Publikationsliste des FG Werkstoffe der Elektrotechnik

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Cheng, Pengfei; Wang, Hongguang; Wang, Honglei; Wang, Dong; Aken, Peter Antonie van; Schaaf, Peter
Plasmon-enhanced light absorption below the bandgap of semiconducting SnS2 microcubes for highly efficient solar water evaporation. - In: Small, ISSN 1613-6829, Bd. 0 (2024), 0, 2400588, S. 1-9

Semiconducting materials show high potential for solar energy harvesting due to their suitable bandgaps, which allow the efficient utilization of light energy larger than their bandgaps. However, the photon energy smaller than their bandgap is almost unused, which significantly limits their efficient applications. Herein, plasmonic Pd/SnS2 microcubes with abundant Pd nanoparticles attached to the SnS2 nanosheets are fabricated by an in situ photoreduction method. The as-prepared Pd/SnS2 microcubes extend the light-harvesting ability of SnS2 beyond its cutoff wavelength, which is attributed to the localized surface plasmon resonance (LSPR) effect of the Pd nanoparticles and the 3D structure of the SnS2 microcubes. Pd nanoparticles can also enhance the light absorption of TiO2 nanoparticles and NiPS3 nanosheets beyond their cutoff wavelengths, revealing the universality for promoting absorption above the cutoff wavelength of the semiconductors. When the plasmonic Pd/SnS2 microcubes are integrated into a hydrophilic sponge acting as the solar evaporator, a solar-to-vapor efficiency of up to 89.2% can be achieved under one sun. The high solar-to-vapor conversion efficiency and the broad applicability of extending the light absorption far beyond the cutoff wavelength of the semiconductor comprise the potential of innovative plasmonic nanoparticle/semiconductor composites for solar desalination.



https://doi.org/10.1002/smll.202400588
Yan, Yong; Li, Tongxian; Oliva Ramírez, Manuel; Zhao, Yuguo; Wang, Shuo; Chen, Xin; Wang, Dong; Schaaf, Peter; Wang, Xiayan; Guo, Guangsheng
Efficient tuning of the selectivity of Cu-based interface for electrocatalytic CO2 reduction by ligand modification. - In: Materials today, ISSN 2468-6069, Bd. 44 (2024), 101620, S. 1-12

The development of efficient strategies to tune the CO2RR selectivity of Cu-based catalytic interfaces, especially on specific domains, such as Cu (200) facets with high activity toward competitive hydrogenation evolution reaction (HER), remains a challenging task. In this work, Cu-based catalytic layers with thiocyanate (-SCN), cyanide (-CN), or ethylenediamine (-NH2R) coordination linkages are prepared on Cu nanocolumns arrays (Cu NCAs) with predominant (200) exposed facets. The coordination of these ligands induces more Cu+ species and inhibits the adsorption of H∗ on the Cu (200) facet, leading to enhanced CO2RR performance and substantially suppressing the competitive HER. The faradaic efficiency (FE) of Cu–SCN, Cu–CN, and Cu–NH2R NWAs for producing HCOOH, C2H4, and C1 mixture products (HCOOH and CO) reach to 66.5%, 21.1%, and 57.1%, respectively. In situ spectroscopic studies reveal Cu–SCN, Cu–CN, and Cu–NH2R exhibit more reasonable adsorption energy toward ∗OCHO, ∗CO, and ∗COOH intermediates, promoting the HCOOH, C2H4, and C1 mixture generation, respectively. This study might provide a new perspective for the development of high-performance Cu-based CO2RR catalytic electrodes based on the combination of various commercial free-standing Cu substrates and organic/inorganic ligands.



https://doi.org/10.1016/j.mtener.2024.101620
Jaekel, Konrad; Jiménez, Juan Jesús; Riegler, Sascha Sebastian; Matthes, Sebastian; Glaser, Marcus; Bergmann, Jean Pierre; Schaaf, Peter; Gallino, Isabella; Morales Sánchez, Francisco Miguel; Müller, Jens; Bartsch, Heike
Influence of additional intermediate thick Al layers on the reaction propagation and heat flow of Al/Ni reactive multilayers. - In: Advanced engineering materials, ISSN 1527-2648, Bd. 0 (2024), 0, 2400522, S. 1-8

This study investigates the effects of sputtering and electron beam evaporation (e-beam) on the microstructure and reactive properties of Al/Ni reactive multilayers (RMLs). The intermixing zone, a critical factor influencing reaction kinetics, is characterized using high-resolution transmission electron microscopy and found to be consistently 3 nm for both fabrication methods. Differential scanning calorimetry reveals that e-beam samples, with thicker Al layers, exhibit slightly higher total molar enthalpy and maintain high reaction temperatures despite reduced reaction velocities in comparison to sputtered samples. X-ray diffraction confirms the formation of both Al3Ni2 and AlNi phases in the e-beam samples. These findings indicate that while thicker bilayer structures reduce reaction velocity, they keep thermal output and mitigate the impact of intermixing zones, leading to similar total molar enthalpy. This analysis underscores the significance of deposition technique and bilayer thickness in optimizing the performance of Al/Ni RML, offering the possibility to establish different phase formations in thicker RML. It advances the control over the reactive properties of RMLs in their applications, for example, reactive bonding.



https://doi.org/10.1002/adem.202400522
Sauni Camposano, Yesenia Haydee; Jaekel, Konrad; Riegler, Sascha S.; Matthes, Sebastian; Glaser, Marcus; Peter, Nicolas J.; Vardo, Emina; Bartsch, Heike; Schwaiger, Ruth; Bergmann, Jean Pierre; Gallino, Isabella; Schaaf, Peter
Controlling propagation velocity in Al/Ni reactive multilayer systems by periodic 2D surface structuring. - In: Advanced engineering materials, ISSN 1527-2648, Bd. n/a (2024), n/a, 2302272, S. 1-11

The chemical energy released as heat during the exothermic reaction of reactive multilayer systems has shown potential applications in various technological areas, e.g., in joining applications. However, controlling the heat release rate and the propagation velocity of the reaction is required to enhance their performance in most of these applications. Herein, a method to control the propagation velocity and heat release rate of the system is presented. The sputtering of Al/Ni multilayers on substrates with periodic 2D surface structures promotes the formation of growth defects into the system. This modification in the morphology locally influences the reaction characteristics. Tailoring the number of 2D structures in the substrate enables the control of the velocity and maximum temperature of the propagation front. The morphology of the produced reactive multilayers is investigated before and after reaction using scanning electron microscopy, transmission electron microscopy, and X-ray diffraction. In addition, the enthalpy of the system is obtained through calorimetric analysis. The self-sustained and self-propagating reaction of the systems is monitored by a high-speed camera and a high-speed pyrometer, thus revealing the propagation velocity and the temperatures with time resolution in the microsecond regime.



https://doi.org/10.1002/adem.202302272
Graske, Marcus; Sauni Camposano, Yesenia Haydee; Vardo, Emina; Matthes, Sebastian; Schaaf, Peter
Mechanical ignition of Al/Ni reactive multilayer systems: influence of impacting material, its properties, and geometric characteristics. - In: Advanced engineering materials, ISSN 1527-2648, Bd. n/a (2024), n/a, 2400479, S. 1-13

Al/Ni reactive multilayer systems (RMS) with a bilayer thickness of Λ = 50 nm and total thickness th = 5 μm on a SiO2 substrate exhibit a self-propagating reaction after ignition. A common method to initiate the self-propagating reaction is by electric spark ignition. Herein, RMS are ignited by a mechanical impact using various materials with indeterminate geometries to investigate the basic mechanisms. SiO2, glass, PMMA, and resin-bonded SiC particles are used as impacting material with different geometrical impact areas. The used materials are placed on top of the RMS and a mechanical impulse is applied. The ignition behavior of the RMS is subsequently evaluated and classified. Additionally, the impacted RMS are examined by microscopy to reveal the damage pattern. By correlating particle size ⟨Dparticle⟩ and spacing ⟨dhole⟩ of the penetrating materials, an ignition threshold can be established. Moreover, the results demonstrate that the energy input threshold can be reduced through a strategic distribution of particles within the impacting and penetrating geometry. This provides valuable insights into the mechanical ignition fundamental and supports future applications of mechanical ignition of RMS.



https://doi.org/10.1002/adem.202400479
Wang, Honglei; Cheng, Pengfei; Wu, Bing; Yan, Yong; Schaaf, Peter; Sofer, Zdeněk; Wang, Dong
2D metal phosphorous trichalcogenides (MPCh3) for sustainable energy storage and conversion: nanoarchitectonics and advanced applications. - In: Advanced functional materials, ISSN 1616-3028, Bd. n/a (2024), n/a, 2407432, S. 1-22

2D metal phosphorous trichalcogenides (MPCh3) have attracted considerable attention in sustainable energy storage and conversion due to their distinct physical and chemical characteristics, such as adjustable energy bandgap, significant specific surface area, and abundant active sites. However, research on 2D MPCh3 primarily focuses on electrocatalysis, and understanding its energy conversion and storage mechanisms remains incomplete. This review comprehensively summarizes recent advancements in energy storage and conversion using 2D MPCh3-based materials of various structures. It begins with a discussion of the distinctive properties and preparation techniques of 2D MPCh3, followed by a focus on the rational design and development of these materials for diverse energy-related applications, including rechargeable batteries, supercapacitors, electrocatalysis, photocatalysis, and desalination. Finally, it outlines the key challenges and prospects for future research on 2D MPCh3 materials.



https://doi.org/10.1002/adfm.202407432
Vardo, Emina; Sauni Camposano, Yesenia Haydee; Matthes, Sebastian; Glaser, Marcus; Bartsch, Heike; Hildebrand, Jörg; Bergmann, Jean Pierre; Schaaf, Peter
Impact of substrate thickness and surface roughness on Al/Ni multilayer reaction kinetics. - In: Advanced engineering materials, ISSN 1527-2648, Bd. n/a (2024), n/a, 2302269, S. 1-10

Reactive multilayers comprising alternating nanoscale layers of Al and Ni exhibit potential across various applications, including localized heating for welding and joining. Control over reaction properties is pivotal for emerging applications, such as chemical time delays or neutralization of biological or chemical weapons. In this research, insights are offered into the intricate interplay between substrate thickness, surface roughness, and the behavior of Al/Ni reactive multilayers, opening avenues for tailored applications in various domains. To observe this interplay, silica with various thicknesses from 0.4 to 1.6 μm is deposited on polished single-crystalline Si and rough poly-Si base substrates. Additionally, to analyze the impact of varying silica thickness along the sample length on reaction behavior, silica in steplike shape is fabricated. Subsequently, Al/Ni multilayers with 5 μm total thickness and 20 or 50 nm bilayer periodicities are deposited. Reaction velocity and temperature are monitored with a high-speed camera and pyrometer. In the results, it is indicated that silica thickness significantly affects self-propagation in multilayers. The reaction is not self-sustained for silica layers ≤ 0.4 μm, depending on bilayer periodicity and substrate roughness. The velocity increases or decreases based on the direction of reaction propagation, whether it moves upward or downward, in relation to the thickness of silica.



https://doi.org/10.1002/adem.202302269
Riegler, Sascha S.; Sauni Camposano, Yesenia Haydee; Jaekel, Konrad; Frey, Maximilian; Neemann, Christian; Matthes, Sebastian; Vardo, Emina; Chegeni, Maryam R.; Bartsch, Heike; Busch, Ralf; Müller, Jens; Schaaf, Peter; Gallino, Isabella
Nanocalorimetry of nanoscaled Ni/Al multilayer films: on the methodology to determine reaction kinetics for highly reactive films. - In: Advanced engineering materials, ISSN 1527-2648, Bd. 0 (2024), 0, 2302279, S. 1-10

Free-standing Ni/Al multilayer films with a planar morphology, a bilayer thickness of 20 nm, and an average composition of Ni50Al50 (at%) deposited by direct current magnetron sputtering are investigated by nanocalorimetry and conventional calorimetry. Both the novel fast differential scanning calorimeter (FDSC) Flash DSC 2+ from Mettler-Toledo (MT) and conventional calorimeter MT DSC 3 are used to cover a range of heating rates from 0.1 to 10^4 K s^−1. A quantitative kinetic study of the interdiffusion and phase reaction sequence is performed via a Kissinger analysis covering five orders of magnitude of heating rates. Using the calorimetric data, the derived apparent activation energies suggest monotonic reaction kinetics over the entire range of heating rates applied. To correct the thermal lag at the highest heating rates with the FDSC for nonadhered free-standing films, a new methodology for its correction is used. Overall, this work extends the application of commercial FDSC to nonadhered films.



https://doi.org/10.1002/adem.202302279
Smyrnova, Kateryna; Sahul, Martin; Haršáni, Marián; Beresnev, Vyacheslav; Truchlý, Martin; Čaplovič, L’ubomír; Čaplovičová, Mária; Kusý, Martin; Kozak, Andrii; Flock, Dominik; Kassymbaev, Alexey; Pogrebnjak, Aleksandr Dmitrievič
Composite materials with nanoscale multilayer architecture based on cathodic-arc evaporated WN/NbN coatings. - In: ACS omega, ISSN 2470-1343, Bd. 9 (2024), 15, S. 17247-17265

Hard nitride coatings are commonly employed to protect components subjected to friction, whereby such coatings should possess excellent tribomechanical properties in order to endure high stresses and temperatures. In this study, WN/NbN coatings are synthesized by using the cathodic-arc evaporation (CA-PVD) technique at various negative bias voltages in the 50-200 V range. The phase composition, microstructural features, and tribomechanical properties of the multilayers are comprehensively studied. Fabricated coatings have a complex structure of three nanocrystalline phases: β-W2N, δ-NbN, and ε-NbN. They demonstrate a tendency for (111)-oriented grains to overgrow (200)-oriented grains with increasing coating thickness. All of the data show that a decrease in the fraction of ε-NbN phase and formation of the (111)-textured grains positively impact mechanical properties and wear behavior. Investigation of the room-temperature tribological properties reveals that with an increase in bias voltage from −50 to −200 V, the wear mechanisms change as follows: oxidative &flech; fatigue and oxidative &flech; adhesive and oxidative. Furthermore, WN/NbN coatings demonstrate a high hardness of 33.6-36.6 GPa and a low specific wear rate of (1.9-4.1) × 10-6 mm3/Nm. These results indicate that synthesized multilayers hold promise for tribological applications as wear-resistant coatings.



https://doi.org/10.1021/acsomega.3c10242
Zhao, Yuguo; Björk, Emma M.; Yan, Yong; Schaaf, Peter; Wang, Dong
Recent progress in transition metal based catalysts and mechanism analysis for alcohol electrooxidation reactions. - In: Green chemistry, ISSN 1463-9270, Bd. 26 (2024), 9, S. 4987-5003

In order to address energy and environmental challenges effectively, there is a need to promote renewable energy-driven electrochemical conversion technologies, particularly electrosynthesis. Electrosynthesis has the potential to convert abundant molecules into valuable chemicals and fuels. However, the widespread adoption of electrosynthesis is often hindered by the slow oxygen evolution reaction (OER). To overcome this limitation, we can employ the more efficient alcohol electrooxidation reaction (AOR), utilizing renewable biomass-derived alcohols as an alternative to OER for producing high-value chemicals. Consequently, the development of efficient AOR catalysts, in conjunction with cathodic reduction reactions (hydrogen evolution, oxygen, and nitrogen electroreduction, etc.), is crucial for sustainable and environmentally-friendly advancements. A thorough understanding of AOR mechanisms is essential for catalyst design and can be achieved through the utilization of in situ characterization techniques and density functional theory (DFT) calculations. This review summarizes recent progress in AOR catalysts, with a particular focus on the electrooxidation of monohydric alcohols, polyols, and associated studies on reaction mechanisms. Additionally, the review identifies key factors impeding AOR development and provides insights into future prospects.



https://doi.org/10.1039/D4GC00227J