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Zhao, Junping; Wang, Yahui; Qian, Yudan; Jin, Huile; Tang, Xinyue; Huang, Zaimei; Lou, Jiayi; Zhang, Qingcheng; Lei, Yong; Wang, Shun
Hierarchical design of cross-linked NiCo2S4 nanowires bridged NiCo-hydrocarbonate polyhedrons for high-performance asymmetric supercapacitor. - In: Advanced functional materials, ISSN 1616-3028, Bd. 33 (2023), 4, 2210238, S. 1-14

Engineering core-shell materials with rationally designed architectures and components is an effective strategy to fulfill the high-performance requirements of supercapacitors. Herein, hierarchical candied-haws-like NiCo2S4NiCo(HCO3)2 core-shell heterostructure (NiCo2S4@HCs) is designed with NiCo(HCO3)2 polyhedrons being tightly strung by cross-linked NiCo2S4 nanowires. This rational design not only creates more electroactive sites but also suppresses the volume expansion during the charge-discharge processes. Meanwhile, density functional theory calculations ascertain that the formation of NiCo2S4@HCs heterostructure simultaneously facilitates OH− adsorption/desorption and accelerates electron transfer within the electrode, boosting fast and efficient redox reactions. Ex situ X-ray diffraction and Raman measurements reveal that gradual phase transformations from NiCo(HCO3)2 to NiCo(OH)2CO3 and then to highly-active NiCoOOH take place during the cycles. Therefore, NiCo2S4@HCs demonstrates an ultrahigh capacitance of 3178.2 F g−1 at 1 A g−1 and a remarkable rate capability of 2179.3 F g−1 at 30 A g−1. In addition, the asymmetric supercapacitor NiCo2S4@HCs//AC exhibits a high energy density of 69.6 W h kg−1 at the power density of 847 W kg−1 and excellent cycling stability with 90.2% retained capacitance after 10 000 cycles. Therefore, this novel structural design has effectively manipulated the interface charge states and guaranteed the structural integrity of electrode materials to achieve superior electrochemical performances.



https://doi.org/10.1002/adfm.202210238
Hähnlein, Bernd; Honig, Hauke; Schaaf, Peter; Krischok, Stefan; Tonisch, Katja
Effect of poly-crystallinity on the magnetoelectric behavior of TiN/AlN/Ni MEMS cantilevers investigated by finite element methods. - In: Physica status solidi, ISSN 1862-6319, Bd. 220 (2023), 16, 2200839, S. 1-6

Herein, magnetoelectric microelectromechanical system (MEMS) cantilevers are investigated on basis of a TiN/AlN/Ni laminate derived from experimental sensors using finite-element simulations. With the anisotropic ΔE effect as an implication of the magnetocrystalline anisotropy, the lateral sensitivity of the sensor is studied for different nickel layer thicknesses and boundary conditions. It is found that above 60% of the cantilever length, the nickel is effectively not contributing to the sensor sensitivity anymore which is supported by the investigation of sensors with partial nickel coverage. The boundary condition of the magnetostrictive layer is found to affect the sensitivity of thick layers while it is negligible for thinning layers. Further investigations on basis of polycrystalline untextured nickel with slightly preferred orientations reveal a stronger effect on thin layers than on thicker ones. It is found to arise from relatively large crystals in the high-sensitivity region near the clamping of the sensor. For thicker polycrystalline layers, the ΔE effect reproduces a characteristic based mainly on the (110) and (111) orientations while the (100) orientation appears to be underrepresented.



https://doi.org/10.1002/pssa.202200839
Ma, Mengmeng; Liu, Jun; Zhao, Huaping; Yue, Shizhong; Zhong, Li; Huang, Yanbin; Jia, Xiaohao; Liu, Kong; Li, Xiaobao; Wang, Zhijie; Qu, Shengchun; Lei, Yong
Broadened photocatalytic capability to near-infrared for CdS hybrids and positioning hydrogen evolution sites. - In: Applied catalysis, ISSN 1873-3883, Bd. 325 (2023), 122327

Wide-spectrum light harvesting is critical in determining practical photocatalysis water splitting. Hybridization presents a viable strategy to broaden photocatalytic capability, yet the direct conversion of near-infrared (NIR) light remains a matter of great concern. Herein, a state-of-art ternary Au nanorodsMoS2-CdS (AMC) hybrid is designed to address this challenge. AMC achieves a leap-forward apparent quantum yield (AQY) of 1.06% at 700 nm and an AQY of 35.7% at 450 nm, extending the hydrogen evolution reaction (HER) capability of CdS hybrids to the NIR region firstly. It is revealed that the energetic hot electrons supplied by Au nanorods (NRs) are responsible for this extension. Indispensable, MoS2 performs a platform to collect the hot electrons from Au NRs and the photoinduced electrons from CdS. The HER active sites are positioned as MoS2-CdS interfaces both from experimental and theoretical viewpoints. This work opens up a new horizon for the forward of the wide-spectrum photocatalysis design.



https://doi.org/10.1016/j.apcatb.2022.122327
Xu, Changfan; Dong, Yulian; Shen, Yonglong; Zhao, Huaping; Li, Liqiang; Shao, Guosheng; Lei, Yong
Fundamental understanding of nonaqueous and hybrid Na-CO2 batteries: challenges and perspectives. - In: Small, ISSN 1613-6829, Bd. 19 (2023), 15, 2206445, S. 1-30

Alkali metal-CO2 batteries, which combine CO2 recycling with energy conversion and storage, are a promising way to address the energy crisis and global warming. Unfortunately, the limited cycle life, poor reversibility, and low energy efficiency of these batteries have hindered their commercialization. Li-CO2 battery systems have been intensively researched in these aspects over the past few years, however, the exploration of Na-CO2 batteries is still in its infancy. To improve the development of Na-CO2 batteries, one must have a full picture of the chemistry and electrochemistry controlling the operation of Na-CO2 batteries and a full understanding of the correlation between cell configurations and functionality therein. Here, recent advances in CO2 chemical and electrochemical mechanisms on nonaqueous Na-CO2 batteries and hybrid Na-CO2 batteries (including O2-involved Na-O2/CO2 batteries) are reviewed in-depth and comprehensively. Following this, the primary issues and challenges in various battery components are identified, and the design strategies for the interfacial structure of Na anodes, electrolyte properties, and cathode materials are explored, along with the correlations between cell configurations, functional materials, and comprehensive performances are established. Finally, the prospects and directions for rationally constructing Na-CO2 battery materials are foreseen.



https://doi.org/10.1002/smll.202206445
Wang, Cai; Zheng, Chunfang; Zhao, Huaping; Fu, Qun; Lei, Yong
TiO2 thickness-dependent charge transfer effect in p-aminothiophenol molecules chemisorbed on TiO2/Ni substrates. - In: Applied surface science, Bd. 610 (2023), 155573

Semiconductors have been modulated in thickness to optimize their surface-enhanced Raman scattering (SERS) activity in noble metal/semiconductor SERS substrates. However, the charge transfer (CT) resonance mechanism caused by the change of the semiconductor thickness has not been fully clarified yet, due to the influence of the strong surface plasmon resonance (SPR) effect from the noble metals. Here, systems of p-aminothiophenol (PATP) molecules chemisorbed on TiO2/Ni nanopillar array films with precisely controlled TiO2 thicknesses (PATP/TiO2/Ni) were developed to systematically evaluate the TiO2 thickness-dependent CT mechanism on the premise of minimizing the SPR influence. Ultraviolet-visible, photoluminescence and X-ray photoelectron spectroscopy results demonstrated that four parts that ascribed to the SERS enhancement, photo-induced CT from Ni to TiO2, resonance excitation of TiO2, CT from TiO2 surface states to PATP molecules, and the molecular resonance of PATP molecules, are highly TiO2-thickness dependent. Hence the whole system exhibits a strong TiO2-thickness-dependent CT effect (at the two interfaces of Ni-TiO2 and TiO2-PATP) and SERS activity with a maximum SERS intensity at a TiO2 thickness of 40 nm. This work shall be valuable for future developing an optimal metal/semiconductor SERS substrates and obtaining an in-depth understanding of the semiconductor-thickness-dependent charge transfer mechanism for SERS applications.



https://doi.org/10.1016/j.apsusc.2022.155573
Großmann, Max; Bohm, Sebastian; Heyder, Stefan; Schwarzburg, Klaus; Kleinschmidt, Peter; Runge, Erich; Hannappel, Thomas
Generalized modeling of photoluminescence transients. - In: Physica status solidi, ISSN 1521-3951, Bd. 260 (2023), 1, 2200339, S. 1-12

Time-resolved photoluminescence (TRPL) measurements and the extraction of meaningful parameters involve four key ingredients: a suitable sample such as a semiconductor double heterostructure, a state-of-the-art measurement setup, a kinetic model appropriate for the description of the sample behavior, and a general analysis method to extract the model parameters of interest from the measured TRPL transients. Until now, the last ingredient is limited to single curve fits, which are mostly based on simple models and least-squares fits. These are often insufficient for the parameter extraction in real-world applications. The goal of this article is to give the community a universal method for the analysis of TRPL measurements, which accounts for the Poisson distribution of photon counting events. The method can be used to fit multiple TRPL transients simultaneously using general kinematic models, but should also be used for single transient fits. To demonstrate this approach, multiple TRPL transients of a GaAs/AlGaAs heterostructure are fitted simultaneously using coupled rate equations. It is shown that the simultaneous fits of several TRPL traces supplemented by systematic error estimations allow for a more meaningful and more robust parameter determination. The statistical methods also quantify the quality of the description by the underlying physical model.



https://doi.org/10.1002/pssb.202200339
Wang, Zidong; Hong, Ping; Zhao, Huaping; Lei, Yong
Recent developments and future prospects of transition metal compounds as electrode materials for potassium-ion hybrid capacitors. - In: Advanced Materials Technologies, ISSN 2365-709X, Bd. 8 (2023), 3, 2200515, insges. 18 S.

Potassium-ion hybrid capacitors (PIHCs) have attracted considerable attention as emerging electrochemical energy storage devices for simultaneously achieving high energy and power density, which the key to success is the development of compatible electrode materials for both battery-type anode and capacitive cathode. Among numerous electrode materials, transition metal compounds (including oxides, chalcogenide, carbides, and nitrides) show great potential owing to their high theoretical capacity to achieve high energy density, but their sluggish reaction kinetics restrict the attainable power density. Hence, in the last few years, different strategies are proposed to improve the performance of transition metal compounds as electrode materials for PIHCs, and significant progress is achieved. Herein, this review outlines recent advances of employing transition metal compounds as electrode materials for PIHCs. The performance and challenges of different transition metal compounds are discussed in detail. Finally, the future prospects of practical applications of transition metal compounds in PIHCs are briefly discussed.



https://doi.org/10.1002/admt.202200515
Hülser, Tobias; Köster, Felix; Lüdge, Kathy; Jaurigue, Lina
Deriving task specific performance from the information processing capacity of a reservoir computer. - In: Nanophotonics, ISSN 2192-8614, Bd. 12 (2023), 5, S. 937-947

In the reservoir computing literature, the information processing capacity is frequently used to characterize the computing capabilities of a reservoir. However, it remains unclear how the information processing capacity connects to the performance on specific tasks. We demonstrate on a set of standard benchmark tasks that the total information processing capacity correlates poorly with task specific performance. Further, we derive an expression for the normalized mean square error of a task as a weighted function of the individual information processing capacities. Mathematically, the derivation requires the task to have the same input distribution as used to calculate the information processing capacities. We test our method on a range of tasks that violate this requirement and find good qualitative agreement between the predicted and the actual errors as long as the task input sequences do not have long autocorrelation times. Our method offers deeper insight into the principles governing reservoir computing performance. It also increases the utility of the evaluation of information processing capacities, which are typically defined on i.i.d. input, even if specific tasks deliver inputs stemming from different distributions. Moreover, it offers the possibility of reducing the experimental cost of optimizing physical reservoirs, such as those implemented in photonic systems.



https://doi.org/10.1515/nanoph-2022-0415
Link, Steffen; Dimitrova, Anna; Krischok, Stefan; Ivanov, Svetlozar
Electrochemical deposition of silicon in organic electrolytes. - In: Reference module in chemistry, molecular sciences and chemical engineering, (2023)

Electrodeposition is a versatile instrumental technique, already applied in many industrial fields. However, the deposition of silicon and other reactive elements is still challenging and requires further research and improvement. Accomplishing an efficient electrodeposition of silicon at room temperature is very attractive due to the high number of manufacturing technologies that would benefit from this approach. This work provides an overview of the electrochemical approaches for silicon deposition performed in organic electrolytes. The main factors that impact this process are individually discussed and exemplified with appropriately updated literature sources. Furthermore, the previously available research on characterization of electrodeposited silicon containing layers is provided. These studies are presented in the context of better understanding the structure, composition, and functional properties of the deposited silicon material, which may attract the attention of young academic scientists and process engineers.



https://doi.org/10.1016/B978-0-323-85669-0.00005-2
Wüster, Julian; Reetz, Andreas; Schmidt-Grund, Rüdiger; Knauer, Andrea; Sinzinger, Stefan
Approaches for the RCWA-based non-destructive characterization of subwavelength-structured gratings. - In: EOS Annual Meeting (EOSAM 2022), (2022), 05012, S. 1-2

Nano-structuring enables us to add additional degrees of freedom to the design of optical elements. Especially the possibility of controlling the polarization is of great interest in the field of nano-structured optics. For being able to exploit the whole range of form-birefringent phase shifts, the aspect ratios of the resulting element are typically much higher than the aspect ratios of conventional diffractive optical elements (DOEs), which does not only pose a challenge on fabrication but also on characterization. We evaluate several well-established approaches for the nondestructive characterization, including Müller-Matrix-Ellipsometry, measurement of the diffraction efficiencies, scattering measurements and calibration with rigorous coupled-wave modelling. The goal is to understand the challenges with all these techniques and combine them to a reliable method for structural reconnaisance of high aspect ratio nanostructures.



https://doi.org/10.1051/epjconf/202226605012