Dissertations from 2018

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Liu, Fengli; Yan, Yong; Chen, Ge; Wang, Dong
Recent advances in ambient electrochemical methane conversion to oxygenates using metal oxide electrocatalysts. - In: Green chemistry, ISSN 1463-9270, Bd. 26 (2024), 2, S. 655-677

To reach a decarbonized future, the conversion of greenhouse gases into green fuels and valuable chemicals is of crucial importance. Methane emissions are the second most significant contributor to global warming. Recent advances in electrocatalytic partial oxidation of methane to high-value fuels at ambient temperatures promise to sidestep the requirement of high temperature in conventional thermal catalysis and provide a revolutionary, sustainable, and decentralized alternative to flaring. Electrocatalysts that can selectively produce valuable compounds from methane under mild conditions are essential for commercialization. This review covers current developments in the electrochemical partial oxidation of methane to oxygenates, with an emphasis on metal oxide electrocatalysts. The regularly deployed strategies, including doping and interface engineering, are systematically reviewed in detail. In addition, the design of the electrolytic cell, the electrolyte, time, potential, and temperature are examined thoroughly and discussed.



https://doi.org/10.1039/D3GC03513A
Li, Feitao; Tan, Xinu; Flock, Dominik; Oliva Ramírez, Manuel; Wang, Dong; Qiu, Risheng; Schaaf, Peter
Structure-dependent oxidation behavior of Au-Cu nanoparticles. - In: Journal of alloys and compounds, ISSN 1873-4669, Bd. 976 (2024), 173179, S. 1-8

Thermal oxidation is an easily controlled method to change the physical and chemical properties of nanoparticles, thus optimizing and expanding their applications. Unfortunately, less attention has been paid to the role of the crystal structure whose atomic arrangements can be critical for oxidation. Au-Cu nanoparticles showing a fast order-disorder transformation are oxidized at two temperatures of ordered (L10) and disordered (A1) phase regions. The oxidation rates between the two phases are compared by the Arrhenius equation, and a lower oxidation rate is determined in the L10 lattice than in the A1 lattice based on the time required for the complete oxidation. One possible reason is attributed to the longer diffusion length in the L10 lattice compared to the A1 lattice due to the anisotropic diffusion path of the former while isotropic diffusion of the latter, resulting in longer oxidation time and then slower oxidation for the ordered sample. The crystalline phase of Au-Cu nanoparticles can be straightforwardly tuned and the resulting atomic disposition is a powerful tool to control oxidation evolution.



https://doi.org/10.1016/j.jallcom.2023.173179
Grad, Marius; Honig, Hauke; Diemar, Andreas; Flock, Dominik; Spieß, Lothar
Complex material analysis of a TiC coating produced by hot pressing with optical light microscopy, EDS, XRD, GDOES and EBSD. - In: Surface and coatings technology, ISSN 1879-3347, Bd. 476 (2024), 130265, S. 1-11

The present study investigates the interface between carbon steel and titanium samples annealed at different temperatures (ϑ1 = Image 1 and ϑ2 = Image 2). In both cases, an observable layer forms at the interface, with its thickness increasing from tϑ1 = 2.75 ± Image 3 at Image 1 to tϑ2 = 8.86 ± Image 4 at Image 2. The layer's composition and thickness evolve with temperature. Analysis reveals approximately 40 at.-% carbon concentration in the exterior region, indicating likely titanium carbide creation. X-ray diffraction identifies titanium carbide peaks, while microscopy and elemental mapping confirm compositional gradients at the interface. Electron Backscatter Diffraction (EBSD) shows a gradient in grain size near the TiC surface, reflecting TiC nucleation rates. XRD data detect both titanium carbide and titanium phases, with TiC becoming more prominent at Image 2. Rietveld analysis further confirms TiC formation. Notably, distinct diffraction patterns on the contact and rear sides suggest a Ti(C, O, N) presence. Depth profiles exhibit varying surface and depth carbon concentrations, attributed to temperature effects. The study successfully demonstrates TiC coating fabrication through hot pressing, wherein Ti(C, O, N) coatings arise from titanium's affinity for reacting with oxygen and nitrogen. This research contributes to the understanding of phase transformations and interfacial properties in titanium-carbon steel systems.



https://doi.org/10.1016/j.surfcoat.2023.130265
Li, Zhiyong; Chen, Guangshen; Cheng, Pengfei; Zhang, Zhang; Liu, Junming
Phototactic photocatalysis enabled by functionalizing active microorganisms with photocatalyst. - In: Advanced sustainable systems, ISSN 2366-7486, Bd. 8 (2024), 2, 2300302, S. 1-10

Positive phototropism enables plants to take advantage of sunlight more efficiently. However, positive phototropism of plant-like photocatalyst has not been reported yet, which cause people's limited understanding on it. Therefore, developing new photocatalysts that can move toward the light source and thus speed up the photocatalytic process, is a great challenge. Herein, a biologically active photocatalyst (graphitic carbon nitride combined with algae microorganisms, g-C3N4/alga) is reported first that can behave like green plants and move toward light source, leading to a great enhancement in photocatalysis. The photocatalytic degradation efficiency of the phototactic g-C3N4/alga is improved up to 570% than that of pure g-C3N4. The phototactic g-C3N4/alga photocatalyst can effectively utilize the synergy of phototaxis of microalgae and photocatalytic activity of g-C3N4 to promote the pollutant decomposition using sunlight. Imparting photocatalyst with positive phototropism will open a new door in photocatalysis field for clean energy production, pollutant treatment, and biomass conversion.



https://doi.org/10.1002/adsu.202300302
Wang, Honglei; Bo, Yifan; Klingenhof, Malte Philipp Helmuth; Peng, Jiali; Wang, Dong; Wu, Bing; Pezoldt, Jörg; Cheng, Pengfei; Knauer, Andrea; Hua, Weibo; Wang, Hongguang; Aken, Peter Antonie van; Sofer, Zdeněk; Strasser, Peter; Guldi, Dirk; Schaaf, Peter
A universal design strategy based on NiPS3 nanosheets towards efficient photothermal conversion and solar desalination. - In: Advanced functional materials, ISSN 1616-3028, Bd. 34 (2024), 8, 2310942, S. 1-11

2D nanomaterials are proposed as promising photothermal materials for interfacial photothermal water evaporation. However, low evaporation efficiency, the use of hazardous hydrofluoric solution, and poor stability severely limit their practical applications. Here, a mixed solvent exfoliation surface deposition (MSESD) strategy for the preparation of NiPS3 nanosheets and NiPS3/polyvinyl alcohol (PVA) converter is successfully developed. The converter is obtained by drop-casting the NiPS3/PVA nanosheets onto a sponge. The PVA is mainly deposited on the edge of NiPS3 nanosheets, which not only improves the stability of NiPS3 nanosheets, but also adheres to the sponge to prepare a 3D photothermal converter, which shows an evaporation rate of 1.48 kg m−2 h−1 and the average photothermal conversion efficiency (PTCE) of 93.5% under a light intensity of 1 kW m−2. The photothermal conversion mechanism reveals that the energy of absorbed photons in NiPS3 nanosheets can be effectively converted into heat through non-radiative photon transitions as well as multiple optical interactions. To the best of the knowledge, this is the first report on the application of 2D metal-phosphorus-chalcogen (MPChx) for solar desalination, which provides new insights and guidance for the development of high-performance 2D photothermal materials.



https://doi.org/10.1002/adfm.202310942
Luo, Wenjun; Xuan, Xinmiao; Shen, Jinfeng; Cheng, Pengfei; Wang, Dong; Schaaf, Peter; Zhang, Zhang; Liu, Junming
High performance photothermal carbon nanotubes/nanostructured hydrogel for solar electricity production and solar water sterilization. - In: Applied surface science, Bd. 643 (2024), 158680

Solar energy is a promising renewable energy source with the potential to contribute to sustainable development. Efficient photothermal conversion is critical for solar energy acquisition and conversion. Here, carbon nanotubes (CNTs) were gelatinized to obtain the nanostructured CNT/hydrogel, and then highly light-absorbing CNT/n-hydrogels with surface texture were obtained by replicating the micrometer structure from the black silicon (b-Si) surface onto CNT/hydrogels by using a PDMS mold. Through the synergistic effect of both surface texture and nanostructures, it demonstrates high efficiency of solar electricity production and solar sterilization. A small thermoelectric (TE) module with an area of 4 × 4 cm2 is integrated with CNT/n-hydrogel absorber for the investigation of photo-thermoelectric conversion. The output power of the CNT/n-hydrogel TE device is 1.42 W•m−2 under 1 sun. And by connecting four devices in series, it has successfully demonstrated for charging mobile phones under two different solar illuminations. This work provides a cost-effective and easy fabrication method for opening up the hydrogel as a photothermal absorber, which is low-cost, reproducible, high-efficiency solar water sterilization and high photothermal conversion efficiency.



https://doi.org/10.1016/j.apsusc.2023.158680
Wöste, Andreas; Hergert, Germann; Silies, Martin; Wang, Dong; Groß, Petra; Lienau, Christoph
Photon-induced near-field interaction in ultrafast point-projection electron microscopy. - In: CLEO, (2023), JTu2A.133, insges. 2 S.

We report the first study of ultrafast, slow (<100 eV) free electron wavepackets with optical near fields. This interaction is probed in a point-projection-microscope with 50fs temporal resolution using strongly localized fields around a nano-antenna.



https://ieeexplore.ieee.org/document/10258768
Diemar, Andreas; Gerth, Uwe; Lahmer, Tom; Teichert, Gerd; Könke, Carsten
Numerische Ermittlung von Zielgrößen und Prozessparametern des Einsatzhärtens unter Berücksichtigung des lokalen Beanspruchungszustandes versagensrelevanter Konstruktionsdetails :
Numerical determination of target values and process parameters of case hardening, taking into account the local stress state of failure-relevant construction details. - In: HTM - journal of heat treatment and materials, ISSN 2194-1831, Bd. 78 (2023), 6, S. 352-368

Through the thermochemical process of case hardening, the local material strength of steel components can be increased. In addition to the increase in stress due to the notch effect, the shape of construction details also has an effect on key component properties after case hardening, such as edge hardness and case hardening depth. The component-related specification of target values for case hardening is currently based on empirical values or expert knowledge. In addition, the effect of design details during case hardening is not taken into account when specifying process parameters in the control and regulation software of case hardening systems. This article presents a concept for the numerical determination of target values and process parameters for case hardening based on the stress state of the component. Compared to the empirically based determination of target values and process parameters for case hardening, the application of the concept makes it possible to adapt the case hardening of components to their stress in the failure range and thus significantly increase the energy and resource efficiency of case hardening.



https://doi.org/10.1515/htm-2023-0023
Bohm, Sebastian; Grunert, Malte; Schwarz, Felix; Runge, Erich; Wang, Dong; Schaaf, Peter; Chimeh, Abbas; Lienau, Christoph
Gold nanosponges: fascinating optical properties of a unique disorder-dominated system. - In: Journal of the Optical Society of America, ISSN 1520-8540, Bd. 40 (2023), 6, S. 1491-1509

Nanoporous gold is a three-dimensional bulk material that is percolated with a random network of nanometer-sized ligaments and made by selective corrosion of bimetallic alloys. It has intriguing geometric, catalytic, and optical properties that have fascinated scientists for many decades. When such a material is made into the form of small, 100-nm-sized particles, so-called nanosponges emerge that offer much flexibility in controlling their geometric, electronic, and optical properties. Importantly, these particles act as an antenna for light that can efficiently localize optical fields on a deep subwavelength scale in certain hotspots at the particle surface. This makes such nanosponges an interesting platform for plasmonic sensing, photocatalysis, and surface-enhanced Raman spectroscopy. Since the optical properties of these nanosponges can be controlled to a large degree by tuning their geometry and/or composition, they have attracted increasing attention in recent years. Here, we provide a concise overview of the current state of the art in this field, covering their fabrication, computational modeling, and specifically the linear and nonlinear optical properties of individual and hybrid nanosponges, for example, plasmon localization in randomly disordered hotspots with a size <10 nm and a long lifetime with an exceptionally high Purcell factor. The resulting nonlinear optical and photoemission properties are discussed for individual and hybrid nanosponges. The results presented have strong implications for further applications of such nanosponges in photonics and photocatalysis.



https://doi.org/10.1364/JOSAB.479739
Glaser, Marcus; Matthes, Sebastian; Riegler, Sascha Sebastian; Hildebrand, Jörg; Bergmann, Jean Pierre; Schaaf, Peter; Gallino, Isabella
Characterization of plastic-metal hybrid composites joined by means of reactive Al/Ni multilayers - evaluation of occurring thermal regime. - In: Engineering for a changing world, (2023), 4.3.056, S. 1-16

Present challenges in material science and joining technology are ever more subject to the desire for lightweight construction and engineering. Plastic-metal composites are suitable material combinations but also require the development and investigation of appropriate joining technologies. A particularly promising approach is the application of reactive multilayer foils. As an innovative method, these foils provide the possibility of flexible and low-distortion joining of dissimilar materials. The underlying reaction mechanism offers fast exothermic reaction propagation with well-known exothermic power output while the energy source is introduced directly into the joining zone. In this work, hybrid lap joints between semi-crystalline polyamide 6 and structured austenitic stainless steel X5CrNi18-10 were joined using reactive Al/Ni multilayer foils. The self-propagating reaction provides immediate temperatures that are well above the melting point of used plastic but decays rapidly after only a few milliseconds. To support ongoing investigations regarding composite formation, analysis of occurring thermal regime is in the focus of this work. Conducted experiments are supported by accompanying thermal simulation in ANSYS Workbench. Besides the estimation regarding sensitivity of thermal material parameters the evaluation of formed melting zone and resulting thermally influenced area is a central topic.



https://doi.org/10.22032/dbt.58913