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Stainless steel AISI 304 surfaces were studied after a mild anodic polarization for oxide growth in the presence and absence of two derivatives of vitamin B2 (riboflavin and flavin mononucleotide) that can be secreted by metal‐reducing bacteria and act as a chelating agent for iron species. The alterations in oxide chemistry were studied by means of surface‐sensitive techniques such as X‐ray photoelectron spectroscopy and time‐of‐flight secondary ion mass spectrometry analysis. The complementary electrochemical characterization revealed a preferential growth of an oxide/hydroxide iron‐rich film that is responsible for an altered pit initiation and nucleation behavior. These findings suggest that as the corrosion behavior is determined by the interplay of the chemical and electronic properties, only a mild anodic polarization in the presence of redox‐active molecules is able to alter the chemical and electronic structure of the passive film formed on stainless steel AISI 304. This helps to achieve a profound understanding of the mechanisms of microbially influenced corrosion (MIC) and especially the possible effects of the redox‐active biomolecules, as they may play an important role in the corrosion susceptibility of stainless steel surfaces.
Comparing the performance of molecular and nanoscale luminophores and luminescent microand nanoparticles and estimating achievable signal amplitudes and limits of detection requires a standardizable intensity scale. This initiated the development of the relative MESF (number of molecules of equivalent soluble fluorochromes) and ERF (equivalent reference fluorophores) scales for flow cytometry and fluorescence microscopy. Both intensity scales rely on fluorescence intensity values assigned to fluorescent calibration beads by an intensity comparison to spectrally closely matching fluorophore solutions of known concentration using a spectrofluorometer. Alternatively, the luminophore or bead brightness (B) can be determined that equals the product of the absorption cross section (σa) at the excitation wavelength (σa(λex)) and the photoluminescence quantum yield (Φpl).
Thereby, an absolute scale based on fundamental and measurable spectroscopic properties can be realized which is independent of particle size, material, and luminophore staining or labeling density and considers the sensitivity of the optical properties of luminophores to their environment. Aiming for establishing such a brightness scale for light-scattering dispersions of luminescent particles with sizes exceeding a few ten nanometers, we demonstrate how the brightness of quasi-monodisperse 25 nm, 100 nm, and 1 μm sized polystyrene particles (PSP), loaded with two different dyes in varying concentrations, can be obtained with a single custom-designed integrating sphere setup that enables the absolute determination of Φpl and transmittance and diffuse reflectance measurements. The resulting Φpl, σa(λex), imaginary parts of the refractive index, and calculated B values of these samples are given in dependence of the number of incorporated dye molecule per particle. Finally, a unitless luminescence efficiency (LE) is defined allowing for the direct comparison of luminescence efficiencies of particles with different sizes.
In order to assess the anisotropy-related uncertainties of relatively determined photoluminescence quantum yields (ΦPL) of molecular emitters and luminescent nanomaterials, we compared ΦPL values measured without and with polarizers using magic angle conditions and studied systematically the dependence of the detected emission intensity on the polarizer settings for samples of varying anisotropy. This includes a dispersion of a spherical quantum dot (QD) with an ideally isotropic emission, a solution of a common small organic dye in a fluid solvent as well as dispersions of elongated quantum dot rods (QDR) with an anisotropic luminescence and a small organic dye in a rigid polymeric matrix, as ideally anisotropic emitter. Our results show that for instruments lacking polarizers, anisotropy-related measurement uncertainties of relative photoluminescence quantum yields can amount to more than 40%, with the size of these systematic errors depending on the difference in emission anisotropy between the sample and the standard.
Luminescence techniques are among the most widely used detection methods in the life and material sciences. At the core of these methods is an ever-increasing variety of fluorescent reporters (i.e., simple dyes, fluorescent labels, probes, sensors and switches) from different fluorophore classes ranging from small organic dyes and metal ion complexes, quantum dots and upconversion nanocrystals to differently sized fluorophore-doped or fluorophore-labeled polymeric particles. A key parameter for fluorophore comparison is the fluorescence quantum yield (Φf), which is the direct measure for the efficiency of the conversion of absorbed light into emitted light. In this protocol, we describe procedures for relative and absolute determinations of Φf values of fluorophores in transparent solution using optical methods, and we address typical sources of uncertainty and fluorophore class-specific challenges. For relative determinations of Φf, the sample is analyzed using a conventional fluorescence spectrometer. For absolute determinations of Φf, a calibrated stand-alone integrating sphere setup is used. To reduce standard-related uncertainties for relative measurements, we introduce a series of eight candidate quantum yield standards for the wavelength region of ~350950 nm, which we have assessed with commercial and custom-designed instrumentation. With these protocols and standards, uncertainties of 5–10% can be achieved within 2 h.
High sensitizer and activator concentrations have been increasingly examined to improve the performance of multi-color emissive upconversion (UC) nanocrystals (UCNC) like NaYF4:Yb,Er and first strategies were reported to reduce concentration quenching in highly doped UCNC. UC luminescence (UCL) is, however, controlled not only by dopant concentration, yet by an interplay of different parameters including size, crystal and shell quality, and excitation power density (P). Thus, identifying optimum dopant concentrations requires systematic studies of UCNC designed to minimize additional quenching pathways and quantitative spectroscopy. Here, we quantify the dopant concentration dependence of the UCL quantum yield (ΦUC) of solid
NaYF4:Yb,Er/NaYF4:Lu upconversion core/shell nanocrystals of varying Yb3+ and Er3+ concentrations (Yb3+ series: 20%‒98% Yb3+; 2% Er3+; Er3+ series: 60% Yb3+; 2%‒40% Er3+). To circumvent other luminescence quenching processes, an elaborate synthesis yielding OH-free UCNC with record ΦUC of ~9% and ~25 nm core particles with a thick surface shell were used. High Yb3+ concentrations barely reduce ΦUC from ~9% (20% Yb3+) to ~7% (98% Yb3+) for an Er3+ concentration of 2%, thereby allowing to strongly increase the particle absorption cross section and UCNC brightness. Although an increased Er3+ concentration reduces ΦUC from ~7% (2% Er3+) to 1% (40%) for 60% Yb3+. Nevertheless, at very high P (> 1 MW/cm2) used for microscopic studies, highly Er3+-doped UCNC display a high brightness because of reduced saturation. These findings underline the importance of synthesis control and will pave the road to many fundamental studies of UC materials.
To assess the clinical course of a sheep stifle joint model for osteochondral (OC) defects, medial femoral condyles (MFC) were exposed without patella luxation using medial parapatellar skin (3–4 cm) and deep incisions (2–3 cm). Two defects (7 mm diameter; 10 mm depth; OC punch) were left empty or refilled with osteochondral autologous transplantation cylinders (OATS) and explanted after six weeks. Incision-to-suture time, anesthesia time, and postoperative wound or impairment scores were compared to those in sham-operated animals. Implant performance was assessed by X-ray, micro-computed tomography, histology, and immunohistology (collagens 1, 2; aggrecan). There were no surgery-related infections or patellar luxations. Operation, anesthesia, and time to complete stand were short (0.5, 1.4, and 1.5 h, respectively). The wound trauma score was low (0.4 of maximally 4; day 7). Empty-defect and OATS animals reached an impairment score of 0 significantly later than sham animals (7.4 and 4.0 days, respectively, versus 1.5 days). Empty defects showed incomplete healing and dedifferentiation/heterotopic differentiation; OATS-filled defects displayed advanced bone healing with remaining cartilage gaps and orthotopic expression of bone and cartilage markers. Minimally-invasive, medial parapatellar surgery of OC defects on the sheep MFC allows rapid and low-trauma recovery and appears well-suited for implant testing.
Evolution relies on the availability of genetic diversity for fitness-based selection. However, most deoxyribonucleic acid (DNA) viruses employ DNA polymerases (Pol) capable of exonucleolytic proofreading to limit mutation rates during DNA replication. The relative genetic stability produced by high-fidelity genome replication can make studying DNA virus adaptation and evolution an intensive endeavor, especially in slowly replicating viruses. Here, we present a proofreading-impaired Pol mutant (Y547S) of Marek’s disease virus that exhibits a hypermutator phenotype while maintaining unimpaired growth in vitro and wild-type (WT)-like pathogenicity in vivo. At the same time, mutation frequencies observed in Y547S virus populations are 2–5-fold higher compared to the parental WT virus. We find that Y547S adapts faster to growth in originally non-permissive cells, evades pressure conferred by antiviral inhibitors more efficiently, and is more easily attenuated by serial passage in cultured cells compared to WT. Our results suggest that hypermutator viruses can serve as a tool to accelerate evolutionary processes and help identify key genetic changes required for adaptation to novel host cells and resistance to antiviral therapy. Similarly, the rapid attenuation achieved through adaptation of hypermutators to growth in cell culture enables identification of genetic changes underlying attenuation and virulence, knowledge that could practically exploited, e.g. in the rational design of vaccines.
Objective: The utilization of fluorescein-guided biopsies and resection has been recently discussed as a suitable strategy to improve and expedite operative techniques for the resection of central nervous system (CNS) tumors. However, little is known about the optical properties of sodium fluorescein (NaFl) in human tumor tissue and their potential impact on ex vivo analyses involving fluorescence-based methods.
Methods: Tumor tissue was obtained from a study cohort of an observational study on the utilization of fluorescein-guided biopsy and resection (n=5). The optical properties of fluorescein-stained tissue were compared to the optical features of the dye in vitro and in control samples consisting of tumor tissue of high-grade glioma patients (n=3) without intravenous (i.v.) application of NaFl. The dye-exposed tumor tissues were used for optical measurements to confirm the detectability of NaFl emission ex vivo. The tissue samples were fixed in 4%PFA, immersed in 30% sucrose, embedded in Tissue-Tek OCT compound, and cut to 10 mm cryosections. Spatially resolved emission spectra from tumor samples were recorded on representative slides with a Confocal Laser Scanning Microscope FV1000 (Olympus GmbH, Hamburg, Germany) upon excitation with lexc = 488 nm.
Results: Optical measurements of fluorescein in 0.9% sodium chloride (NaCl) under in vitro conditions showed an absorption maximum of lmax abs = 479 nm as detected with spectrophotometer Specord 200 and an emission peak at lmax em = 538 nm recorded with the emCCD detection system of a custom-made microscope-based single particle setup using a 500 nm long-pass filter. Further measurements revealed pH- and concentration-dependent emission spectra of NaFl. Under ex vivo conditions, confocal laser scanning microscopy of fluorescein tumor samples revealed a slight bathochromic shift and a broadening of the emission band.
Conclusion: Tumor uptake of NaFl leads to changes in the optical properties – a bathochromic shift and broadening of the emission band – possibly caused by the dye’s high pH sensitivity and concentration-dependent reabsorption acting as an innerfilter of the dye’s emission, particularly in the short wavelength region of the Emission spectrum where absorption and fluorescence overlap. Understanding the ex vivo optical properties of fluorescein is crucial for testing and validating its further applicability as an optical probe for intravital microscopy, immunofluorescence localization studies, and flow cytometry analysis.
We present a versatile and simple method using electrochemistry for the exclusive functionalization of the edge of a graphene monolayer with metal nanoparticles or polymeric amino groups. The attachment of metal nanoparticles allows us to exploit surface-enhanced Raman scattering to characterize the chemistry of both the pristine and the functionalized graphene edge. For the pristine patterned graphene edge, we observe the typical edge-related modes, while for the functionalized graphene edge we identify the chemical structure of the functional layer by vibrational fingerprinting. The ability to obtain single selectively functionalized graphene edges routinely on an insulating substrate opens an avenue for exploring the effect of edge chemistry on graphene properties systematically.
Aim of study: In this study, natural durability of some domestic and foreign wood species against Hylotrupes bajulus and Anobium punctatum larvae were tested on laboratory scale
Area of study: This study was conducted at Department of Forest Products Engineering in Duzce University, Turkey and Federal Institute for Materials Research and Testing (BAM), Germany.
Material and Methods: Scotch pine (Pinus sylvestris), fir (Abies nordmanniana), spruce (Picea orientalis), cedar (Cedrus libani), poplar (Populus tremula) and beech (Fagus orientalis) woods were used to test H. bajulus larvae (EN 46-1). Alder (Alnus glutinosa), oak (Quercus cerris), poplar (Populus tremula), beech (Fagus orientalis), maple (Acer carpinifolium), ash (Fraxinus angustifolia), teak (Tectona grandis), ayous (Triplochiton scleroxylon), movingui (Distemonanthus benthamianus), dahoma (Piptadeniastrum africanum), iroko (Chlorophora excelsa), bubinga (Guibourtia tessmannii) and sapele (Entandrophragma cylindiricum) woods were used for A. punctatum larvae (EN 49-1). At the end of the experiment, the mortality rates of the larvae were determined and the size and weights of the surviving larvae were measured.
Main results: F. orientalis and C. libani were found to be the most resistant wood species against H. bajulus larvae while A. nordmanniana was the least resistant. All tropical wood species and oak and maple from domestic wood species showed 100% mortality rate therefore found to be the most resistant against A. punctatum larvae. The most vulnerable wood species was found to be alder with a 35% mortality.
Research highlights: while F. orientalis, C. libani, and P. tremula were found the most resistance wood species against H. bajulus, P. sylvestris and A. nordmanniana were determined as most vulnerable. All tropical wood species and two domestic species (Q. cerris and A. carpinifolium) showed the highest mortality rate as 100%. The least durable domestic wood was determined as alder.
Through experimental observation and auxiliary numerical simulation, this investigation studies the different types of grain refinement of 5754 aluminum alloy laser beam welding by applying a transverse oscillating magnetic field. Scanning electron microscope results have proved that the application of a magnetic field can reduce the average crystal branch width and increase its number. The interaction between the induced eddy current generated by the Seebeck effect and the applied external magnetic field produces a Lorentz force, which is important for the increase in the number of crystal branches. Based on the theory of dendrite fragmentation and the magnetic field-induced branches increment, the grain size reduction caused by the magnetic field is studied. Furthermore, the effects of the magnetic field are analyzed by combining a phase field method model and simulations of nucleation and grain growth. The grain distribution and average grain
size after welding verify the reliability of the model. In addition, the introduction of a magnetic field can increase the number of periodic three-dimensional solidification patterns. In the intersection of two periods of solidification patterns, the metal can be re-melted and then re-solidified, which prevents the grains, that have been solidified and formed previously, from further growth and generates some small cellular grains in the new fusion line. The magnetic field increases the building frequency of these solidification structures and thus promotes this kind of grain refinement.
The effect of the oscillating metal vapor plume on the keyhole and molten pool behavior during the laser beam welding of AlMg3 aluminum alloys is investigated by experimental and numerical methods. The real-time height of the metal vapor plume is measured by high-speed camera observation. The obtained experimental results are used to evaluate the additional heating source and laser beam attenuation caused by the scattering and absorption based on the Beer–Lambert theory. Furthermore, the dynamic behavior of the metal vapor plume is incorporated into a 3D transient heat transfer and fluid flow model, coupled with the ray tracing method, for the laser beam welding of the AlMg3 alloy. It is found that additional heating resulting from the scattered and absorbed laser beam energy by the metal vapor plume significantly expands the shape of the molten pool on the top region. Moreover, the oscillating metal vapor plume caused the fluctuation of the high-temperature region in the molten pool. The probability of keyhole collapse at the bottom increases 17% due to the oscillating laser power induced by the laser beam attenuation. The internal interplay between the metal vapor plume, molten pool shape, and keyhole collapse is obtained. The developed model has been validated by experiments, which shows a good agreement.
Liquid metal embrittlement (LME) cracking is a phenomenon observed during resistance spot welding (RSW) of zinccoated advanced highstrength steels (AHSS) in automotive manufacturing. In this study, severe cracks are observed at the edge of the sheet under reduced flange widths. These cracks, traversing the AHSS sheet, culminate at the edge with a width of approximately 1.2 mm.
Through combined numerical and experimental investigations, and material testing, these cracks are identified and validated as a new type of LME crack. The mechanism behind this crack formation is attributed to unique geometric conditions that, when compared to center welding, amplify radial material flow by ninefold to 0.87 mm. The resultant tangential tensile stresses approximate 760 MPa, which exceed the yield strength of the examined advanced highstrength steel (AHSS) under heightened temperature conditions, and when combined with liquid zinc, promote the formation of this new type of LME crack.
Water is generally considered to be an undesirable substance in fuel system, which may lead to microbial contamination. The antibacterial strategies that can turn water into things of value with high disinfection efficacy have been urgently needed for fuel system. Here, we reveal a water-fueled autocatalytic bactericidal pathway comprised by bi-metal micro-electrode system, which can spontaneously produce reactive oxygen species (mainly H2O2 and O2•–) by the electron Fenton-like reaction in water medium without external energy., The respiratory chain component of bacteria and the galvanic corrosion on the coated metals were two electron sources in the system. The specific model of Ag-Ru water-fueled autocatalytic (WFA) microelectrode particles presents extremely high disinfection efficiency (>99.9999%) in less than one hour for three aerobic bacteria (Escherichia coli, Pseudomonas aeruginosa and Bacillus subtilis) in LB media and high disinfection efficiency for the anaerobic bacteria (Desulfovibrio alaskensis) in Postgate E media without natural light irradiation. Overall, the novel WFA Ag-Ru antibacterial material explored in this study has a high potential for sterilizing applications in fuel system and this work provides the potential for the development of non-chemical and water-based antibacterial materials, such as WFA Ag-Ru antibacterial coating on stainless steel.
Li dendrites penetration through solid electrolytes (SEs) challenges the development of solid-state Li batteries (SSLBs). To date, significant efforts are devoted to understand the mechanistic dynamics of Li dendrites nucleation, growth, and propagation in SEs, and various strategies that aim to alleviate and even inhibit Li dendrite formation have been proposed. Nevertheless, most of these conventional strategies require either additional material processing steps or new materials/layers that eventually increase battery cost and complexity. In contrast, using external fields, such as mechanical force, temperature physical field, electric field, pulse current, and even magnetic field to regulate Li dendrites penetration through SEs, seems to be one of the most cost-effective strategies. This review focuses on the current research progress of utilizing external physical fields in regulating Li dendrites growth in SSLBs. For this purpose, the mechanical properties of Li and SEs, as well as the experimental results that visually track Li penetration dynamics, are reviewed. Finally, the review ends with remaining open questions in future studies of Li dendrites growth and penetration in SEs. It is hoped this review can shed some light on understanding the complex Li dendrite issues in SSLBs and potentially guide their rational design for further development.
A simple batch test leaching procedure is used in many countries, as a compliance test, to evaluate the leaching of mainly inorganic substances from soil. However, agitating certain types of soil and then passing the solution through a membrane filter with 0.45-µm pores yields filtrates that have been colored by the colloidal particles. These colloids might affect the results of the inorganic substances obtained in the batch tests. In this study, we evaluated the effects of colloidal particles on the results and the reproducibility of batch tests on contaminated soil using different agitation methods and membrane filters with different pore sizes. The leaching behaviors of As, Pb, Se, F and Cl from three types of soil were studied. The As and Pb concentrations in the leachates of some types of soil were clearly affected by the amount of colloidal particles with a diameter of 0.10–0.45 µm and by the agitation method used. This was probably because As and Pb were present mainly in the particulate form in the leachate that had been passed through a membrane filter with 0.45-µm pores. This is not the case for every type of soil. The results of batch leaching tests showed that not only dissolved but also colloidal forms with a diameter of 0.10–0.45 µm might be included and that the existence of colloidal particles in the leachate decreases the batch leaching test reproducibility.
Introducing fluorine into molecules has a wide range of effects on their physicochemical properties, often desirable but in most cases unpredictable. The fluorine atom imparts the C–F bond with low polarizability and high polarity, and significantly affects the behavior of neighboring functional groups, in a covalent or noncovalent manner. Here, we report that fluorine, present in the form of a single fluoroalkyl amino acid side chain in the P1 position of the well-characterized serine-protease inhibitor BPTI, can fully restore inhibitor activity to a mutant that contains the corresponding hydrocarbon side chain at the same site. High resolution crystal structures were obtained for four BPTI variants in complex with bovine b-trypsin, revealing changes in the stoichiometry and dynamics of water molecules in the S1 subsite. These results demonstrate that the introduction of fluorine into a protein environment can result in “chemical complementation” that has a significantly favorable impact on protein–protein interactions.
Trace elements play an important role in the fine-tuning of complex material properties. This study focuses on the correlation of microstructure, lattice misfit and creep properties. The compositionally complex alloy Al10Co25Cr8Fe15Ni36Ti6 (in at. %) was tuned with high melting trace elements Hf and W. The microstructure consists of a γ matrix, γ' precipitates and the Heusler phase and it is accompanied by good mechanical properties for high temperature applications. The addition of 0.5 at.% Hf to the Al10Co25Cr8Fe15Ni36Ti6 alloy resulted in more sharp-edged cubic γ′ precipitates and an increase in the Heusler phase amount. The addition of 1 at.% W led to more rounded γ′ precipitates and the dissolution of the Heusler phase. The shapes of the γ' precipitates of the alloys Al9.25Co25Cr8Fe15Ni36Ti6Hf0.25W0.5 and Al9.25Co25Cr8Fe15Ni36Ti6Hf0.5W0.25, that are the alloys of interest in this paper, create a transition from the well-rounded precipitates in the alloy with 1% W containing alloy to the sharp angular particles in the alloy with 0.5% Hf. While the lattice misfit has a direct correlation to the γ' precipitates shape, the creep rate is also related to the amount of the Heusler phase. The lattice misfit increases with decreasing corner radius of the γ' precipitates. So does the creep rate, but it also increases with the amount of Heusler phase. The microstructures were investigated by SEM and TEM, the lattice misfit was calculated from the lattice parameters obtained by synchrotron radiation measurements.
The phase behavior and molecular ordering of hexakishexyloxy triphenylene (HAT6) DLC under cylindrical nanoconfinement is studied utilizing differential scanning calorimetry (DSC) and dielectric spectroscopy (DS), where cylindrical nanoconfinement is established through embedding HAT6 into the nanopores of anodic aluminum oxide membranes (AAO), and a silica membrane with pore diameters ranging from 161 nm down to 12 nm. Both unmodified and modified pore walls were considered, and in the latter case the pore walls of AAO membranes were chemical treated with n octadecylphosphonic acid (ODPA) resulting in the formation of a 2.2 nm thick layer of grafted alkyl chains. Phase transition enthalpies decrease with decreasing pore size, indicating that a large proportion of the HAT6 molecules within the pores has a disordered structure, which increases with decreasing pore size for both pore walls. In the case of the ODPA modification the amount of ordered HAT6 is increased compared to the unmodified case. The pore size dependencies of the phase transition temperatures were approximated using the Gibbs Thomson equation, where the estimated surface tension is dependent on the molecular ordering of HAT6 molecules within the pores and upon their surface. DS was employed to investigate the molecular ordering of HAT6 within the nanopores. These investigations revealed that with a pore size of around 38 nm, for the samples with the unmodified pore walls, the molecular ordering changes from planar axial to homeotropic radial. However, the planar axial configuration, which is suitable for electronic applications, can be successfully preserved through ODPA modification for most of the pore sizes.
The digitalization of quality control processes and the underlying data infrastructures for safety relevant components, such as hydrogen pressure vessels, plays a significant role in the transition towards Industry 4.0. In the current safety regulations for hydrogen pressure vessels, there is no established concept for structural health monitoring. The development of a reliable structural health monitoring methodology for monitoring the structural integrity of pressure vessels enables a fast-forward transition from personnel- and costintensive recurring inspections, a.k.a. periodic maintenance, to predictive maintenance. In the work presented; we investigated the application of ultrasonic guided wave propagation to monitor and assess the condition of Type IV composite overwrapped pressure vessel (COPV). A sensor network of fifteen piezo-electric wafers is placed on the carbon fibre reinforced composite cylinder. Five different artificial damage configurations are created by gluing two different weight blocks on three different locations. The database containing measured guided wave data sets is enriched by two different boundary conditions. We utilized an open-source software, openBIS labnotebook, to store and analyse experimental datasets. The guided wave ultrasonic signals were investigated and analysed by using commonly used ultrasonic features (e.g., amplitude, frequency, time of flight) as well as non-traditional time-series features (kurtosis, skewness, variance). The features were used to calculate damage index and the detection performance for the results has been evaluated. The results suggest that both traditional and non-traditional features assume significant importance in artificial damage detection. The future works will additionally involve the impacts of operational conditions, such as periodic pressure variations temperature loadings as well as material degradations.