Journal articles from 2018

Anzahl der Treffer: 687
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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. 0 (2024), 0, insges. 17 S.

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.
Hannappel, Thomas; Shekarabi, Sahar; Jaegermann, Wolfram; Runge, Erich; Hofmann, Jan Philipp; Krol, Roel van de; May, Matthias M.; Paszuk, Agnieszka; Hess, Franziska; Bergmann, Arno; Bund, Andreas; Cierpka, Christian; Dreßler, Christian; Dionigi, Fabio; Friedrich, Dennis; Favaro, Marco; Krischok, Stefan; Kurniawan, Mario; Lüdge, Kathy; Lei, Yong; Roldán Cuenya, Beatriz; Schaaf, Peter; Schmidt-Grund, Rüdiger; Schmidt, W. Gero; Strasser, Peter; Unger, Eva; Montoya, Manuel Vasquez; Wang, Dong; Zhang, Hongbin
Integration of multi-junction absorbers and catalysts for efficient solar-driven artificial leaf structures : a physical and materials science perspective. - In: Solar RRL, ISSN 2367-198X, Bd. 0 (2024), 0, S. 1-88

Artificial leaves could be the breakthrough technology to overcome the limitations of storage and mobility through the synthesis of chemical fuels from sunlight, which will be an essential component of a sustainable future energy system. However, the realization of efficient solar-driven artificial leaf structures requires integrated specialized materials such as semiconductor absorbers, catalysts, interfacial passivation, and contact layers. To date, no competitive system has emerged due to a lack of scientific understanding, knowledge-based design rules, and scalable engineering strategies. Here, we will discuss competitive artificial leaf devices for water splitting, focusing on multi-absorber structures to achieve solar-to-hydrogen conversion efficiencies exceeding 15%. A key challenge is integrating photovoltaic and electrochemical functionalities in a single device. Additionally, optimal electrocatalysts for intermittent operation at photocurrent densities of 10-20 mA cm^-2 must be immobilized on the absorbers with specifically designed interfacial passivation and contact layers, so-called buried junctions. This minimizes voltage and current losses and prevents corrosive side reactions. Key challenges include understanding elementary steps, identifying suitable materials, and developing synthesis and processing techniques for all integrated components. This is crucial for efficient, robust, and scalable devices. Here, we discuss and report on corresponding research efforts to produce green hydrogen with unassisted solar-driven (photo-)electrochemical devices. This article is protected by copyright. All rights reserved.
Schaaf, Peter; Constantinescu, Catalin; Matei, Andreea
Laser material processing: from fundamental interactions to innovative applications (E-MRS). - In: Applied surface science advances, ISSN 2666-5239, Bd. 21 (2024), 100592, insges. 1 S.
Zhang, Yuanpeng; Cheng, Pengfei; Wang, Dong; Wang, Hui; Tang, Yongliang; Wang, Wei; Li, Yuhang; Sun, Zeqi; Lv, Wenmei; Liu, Qingxiang
Evaluating the field emission properties of N-type black silicon cold cathodes based on a three-dimensional model. - In: ACS applied materials & interfaces, ISSN 1944-8252, Bd. 16 (2024), 2, S. 2932-2939

Black silicon (BS), a nanostructured silicon surface containing highly roughened surface morphology, has recently emerged as a promising candidate for field emission (FE) cathodes in novel electron sources due to its huge number of sharp tips with ease of large-scale fabrication and controllable geometrical shapes. However, evaluating the FE performance of BS-based nanostructures with high accuracy is still a challenge due to the increasing complexity in the surface morphology. Here, we demonstrate a 3D modeling methodology to fully characterize highly disordered BS-based field emitters randomly distributed on a roughened nonflat surface. We fabricated BS cathode samples with different morphological features to demonstrate the validity of this method. We utilize parametrized scanning electron microscopy images that provide high-precision morphology details, successfully describing the electric field distribution in field emitters and linking the theoretical analysis with the measured FE property of the complex nanostructures with high precision. The 3D model developed here reveals a relationship between the field emission performance and the density of the cones, successfully reproducing the classical relationship between current density J and electric field E (J-E curve). The proposed modeling approach is expected to offer a powerful tool to accurately describe the field emission properties of large-scale, disordered nano cold cathodes, thus serving as a guide for the design and application of BS as a field electron emission material.
Schaaf, Peter; Zyabkin, Dmitry
Mössbauer spectroscopy. - In: Encyclopedia of condensed matter physics, (2024), S. 15-28

The current chapter provides the reader with a general introduction of Mössbauer effect following by its unique utilization, which became known as Mössbauer spectroscopy. Mössbauer spectroscopy is based on the recoilless emission and following resonant absorption of gamma radiation by atomic nuclei and has been at the scientific forefront of physics, chemistry, biology, mineralogy for more than 60 years. Soon after the discovery of the Mössbauer effect, it became obvious that this effect can be used to study various properties of materials on a microscopic scale via hyperfine interactions with an unprecedented resolution. This was the beginning of a new analytical tool - Mössbauer spectroscopy. Today, it has developed into a standard analytical technique used in many laboratories and big research facilities. The current chapter provides the reader with a general introduction, explains the underlying hyperfine interactions and gives examples of the possible application of the method.

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.
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.
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.
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.
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.