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End date: 2023 × Subject: stability ×

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    Development of Highly Stable Low Ni Content Catalyst for Dry Reforming of CH4-Rich Feedstocks
    (Weinheim : WILEY-VCH Verlag, 2020) Ha, Quan Luu Manh; Lund, Henrik; Kreyenschulte, Carsten; Bartling, Stephan; Atia, Hanan; Vuong, Than Huyen; Wohlrab, Sebastian; Armbruster, Udo
    Highly active and coking-resistant Ni catalysts suited for the dry reforming of CH4-rich gases (70 vol %, e. g. biogas or sour natural gas) were prepared starting from a Mg-rich Mg−Al hydrotalcite support precursor. Calcination at 1000 °C yields two phases, MgO and MgAl2O4 spinel. Complexation-deposition of Ni with citric acid on the preformed support as well as lanthanum addition yields a catalyst with remarkably low carbon accumulation over 100 h on stream attributed to both high Ni dispersion and preferred interactions of Ni with MgO on MgAl2O4. © 2020 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.
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    Development of structural correlations and synchronization from adaptive rewiring in networks of Kuramoto oscillators
    (Woodbury, NY : American Institute of Physics, 2017) Papadopoulos, Lia; Kim, Jason Z.; Kurths, Jürgen; Bassett, Danielle S.
    Synchronization of non-identical oscillators coupled through complex networks is an important example of collective behavior, and it is interesting to ask how the structural organization of network interactions influences this process. Several studies have explored and uncovered optimal topologies for synchronization by making purposeful alterations to a network. On the other hand, the connectivity patterns of many natural systems are often not static, but are rather modulated over time according to their dynamics. However, this co-evolution and the extent to which the dynamics of the individual units can shape the organization of the network itself are less well understood. Here, we study initially randomly connected but locally adaptive networks of Kuramoto oscillators. In particular, the system employs a co-evolutionary rewiring strategy that depends only on the instantaneous, pairwise phase differences of neighboring oscillators, and that conserves the total number of edges, allowing the effects of local reorganization to be isolated. We find that a simple rule-which preserves connections between more outof- phase oscillators while rewiring connections between more in-phase oscillators-can cause initially disordered networks to organize into more structured topologies that support enhanced synchronization dynamics. We examine how this process unfolds over time, finding a dependence on the intrinsic frequencies of the oscillators, the global coupling, and the network density, in terms of how the adaptive mechanism reorganizes the network and influences the dynamics. Importantly, for large enough coupling and after sufficient adaptation, the resulting networks exhibit interesting characteristics, including degree-frequency and frequency-neighbor frequency correlations. These properties have previously been associated with optimal synchronization or explosive transitions in which the networks were constructed using global information. On the contrary, by considering a time-dependent interplay between structure and dynamics, this work offers a mechanism through which emergent phenomena and organization can arise in complex systems utilizing local rules.
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    Li+/H+ exchange of Li7La3Zr2O12 single and polycrystals investigated by quantitative LIBS depth profiling
    (Cambridge : Royal Society of Chemistry, 2022) Smetaczek, Stefan; Limbeck, Andreas; Zeller, Veronika; Ring, Joseph; Ganschow, Steffen; Rettenwander, Daniel; Fleig, Jürgen
    Li7La3Zr2O12 (LLZO) garnets are highly attractive to be used as solid electrolyte in solid-state Li batteries. However, LLZO suffers from chemical interaction with air and humidity, causing Li+/H+ exchange with detrimental implication on its performance, processing and scalability. To better understand the kinetics of the detrimental Li+/H+ exchange and its dependence on microstructural features, accelerated Li+/H+ exchange experiments were performed on single crystalline and polycrystalline LLZO, exposed for 80 minutes to 80 °C hot water. The resulting chemical changes were quantified by analytical methods, i.e. inductively coupled plasma optical emission spectroscopy (ICP-OES) and laser induced breakdown spectroscopy (LIBS). From the time dependence of the Li+ enrichment in the water, measured by ICP-OES, a bulk interdiffusion coefficient of Li+/H+ could be determined (7 × 10−17 m2 s−1 at 80 °C). Depth dependent concentrations were obtained from the LIBS data for both ions after establishing a calibration method enabling not only Li+ but also H+ quantification in the solid electrolyte. Short interdiffusion lengths in the 1 μm range are found for the single crystalline Ga:LLZO, in accordance with the measured bulk diffusion coefficient. In polycrystalline Ta:LLZO, however, very long diffusion tails in the 20 μm range and ion exchange fractions up to about 70% are observed. Those are attributed to fast ion interdiffusion along grain boundaries. The severe compositional changes also strongly affect the electrical properties measured by impedance spectroscopy. This study highlights that microstructural effects may be decisive for the Li+/H+ ion exchange kinetics of LLZO.
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    Ageing of alkylthiol-stabilized gold nanoparticles
    (Hoboken, NJ : Wiley, 2015) Lacava, Johann; Weber, Anika; Kraus, Tobias
    The ageing of spherical gold nanoparticles having 6-nm-diameter cores and a ligand shell of dodecanethiol is investigated under different storage conditions. Losses caused by agglomeration and changes in optical particle properties are quantified. Changes in colloidal stability are probed by analytical centrifugation in a polar solvent mixture. Chemical changes are detected by elementary analysis of particles and solvent. Fractionation occurs under all storage conditions. Ageing is not uniform but broadens the property distributions of the particles. Small-number statistics in the ligand shell density and the morphological heterogeneity of particles are possible explanations. Washing steps exacerbate ageing, a process that could not be fully reversed by excess ligands. Dry storage is not preferable to storage in solvent. Storage under inert argon atmosphere reduces losses more than all other conditions but could not prevent it entirely.
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    Identifying a Safe and Just Corridor for People and the Planet
    (Hoboken, NJ : Wiley-Blackwell, 2021) Rockström, Johan; Gupta, Joyeeta; Lenton, Timothy M.; Qin, Dahe; Lade, Steven J.; Abrams, Jesse F.; Jacobson, Lisa; Rocha, Juan C.; Zimm, Caroline; Bai, Xuemei; Bala, Govindasamy; Bringezu, Stefan; Broadgate, Wendy; Bunn, Stuart E.; DeClerck, Fabrice; Ebi, Kristie L.; Gong, Peng; Gordon, Chris; Kanie, Norichika; Liverman, Diana M.; Nakicenovic, Nebojsa; Obura, David; Ramanathan, Veerabhadran; Verburg, Peter H.; van Vuuren, Detlef P.; Winkelmann, Ricarda
    Keeping the Earth system in a stable and resilient state, to safeguard Earth's life support systems while ensuring that Earth's benefits, risks, and related responsibilities are equitably shared, constitutes the grand challenge for human development in the Anthropocene. Here, we describe a framework that the recently formed Earth Commission will use to define and quantify target ranges for a “safe and just corridor” that meets these goals. Although “safe” and “just” Earth system targets are interrelated, we see safe as primarily referring to a stable Earth system and just targets as being associated with meeting human needs and reducing exposure to risks. To align safe and just dimensions, we propose to address the equity dimensions of each safe target for Earth system regulating systems and processes. The more stringent of the safe or just target ranges then defines the corridor. Identifying levers of social transformation aimed at meeting the safe and just targets and challenges associated with translating the corridor to actors at multiple scales present scope for future work.
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    Bis(stearoyl) Sulfide: A Stable, Odor-Free Sulfur Precursor for High-Efficiency Metal Sulfide Quantum Dot Photovoltaics
    (Weinheim : Wiley-VCH, 2023) Albaladejo‐Siguan, Miguel; Prudnikau, Anatol; Senina, Alina; Baird, Elizabeth C.; Hofstetter, Yvonne J.; Brunner, Julius; Shi, Juanzi; Vaynzof, Yana; Paulus, Fabian
    The synthesis of metal sulfide nanocrystals is a crucial step in the fabrication of quantum dot (QD) photovoltaics. Control over the QD size during synthesis allows for precise tuning of their optical and electronic properties, making them an appealing choice for electronic applications. This flexibility has led to the implementation of QDs in both highly-efficient single junction solar cells and other optoelectronic devices including photodetectors and transistors. Most commonly, metal sulfide QDs are synthesized using the hot-injection method utilizing a toxic, and air- and moisture-sensitive sulfur source: bis(trimethylsilyl) sulfide ((TMS)2S). Here, bis(stearoyl) sulfide (St2S) is presented as a new type of air-stable sulfur precursor for the synthesis of sulfide-based QDs, which yields uniform, pure, and stable nanocrystals. Photovoltaic devices based on these QDs are equally efficient as those fabricated by (TMS)2S but exhibit enhanced operational stability. These results highlight that St2S can be widely adopted for the synthesis of metal sulfide QDs for a range of optoelectronic applications.
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    Reliability of inference of directed climate networks using conditional mutual information
    (Basel : MDPI, 2013) Hlinka, Jaroslav; Hartman, David; Vejmelka, Martin; Runge, Jakob; Marwan, Norbert; Kurths, Jürgen; Paluš, Milan
    Across geosciences, many investigated phenomena relate to specific complex systems consisting of intricately intertwined interacting subsystems. Such dynamical complex systems can be represented by a directed graph, where each link denotes an existence of a causal relation, or information exchange between the nodes. For geophysical systems such as global climate, these relations are commonly not theoretically known but estimated from recorded data using causality analysis methods. These include bivariate nonlinear methods based on information theory and their linear counterpart. The trade-off between the valuable sensitivity of nonlinear methods to more general interactions and the potentially higher numerical reliability of linear methods may affect inference regarding structure and variability of climate networks. We investigate the reliability of directed climate networks detected by selected methods and parameter settings, using a stationarized model of dimensionality-reduced surface air temperature data from reanalysis of 60-year global climate records. Overall, all studied bivariate causality methods provided reproducible estimates of climate causality networks, with the linear approximation showing higher reliability than the investigated nonlinear methods. On the example dataset, optimizing the investigated nonlinear methods with respect to reliability increased the similarity of the detected networks to their linear counterparts, supporting the particular hypothesis of the near-linearity of the surface air temperature reanalysis data.
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    A jump-diffusion Libor model and tits robust calibration
    (Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2006) Belomestrny, Denis; Schoenmakers, John G.M.
    In this paper we propose a jump-diffusion Libor model with jumps in a high-dimensional space and test a stable non-parametric calibration algorithm which takes into account a given local covariance structure. The algorithm returns smooth and simply structured Lévy densities, and penalizes the deviation from the Libor market model. In practice, the procedure is FFT based, thus fast, easy to implement, and yields good results, particularly in view of the ill-posedness of the underlying inverse problem.
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    Rate-independent evolution of sets
    (Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2019) Rossi, Riccarda; Stefanelli, Ulisse; Thomas, Marita
    The goal of this work is to analyze a model for the rate-independent evolution of sets with finite perimeter. The evolution of the admissible sets is driven by that of a given time-dependent set, which has to include the admissible sets and hence is to be understood as an external loading. The process is driven by the competition between perimeter minimization and minimization of volume changes. In the mathematical modeling of this process, we distinguish the adhesive case, in which the constraint that the (complement of) the `external load' contains the evolving sets is penalized by a term contributing to the driving energy functional, from the brittle case, enforcing this constraint. The existence of Energetic solutions for the adhesive system is proved by passing to the limit in the associated time-incremental minimization scheme. In the brittle case, this time-discretization procedure gives rise to evolving sets satisfying the stability condition, but it remains an open problem to additionally deduce energy-dissipation balance in the time-continuous limit. This can be obtained under some suitable quantification of data. The properties of the brittle evolution law are illustrated by numerical examples in two space dimensions.
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    An iterative method for the multipliers of periodic delay-differential equations and the analysis of a PDE milling model
    (Berlin : Weierstraß-Institut für Angewandte Analysis und Stochastik, 2009) Rott, Oliver; Jarlebring, Elisa
    Locally convergent iterative schemes have turned out to be very useful in the analysis of the characteristic roots of delay-differential equations (DDEs) with constant coefficients. In this work we present a locally convergent iterative scheme for the characteristic multipliers of periodic-coefficient DDEs. The method is an adaption of an iterative method called residual inverse iteration. The possibility to use this method stems from an observation that the characteristic matrix can be expressed with the fundamental solution of a differential equation. We apply the method to a coupled milling model containing a partial and an ordinary differential equation. The conclusion of the numerical results is that the stability diagram of the coupled model differs significantly from the combined stability diagrams for each subsystem