INMdok (Leibniz Institute for New Materials)
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Optical detection of di- and triphosphate anions with mixed monolayer-protected gold nanoparticles containing zinc(II)–dipicolylamine complexes
Get PDFGold nanoparticles covered with a mixture of ligands of which one type contains solubilizing triethylene glycol residues and the other peripheral zinc(II)–dipicolylamine (DPA) complexes allowed the optical detection of hydrogenphosphate, diphosphate, and triphosphate anions in water/methanol 1:2 (v/v). These anions caused the bright red solutions of the nanoparticles to change their color because of nanoparticle aggregation followed by precipitation, whereas halides or oxoanions such as sulfate, nitrate, or carbonate produced no effect. The sensitivity of phosphate sensing depended on the nature of the anion, with diphosphate and triphosphate inducing visual changes at significantly lower concentrations than hydrogenphosphate. In addition, the sensing sensitivity was also affected by the ratio of the ligands on the nanoparticle surface, decreasing as the number of immobilized zinc(II)–dipicolylamine groups increased. A nanoparticle containing a 9:1 ratio of the solubilizing and the anion-binding ligand showed a color change at diphosphate and triphosphate concentrations as low as 10 μmol/L, for example, and precipitated at slightly higher concentrations. Hydrogenphosphate induced a nanoparticle precipitation only at a concentration of ca. 400 μmol/L, at which the precipitates formed in the presence of diphosphates and triphosphates redissolved. A nanoparticle containing fewer binding sites was more sensitive, while increasing the relative number of zinc(II)–dipicolylamine complexes beyond 25% had a negative impact on the limit of detection and the optical response. Transmission electron microscopy provided evidence that the changes of the nanoparticle properties observed in the presence of the phosphates were due to a nanoparticle crosslinking, consistent with the preferred binding mode of zinc(II)–dipicolylamine complexes with phosphate anions which involves binding of the anion between two metal centers. This work thus provided information on how the behavior of mixed monolayer-protected gold nanoparticles is affected by multivalent interactions, at the same time introducing a method to assess whether certain biologically relevant anions are present in an aqueous solution within a specific concentration range
Anti-correlation of HER2 and focal adhesion complexes in the plasma membrane
Get PDFExcess presence of the human epidermal growth factor receptor 2 (HER2) as well as of the focal adhesion protein complexes are associated with increased proliferation, migratory, and invasive behavior of cancer cells. A cross-regulation between HER2 and integrin signaling pathways has been found, but the exact mechanism remains elusive. Here, we investigated whether HER2 colocalizes with focal adhesion complexes on breast cancer cells overexpressing HER2. For this purpose, vinculin or talin green fluorescent protein (GFP) fusion proteins, both key constituents of focal adhesions, were expressed in breast cancer cells. HER2 was either extracellularly or intracellularly labeled with fluorescent quantum dots nanoparticles (QDs). The cell-substrate interface was analyzed at the location of the focal adhesions by means of total internal reflection fluorescent microscopy or correlative fluorescence- and scanning transmission electron microscopy. Expression of HER2 at the cell-substrate interface was only observed upon intracellular labeling, and was heterogeneous with both HER2-enriched and -low regions. In contrast to an expected enrichment of HER2 at focal adhesions, an anti-correlated expression pattern was observed for talin and HER2. Our findings suggest a spatial anti-correlation between HER2 and focal adhesion complexes for adherent cells
Liquid-Phase Electron Microscopy for Soft Matter Science and Biology
Get PDFAbstract Innovations in liquid-phase electron microscopy (LP-EM) have made it possible to perform experiments at the optimized conditions needed to examine soft matter. The main obstacle is conducting experiments in such a way that electron beam radiation can be used to obtain answers for scientific questions without changing the structure and (bio)chemical processes in the sample due to the influence of the radiation. By overcoming these experimental difficulties at least partially, LP-EM has evolved into a new microscopy method with nanometer spatial resolution and sub-second temporal resolution for analysis of soft matter in materials science and biology. Both experimental design and applications of LP-EM for soft matter materials science and biological research are reviewed, and a perspective of possible future directions is given
Transcriptomic expression patterns of two contrasting lowland rice varieties reveal high iron stress tolerance
Get PDFIron (Fe) toxicity is a major challenge for plant cultivation in acidic water-logged soil environments, where lowland rice is a major staple food crop. Only few studies addressed the molecular characterization of excess Fe tolerance in rice, and these highlight different mechanisms for Fe tolerance in the studied varieties.
Here, we screened 16 lowland rice varieties for excess Fe stress growth responses to identify contrasting lines, Fe-tolerant Lachit and -susceptible Hacha. Hacha and Lachit differed in their physiological and morphological responses to excess Fe, including leaf growth, leaf rolling, reactive oxygen species generation, Fe and metal contents. These responses were mirrored by differential gene expression patterns, obtained through RNA-sequencing, and corresponding GO term enrichment in tolerant versus susceptible lines. From the comparative transcriptomic profiles between Lachit and Hacha in response to excess Fe stress, individual genes of the category metal homeostasis, mainly root-expressed, may contribute to the tolerance of Lachit. 22 out of these 35 metal homeostasis genes are present in selection sweep genomic regions, in breeding signatures and/or differentiated during rice domestication. These findings will serve to design targeted Fe tolerance breeding of rice crops
Growth rate of lithium filaments in ceramic electrolytes
Get PDF© 2020 Lithium-ion batteries with single ion-conductor ceramic electrolytes short-circuit when subjected to charging currents above a critical current density. Here, we analyse the rate at which a lithium (Li) filament (sometimes referred to as a dendrite) will grow from the cathode towards the anode during charging of such batteries. The filament is modelled as a climbing edge dislocation with its growth occurring by Li+ flux from the electrolyte into the filament tip at constant chemical potential. The growth rate is set by a balance between the reduction of free-energy at the filament tip and energy dissipation associated with the resistance to the flux of Li+ through the filament tip. For charging currents above the critical current density, the filament growth rate increases with decreasing filament tip resistance. Imperfections, such as voids in the Li cathode along the electrolyte/cathode interface, decrease the critical current density but filament growth rates are also lower in these cases as filament growth rates scale with the charging currents. The predictions of the model are in excellent quantitative agreement with measurements and confirm that above the critical current density a filament can traverse the electrolyte in minutes or less. This suggests that initiation of filament growth is the critical step to prevent short-circuiting of the battery
Ether functionalisation, ion conformation and the optimisation of macroscopic properties in ionic liquids
Get PDFIonic liquids are an attractive material class due to their wide liquid range, intrinsic ionic conductivity, and high chemical as well as electrochemical stability. However, the widespread use of ionic liquids is hindered by significantly higher viscosities compared to conventional molecular solvents. In this work, we show how the transport properties of ionic liquids can be altered significantly, even for isostructural ions that have the same backbone. To this end, structure–property relationships have been determined for a set of 16 systematically varied representative ionic liquids. Variations in molecular structure include ammonium vs. phosphonium, ether vs. alkyl side chains, and rigid vs. flexible anions. Ab initio calculations are used to relate molecular structures to the thermal, structural and transport properties of the ionic liquids. We find that the differences in properties of ether and alkyl functionalised ionic liquids are primarily dependent on minimum energy geometries, with the conformational flexibility of ether side chains appearing to be of secondary importance. We also show unprecedented correlations between anion conformational flexibility and transport properties. Critically, increasing fluidity upon consecutive introduction of ether side chains and phosphonium centres into the cation is found to be dependent on whether the anion is flexible or rigid. We demonstrate that targeted design of functional groups based on structure–property relationships can yield ionic liquids of exceptionally high fluidity
Flexible Pseudocapacitive Electrochromics via Inkjet Printing of Additive-Free Tungsten Oxide Nanocrystal Ink
Get PDFDirect inkjet printing of functional inks is an emerging and promising technique for the fabrication of electrochemical energy storage devices. Electrochromic energy devices combine electrochromic and energy storage functions, providing a rising and burgeoning technology for next-generation intelligent power sources. However, printing such devices has, in the past, required additives or other second phase materials in order to create inks with suitable rheological properties, which can lower printed device performance. Here, tungsten oxide nanocrystal inks are formulated without any additives for the printing of high-quality tungsten oxide thin films. This allows the assembly of novel electrochromic pseudocapacitive zinc-ion devices, which exhibit a relatively high capacity (≈260 C g−1 at 1 A g−1) with good cycling stability, a high coloration efficiency, and fast switching response. These results validate the promising features of inkjet-printed electrochromic zinc-ion energy storage devices in a wide range of applications in flexible electronic devices, energy-saving buildings, and intelligent systems
Nanoporous materials for optical applications
Get PDFIn this work, a new process of generating nanobubbles* in transparent polymers was developed. The azo-chemical initiators AIBN (Azobisisobutyronitrile) and ABVN (2,2’-Azobis(2,4-dimethylvaleronitrile)) were used as chemical blowing agents (CBA) that deliver nitrogen gas to form the bubbles. Specifically, the photo initiator Irgacure 819, which could be activated by a longer wavelength of UV (405 nm) than that of AIBN (345 nm), was added to the solution in order to minimize the decomposition of the azo chemicals during the first stage of sample preparation by UV-pre-curing. As a result, the CBAs remained unreacted, thus they could decompose and be used merely as a blowing agent. In addition, the post-foaming processes were conducted under the different foaming conditions to investigate critical factors affecting the nucleation and growth of bubbles. The results were discussed based on thermodynamics, mainly by conventional nucleation theory (CNT). Finally, stepwise optimization of those factors led to the generation of nanobubbles. This technique could be applicable to UV curable polymer systems in general. This novel approach was used to make prototype optical devices, such as security mark coating and light out-coupling in optical waveguide. This study also gives important information about the nucleation and growth of bubbles in meta-stable state of polymers, which could help to verify the background theories.In dieser Arbeit wurde ein neues Verfahren zur Herstellung von Nanobläschen in transparenten Polymeren entwickelt. Die azo-chemischen Initiatoren AIBN (Azobisisobutyronitril) und ABVN (2,2'-Azobis(2,4-Dimethylvaleronitril)) wurden als chemische Treibmittel (CBA) verwendet, die Stickstoff zur Bildung der Blasen abgeben. Der Photoinitiator Irgacure 819, der durch längeres UV-Licht (405 nm) als AIBN (345 nm) aktiviert werden kann, wurde zu der Lösung gegeben, um die Zersetzung der Azochemikalien während der ersten Stufe, der Probenvorbereitung durch UV-Vorhärtung, zu minimieren. Die nicht umgesetzten CBAs, zersetzten sich bei Erwärmung und fungierten als Treibmittel. Die Bedingungen der Aufschäumprozesse wurden variiert, um kritische Faktoren zu untersuchen, die Keimbildung und Wachstum von Blasen beeinflussen. Die Ergebnisse wurden auf der Grundlage der Thermodynamik im Kontext der konventionellen Keimbildungstheorie diskutiert. Die schrittweise Optimierung dieser Faktoren führte zur Erzeugung von Nanobläschen. Diese Technik könnte allgemein auf UV-härtbare Polymersysteme anwendbar sein. Dieser neuartige Ansatz wurde verwendet, um für optische Anwendungen Prototypen herzustellen, wie z.B. Beschichtung von Sicherheitsmarkierungen und Lichtauskopplung in optischen Wellenleitern. Diese Studie liefert auch wichtige Informationen zu Keimbildung und Wachstum von Blasen im metastabilen Zustand von Polymeren, die zur Verifizierung der Hintergrundtheorien beitragen könnten
The influence of mean strain on the high-cycle fatigue of Nitinol with application to medical devices
Get PDFOne of the contentious issues associated with the high-cycle fatigue of Nitinol, a nominally equiatomic alloy of nickel and titanium, is the claim that increasing the applied mean strain can increase, or at least have no negative impact, on the fatigue lifetime, in conflict with reported behavior for the vast majority of other metallic materials. To investigate this in further detail, cyclic fatigue tests in bending were carried out on electropolished medical grade Nitinol at 37 °C for lives of up to 400 million cycles of strain involving various levels of the mean strain. A constant life model was developed through statistical analysis of the fatigue data, with 90% reliability at a confidence level of 95% on the effective fatigue strain. Our results show that the constant life diagram, a plot of strain amplitude versus mean strain, is monotonic yet nonlinear for lives of 400 million cycles of fatigue loading. Specifically, we find that in contradiction to the aforementioned claim, the strain amplitude limit at zero mean strain is 0.55% to achieve a 400 million cycle lifetime, at 90% reliability with 95% confidence; however, to achieve the same lifetime, reliability and confidence level in the presence of a 3% or more mean strain, the required strain amplitude limit is decreased by over a factor of three to 0.16%. Moreover, for mean strains from 3% to 7%, the strain amplitude limit that allows a 400 million cycle lifetime, at 90% reliability with 95% confidence, is ~ 0.16%, and essentially independent of mean strain. We conclude that the debatable claim that an increase in the applied mean strain can increase the fatigue life of Nitinol components is not supported by the current data
Safe-by-Design part I: Proposal for nanospecific human health safety aspects needed along the innovation process
Get PDFSafe-by-Design aims to reduce uncertainties and/or increase the human health and environmental safety from already early in the innovation process onwards and will thereby contribute to increased innovation efficiency, economic viability, interdisciplinary collaboration, consumers trust and improve sustainability. Since most innovators or designers are neither toxicologists nor risk assessors, considering human health safety aspects within their innovation process may be challenging. This paper provides sets of questions that can help innovators to assess nanospecific human health safety aspects of their product or material along the various stages of the innovation process. Addressing these questions will facilitate innovators to identify which type of information may support decisions on how to address potential human health risks in the innovation process. The identified information on the human health safety aspects can help innovators to decide if further investments in the product or material are beneficial. It may allow them to rank, prioritize and choose safer alternatives early in the innovation process. This may enable innovators to better anticipate on potential safety issues in an early stage, preventing these safety issues to become an innovation killer in a later stage of the innovation process. This approach to identify potential nanospecific human health risks should be considered as complementary to current regulations. The applicability of this approach was evaluated using a few industrial case studies. To determine if the approach is applicable to the innovation of a broader group of nanomaterials and nano-enabled products, more experience within various industrial sectors is needed