparticles. In contrast, industrial nanoscale powders usually require dedicated sample preparation procedures developed for the analysis method of choice. These nano-powders tend to agglomerate and/or aggregate, a behavior which in combination with an innate broad particle size distribution and irregular shape often significantly alters the achievable accuracy of the measured size parameters. The present study systematically tests two commercially available nanoscale powders using different sample preparation methods for correlative analysis by scanning electron microscopy, dynamic light scattering, Brunauer–Emmet–Teller method and differential mobility analysis. One focus was set on the sample preparation by embedding nanoparticles in carbon-based hot-mounting resin. Literature on this topic is scarce and the accuracy of the data extracted from cross sections of these particles is unclearly stated. In this paper systematic simulations on the deviation of the size parameters of well-defined series of nanoparticles with different shapes from the nominal value were carried out and the contributing factors are discussed.
Fused cement clinker can be produced from molten basic oxygen furnace slag (BOFS) by way of a reductive thermochemical treatment. During the thermochemical treatment, oxidic iron is reduced to metallic iron and separated. The resulting low-iron slag has a chemical and mineralogical composition similar to ordinary Portland cement (OPC) clinker. In this study, the hydraulic reactivity of the fused clinker from BOFS with and without gypsum was investigated using isothermal calorimetry, differential scanning calorimetry, in situ X-ray diffraction and powder X-ray diffraction. Furthermore, a synthetic fused clinker without foreign ions and fused clinker produced by a mixture of both materials was studied. The hydraulic reaction of the fused clinker from BOFS was considerably slower than that of OPC. However, the reaction can be accelerated by adding gypsum as a sulfate carrier. Furthermore, the results showed an increased reaction rate with decreasing content of foreign ions such as Fe, P or Mn.
Re-melting of scrap in an electric arc furnace (EAF) results in the accumulation of filter dust from off-gas treatment that predominantly consists of iron and zinc oxides. Filter dust is classified as hazardous waste due to its high contents of potentially toxic or ecotoxic elements such as Pb, Cr, Cd, and As. A promising processing route for this waste is selective chlorination, in which the non-ferrous metal oxides are chlorinated and selectively evaporated in form of their respective chlorides from the remaining solids via the process gas flow. Here, we investigate stepwise thermochemical treatment of EAF dust with either waste iron(II) chloride solution or hydrochloric acid at 650, 800, and 1100 ◦C. The Zn and Pb contents of the thermochemically processed EAF dust could be lowered from 29.9% and 1.63% to 0.09% and 0.004%, respectively. Stepwise heating allowed high separation between zinc chloride at the 650 ◦C step and sodium-, potassium-, and lead-containing chlorides at higher temperatures. Furthermore, the lab-scale results were transferred to the use of an experimental rotary kiln highlighting the possibilities of upscaling the presented process. Selective chlorination of EAF dust with liquid chlorine donors is, therefore, suggested as a potential recycling method for Zn-enriched steelworks dusts.
Understanding Stimulation of Conjugal Gene Transfer by Nonantibiotic Compounds: How Far Are We?
(2024)
A myriad of nonantibiotic compounds is released into the environment, some of which may contribute to the dissemination of antimicrobial resistance by stimulating conjugation. Here, we analyzed a collection of studies to (i) identify patterns of transfer stimulation across groups and concentrations of chemicals, (ii) evaluate the strength of evidence for the proposed mechanisms behind conjugal stimulation, and (iii) examine the plausibility of alternative mechanisms. We show that stimulatory nonantibiotic compounds act at concentrations from 1/1000 to 1/10 of the minimal inhibitory concentration for the donor strain but that stimulation is always modest (less than 8-fold). The main proposed mechanisms for stimulation via the reactive oxygen species/SOS cascade and/or an increase in cell membrane permeability are not unequivocally supported by the literature. However, we identify the reactive oxygen species/SOS cascade as the most likely mechanism. This remains to be confirmed by firm molecular evidence. Such evidence and more standardized and high-throughput conjugation assays are needed to create technologies and solutions to limit the stimulation of conjugal gene transfer and contribute to mitigating global antibiotic resistance.
In this study, we investigated the diverse range of materials used for sizing in Iranian paper manuscripts during the Timurid (fifteenth century) to Safavid (sixteenth century) and Qajar (nineteenth century) periods. Our approach combined historical analysis with scientific examination of reconstructed sizings. We reconstructed 15 sizing materials based on identified Persian historical recipes and analysed their physical, optical, and spectral characteristics. Additionally, we assessed their behaviour against the mould fungus Aspergillus flavus. The results revealed distinctive properties for each sizing material, shedding light on their potential applications in paper preservation. Furthermore, our investigation demonstrated variations in hygroscopicity, thickness, grammage, and ash content post-sizing. The sizing materials also exhibited different effects on paper reflectance properties. Additionally, our study revealed insights into the impact of sizing on burnished papers, indicating that the mechanical process of burnishing did not significantly alter the chemical composition or spectral properties of the paper, with only minor changes in brightness observed in specific cases. All tested sizing materials supported varying levels of mould growth, indicating potential implications for paper conservation. Our findings provide valuable insights into the historical practices of Iranian paper sizing and offer practical considerations for the preservation of paper manuscripts.
The emission of ultrafine particles from small desktop Fused Filament Fabrication (FFF) 3D printers has been frequently investigated in the past years. However, the vast majority of FFF emission and exposure studies have not considered the possible occurrence of particles below the typical detection limit of Condensation Particle Counters and could have systematically underestimated the total particle emission as well as the related exposure risks. Therefore, we comparatively measured particle number concentrations and size distributions of sub-4 nm particles with two commercially available diethylene glycol-based instruments – the TSI 3757 Nano Enhancer and the Airmodus A10 Particle Size Magnifier. Both instruments were evaluated for their suitability of measuring FFF-3D printing emissions in the sub-4 nm size range while operated as a particle counter or as a particle size spectrometer. For particle counting, both instruments match best when the Airmodus system was adjusted to a cut-off of 1.5 nm. For size spectroscopy, both instruments show limitations due to either the fast dynamics or rather low levels of particle emissions from FFF-3D printing in this range. The effects are discussed in detail in this article. The findings could be used to implement sub-4 nm particle measurement in future emission or exposure studies, but also for the development of standard test protocols for FFF-3D printing emissions.
The biogenesis of iron–sulfur (Fe/S) proteins entails the synthesis and trafficking of Fe/S clusters, followed by their insertion into target apoproteins. In eukaryotes, the multiple steps of biogenesis are accomplished by complex protein machineries in both mitochondria and cytosol. The underlying biochemical pathways have been elucidated over the past decades, yet the mechanisms of cytosolic [2Fe-2S] protein assembly have remained ill-defined. Similarly, the precise site of glutathione (GSH) requirement in cytosolic and nuclear Fe/S protein biogenesis is unclear, as is the molecular role of the GSH-dependent cytosolic monothiol glutaredoxins (cGrxs). Here, we investigated these questions in human and yeast cells by various in vivo approaches. [2Fe-2S] cluster assembly of cytosolic target apoproteins required the mitochondrial ISC machinery, the mitochondrial transporter Atm1/ABCB7 and GSH, yet occurred independently of both the CIA system and cGrxs. This mechanism was strikingly different from the ISC-, Atm1/ABCB7-, GSH-, and CIA-dependent assembly of cytosolic–nuclear [4Fe-4S] proteins. One notable exception to this cytosolic [2Fe-2S] protein maturation pathway defined here was yeast Apd1 which used the CIA system via binding to the CIA targeting complex through its C-terminal tryptophan. cGrxs, although attributed as [2Fe-2S] cluster chaperones or trafficking proteins, were not essential in vivo for delivering [2Fe-2S] clusters to either CIA components or target apoproteins. Finally, the most critical GSH requirement was assigned to Atm1-dependent export, i.e. a step before GSH-dependent cGrxs function. Our findings extend the general model of eukaryotic Fe/S protein biogenesis by adding the molecular requirements for cytosolic [2Fe-2S] protein maturation.
Here, we report a comparative study of different sum parameter analysis methods for the extraction of per- and polyfluoroalkyl substances (PFAS) from manufactured consumer products, which can be measured by combustion ion chromatography (CIC). Therefore, a hydrolysis-based extraction method was further developed, which accounts for the addition of hydrolyzable covalently bound polyfluoroalkylated side-chain polymers (SFPs) to the extractable organic fluorine portion of the mass balance proposed as "hydrolyzable organically bound fluorine" (HOF). To test this hypothesis, the method was applied to 39 different consumer products containing fluoropolymers or monomeric PFAS taken from four different categories: outdoor textiles, paper packaging, carpeting, and permanent baking sheets. We also evaluated the method's efficiency by extracting four synthesized fluorotelomer polyacrylate reference compounds. The total fluorine (TF) and extractable organically bound fluorine (EOF) values were measured through CIC using established protocols. The TF values ranged from sub-ppb to %-levels, depending on the compound class. All samples showed results for hydrolyzed organofluorine (HOF) between 0.03 and 76.3 μg/g, while most EOF values were lower (<LOD to 58.1 μg/g). Moreover, the methods were contrasted with the "total hydrolyzable precursor" (THP) assay analyzed using gas-chromatography coupled mass spectrometry (GC-MS), which yielded concentrations of 6:2–10:2 fluorotelomer alcohols (<LOD-568 μg/g) for textile and paper samples. Furthermore, targeted analytical investigation of 25 compounds via liquid chromatography coupled tandem mass spectrometry (LC-MS/MS) was conducted and accounted for significantly lower sum amounts (<LOD-0.98 μg PFAS/g). To estimate the fluorine mass balance of all methods, the fluorine levels of target analytical data were calculated and compared to the sum parameter values and evaluated. Finally, the efficiency of the extraction method was approximated by the recovery analysis of four selected SFP model compounds compared to their TF values, yielding 36.7–74.0% after extraction and 3.8–36.3% after processing the extract for the HOF sum parameter.
The use of ashes from municipal solid waste incineration as secondary building materials is an important pillar for the circular economy in Germany. However, leaching of potential toxic elements from these materials must be at environmentally acceptable levels. Normally, a three-month ageing period immobilizes most hazardous heavy metals, but antimony (Sb) and vanadium (V) showed previously unusual leaching. In order to clarify the mechanisms, we analyzed the Sb and V species in various bottom and fly ashes from municipal waste incineration by XANES spectroscopy. Antimony oxidizes from Sb(+ III) species used as flame retardants in plastics to Sb(+ V) compounds during waste incineration. However, owing to the similarity of different Sb(+ V) compound in the Sb K- and L-edge XANES spectra, it was not possible to accurately identify an exact Sb(+ V) species. Moreover, V is mainly present as oxidation state + V compound in the analyzed ashes. However, the coarse and magnetic fraction of the bottom ashes contain larger amounts of V(+ III) and V(+ IV) compounds which might enter the waste incineration from vanadium carbide containing steel tools. Thus, Sb and V could be critical potential toxic elements in secondary building materials and long-term monitoring of the release should be taken into account in the future.
Investigation on the Durability of a Polypropylene Geotextile under Artificial Aging Scenarios
(2024)
Geosynthetics are widely used in various civil engineering applications, such as geotextiles in coastal protection, and display a sustainable alternative to natural mineral materials. However, the full benefits of using geosynthetics can only be gained with a long service lifetime of the products. With the use of added stabilizers to the polymers, service lifetimes can be achieved in the range of 100 years. Therefore, accelerated aging methods are needed for the assessment of the long-term performance of geotextiles. In the present study, the behavior of geosynthetic materials made of polypropylene was investigated under artificial aging conditions involving elevated temperatures ranging from 30 to 80 °C, increased oxygen pressures ranging from 10 to 50 bar in water-filled autoclaves, and UV irradiation under atmospheric conditions. ATR-IR spectroscopy was employed to detect the increase in the carbonyl index over various aging durations, indicating the oxidative degradation of the geotextile. The most pronounced increase was observed in the case of aging through UV irradiation, followed by thermal aging. Elevated pressure, on the other hand, had a lower impact on oxidation. High-temperature size exclusion chromatography was utilized to follow the reduction in molar mass under different degradation conditions, and the results were consistent with those obtained from ATR-IR spectroscopy. In polyolefins such as polypropylene, Hindered Amine Stabilizers (HAS) are used to suppress oxidation caused by UV radiation. The quantitative analysis of HAS was carried out using a UV/Vis method and HPLC. The degradation of UV stabilizers during the aging of geotextiles is responsible for the oxidation and the reduction in the molar mass of polypropylene. From the results, it can be concluded that applications of PP geotextile without soil or sand cover might cause the risk of the formation of microplastic particles. Material selection, design, and maintenance of the construction must follow best practices, including the system’s removal or replacement at end-of-life. Otherwise, a sustainable use of geotextiles in civil engineering is not possible.