Intracellular dynamic assembly of deep-red emitting supramolecular nanostructures based on the Pt…Pt metallophilic interaction. - In: Advanced materials, ISSN 1521-4095, Bd. 33 (2021), 37, 2008613, insges. 13 S.
https://doi.org/10.1002/adma.202008613
Second floor of flatland: epitaxial growth of graphene on hexagonal boron nitride. - In: Small, ISSN 1613-6829, Bd. 17 (2021), 36, 2102747, insges. 9 S.
In the studies presented here, the subsequent growth of graphene on hexagonal boron nitride (h-BN) is achieved by the thermal decomposition of molecular precursors and the catalytic assistance of metal substrates. The epitaxial growth of h-BN on Pt(111) is followed by the deposition of a temporary Pt film that acts as a catalyst for the fabrication of the graphene sheet. After intercalation of the intermediate Pt film underneath the boron-nitride mesh, graphene resides on top of h-BN. Scanning tunneling microscopy and density functional calculations reveal that the moiré pattern of the van-der-Waals-coupled double layer is due to the interface of h-BN and Pt(111). While on Pt(111) the graphene honeycomb unit cells uniformly appear as depressions using a clean metal tip for imaging, on h-BN they are arranged in a honeycomb lattice where six protruding unit cells enframe a topographically dark cell. This superstructure is most clearly observed at small probe-surface distances. Spatially resolved inelastic electron tunneling spectroscopy enables the detection of a previously predicted acoustic hybrid phonon of the stacked materials. Its' spectroscopic signature is visible in surface regions where the single graphene sheet on Pt(111) transitions into the top layer of the stacking.
https://doi.org/10.1002/smll.202102747
Differential-algebraic systems are generically controllable and stabilizable. - In: Mathematics of control, signals, and systems, ISSN 1435-568X, Bd. 33 (2021), 3, S. 359-377
We investigate genericity of various controllability and stabilizability concepts of linear, time-invariant differential-algebraic systems. Based on well-known algebraic characterizations of these concepts (see the survey article by Berger and Reis (in: Ilchmann A, Reis T (eds) Surveys in differential-algebraic equations I, Differential-Algebraic Equations Forum, Springer, Berlin, pp 1-61. https://doi.org/10.1007/978-3-642-34928-7_1)), we use tools from algebraic geometry to characterize genericity of controllability and stabilizability in terms of matrix formats.
https://doi.org/10.1007/s00498-021-00287-x
Low-field and variable-field NMR relaxation studies of H2O and D2O molecular dynamics in articular cartilage. - In: PLOS ONE, ISSN 1932-6203, Bd. 16 (2021), 8, e0256177, insges. 34 S.
Im Titel ist "2" tiefgestellt
https://doi.org/10.1371/journal.pone.0256177
Insights into the interfacial chemistry and conversion mechanism of iron oxalate toward the reduction by lithium. - In: The chemical engineering journal, ISSN 1873-3212, Bd. 426 (2021), 131446
The origin of excellent lithium storage ability and high irreversible capacity is probably the least understood component for transition-metal oxalates as anode materials in lithium-ion batteries. Considerable efforts have been put into understanding their electrochemical reaction mechanisms, but these insights have mostly been unilateral and unsystematic. Herein, the interface characteristic between iron oxalate anode and electrolyte and detailed conversion process were investigated to explore the source of irreversible Li+ storage. In particular, a gelatinous "organic" layer identified oxygen, fluorine and phosphorus as the main chemical elements can be re-oxidized and exhibits an obviously reversible conversion between sedimentation and decomposition during its initial lithiation process, despite the general belief that it shows similar electrochemically inert to solid-electrolyte interphase (SEI). Meanwhile, this special interface layer leads to higher ability of Li+ ions diffusion and smaller charge-transfer resistance, which is the vital role for excellent rate capability. Furthermore, ex situ FTIR analysis confirms the formation and residue of new intermediate compound of Li2Fe(C2O4)2, thus making a part of initial irreversible capacity. It is also found that the iron oxalate electrode with larger capacitive contribution still has more widely application in energy storage of supercapacitors in future.
https://doi.org/10.1016/j.cej.2021.131446
Colorimetric method for instant detection of lysine and arginine using novel Meldrum's acid-furfural conjugate. - In: ChemistrySelect, ISSN 2365-6549, Bd. 6 (2021), 27, S. 6834-6840
In the past few years Meldrum's acid furfural conjugate (MAFC) have been extensively explored as starting material for the synthesis of photo switchable donor acceptor stenhouse adducts (DASA). Hereby, we have explored the interaction of MAFC with various amino acids. To our surprise, nitrogen rich amino acids like lysine and arginine interact spontaneously with MAFC to give colored adduct immediately, whereas other amino acids, including nitrogen rich histidine, didn't show any coloration. Naked eye detection of lysine in benign solvent make this reagent an attractive new entry to the collection of chemosensors for the colorimetric detection of lysine and arginine. Intense coloration corresponds to the absorption at 514 nm under UV-Vis spectrometer. Lowest concentration of 100 m can be detected with UV-Vis spectrometer. NMR titrations reveals that the appearance of color is due to ring opening of a furfural that leads to the formation of conjugated triene species. Compared to previously reported chemosensors for lysine and arginine, MAFC offers advantages including simple synthesis, easy handling, high speed, low cost, good sensitivity/selectivity.
https://doi.org/10.1002/slct.202101140
Molecular scale insights into interaction mechanisms between organic inhibitor film and copper. - In: npj Materials degradation, ISSN 2397-2106, Bd. 5 (2021), 22, insges. 8 S.
A model experimental approach, providing molecular scale insight into the build up mechanisms of a corrosion inhibiting interface, is reported. 2-mercaptobenzimidazole (2-MBI), a widely used organic inhibitor, was deposited from the vapor phase at ultra-low pressure on copper surfaces in chemically-controlled state, and X-ray photoelectron spectroscopy was used in situ to characterize the adsorption mechanisms upon formation of the inhibiting film. On copper surfaces prepared clean in the metallic state, the intact molecules lie flat at low exposure, with sulfur and both nitrogen atoms bonded to copper. A fraction of the molecules decomposes upon adsorption, leaving atomic sulfur on copper. At higher exposure, the molecules adsorb in a tilted position with sulfur and only one nitrogen bonded to copper, leading to a densification of 2-MBI in the monolayer. A bilayer is formed at saturation with the outer layer not bonded directly to copper. In the presence of a pre-adsorbed 2D oxide, oxygen is substituted and the molecules adsorb intactly without decomposition. A 3D oxide prevents the bonding of sulfur to copper. The molecular film formed on metallic and 2D oxide pre-covered surfaces partially desorbs and decomposes at temperature above 400 ˚C, leading to the adsorption of atomic sulfur on copper.
https://doi.org/10.1038/s41529-021-00168-3
Distributed optimization using ALADIN for MPC in smart grids. - In: IEEE transactions on control systems technology, ISSN 1558-0865, Bd. 29 (2021), 5, S. 2142-2152
This article presents a distributed optimization algorithm tailored to solve optimization problems arising in smart grids. In detail, we propose a variant of the augmented Lagrangian-based alternating direction inexact Newton (ALADIN) method, which comes along with global convergence guarantees for the considered class of linear-quadratic optimization problems. We establish local quadratic convergence of the proposed scheme and elaborate its advantages compared with the alternating direction method of multipliers (ADMM). In particular, we show that, at the cost of more communication, ALADIN requires fewer iterations to achieve the desired accuracy. Furthermore, it is numerically demonstrated that the number of iterations is independent of the number of subsystems. The effectiveness of the proposed scheme is illustrated by running both an ALADIN and an ADMM-based model predictive controller on a benchmark case study.
https://doi.org/10.1109/TCST.2020.3033010
A steepest descent method for set optimization problems with set-valued mappings of finite cardinality. - In: Journal of optimization theory and applications, ISSN 1573-2878, Bd. 190 (2021), 3, S. 711-743
In this paper, we study a first-order solution method for a particular class of set optimization problems where the solution concept is given by the set approach. We consider the case in which the set-valued objective mapping is identified by a finite number of continuously differentiable selections. The corresponding set optimization problem is then equivalent to find optimistic solutions to vector optimization problems under uncertainty with a finite uncertainty set. We develop optimality conditions for these types of problems and introduce two concepts of critical points. Furthermore, we propose a descent method and provide a convergence result to points satisfying the optimality conditions previously derived. Some numerical examples illustrating the performance of the method are also discussed. This paper is a modified and polished version of Chapter 5 in the dissertation by Quintana (On set optimization with set relations: a scalarization approach to optimality conditions and algorithms, Martin-Luther-Universität Halle-Wittenberg, 2020).
https://doi.org/10.1007/s10957-021-01887-y
Gas-flow-assisted wrinkle-free transfer of a centimeter-scale ultrathin alumina membrane onto arbitrary substrates. - In: ACS applied materials & interfaces, ISSN 1944-8252, Bd. 13 (2021), 29, S. 35124-35132
The transfer of an ultrathin membrane onto arbitrary substrates is important in different practical fields. Conventional wet-transfer methods inevitably induce wrinkle defects as a result of the large contact angle of the trapped droplet between the membrane and the substrate. Here, we demonstrate a gas flow-assisted method (GFAM) to transfer centimeter (cm)-scale ultrathin membranes onto arbitrary substrates (including a curved substrate) without wrinkles. GFAM makes use of contact angle hysteresis to bulge the trapped droplet between the substrate and the ultrathin membrane and simultaneously stretch the ultrathin membrane during rapid dewetting driven by gas flow. Moreover, GFAM can be easily fulfilled by using compressed air for seconds. Compared with conventional hydrophilic treatments or organic liquid wetting, this method has no durability concern and does not change the surface nature of substrates. Taking a widely used ultrathin anodic aluminum oxide (AAO) membrane as an example, we successfully demonstrate the application of a large-area wrinkle-free ultrathin AAO membrane to defect-free ordered nanostructure array fabrication and investigate the micro-scale details of macro-scale wrinkles generated by the conventional ways. In addition, its corresponding superiority over the defective counterpart is further studied in optical sensing. This method is highly valuable for promoting the simplicity of large-area ultrathin membrane transfer in practice.
https://doi.org/10.1021/acsami.1c07574